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2021, Vol. 53, No. 2　Online: 15 February 2021

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Hollow FeCo-FeCoP@C nanocubes embedded in nitrogen-doped carbon nanocages for efficient overall water splitting Yuzhi Li, Siwei Li, Jing Hu, Yuanyuan Zhang, Yuchen Du, Xijiang Han, Xi Liu, Ping Xu 2021, 53(2): 1-8.  DOI: 10.1016/j.jechem.2020.05.012 Abstract ( 5 )   PDF (3180KB) ( 4 )   Designing readily available and highly active electrocatalysts for water splitting is essential for renewable energy technologies. Here we present the construction of FeCo-FeCoP@C hollow nanocubes encapsulated in nitrogen-doped carbon nanocages (FeCo-FeCoP@C@NCCs) through controlled carbonization and subse-quent phosphorization of a Prussian blue analogue. With stronger electronic interaction and hollow structure, the as-obtained FeCo-FeCoP@C@NCCs material requires small overpotentials of 91 mV and 280 mV to deliver 10 mA cm-2 in 1 M KOH toward hydrogen and oxygen evolution, respectively. More importantly, applying this material for overall water splitting, it only requires 1.64 V to afford 10 mA cm-2 and exhibits impressively durability over 40 h without obvious performance decay. The pre-sent approach inspires potentials for the controllable synthesis of multi-component catalysts for practical applications.

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Enhanced active site extraction from perovskite LaCoO3 using encapsulated PdO for efficient CO2 methanation Kuncan Wang, Wen Li, Junjie Huang, Jiale Huang, Guowu Zhan, Qingbiao Li 2021, 53(2): 9-19.  DOI: 10.1016/j.jechem.2020.05.027 Abstract ( 3 )   PDF (6056KB) ( 2 )   The extraction of metallic nanoparticles from perovskite-type oxides (ABO3) under mild reducing condi-tions is a novel way to prepare well-dispersed supported catalysts (B/AOδ). Herein, we found that the encapsulated PdO in perovskite LaCoO3 (PdO@LaCoO3) could facilitate the phase transformation of the perovskite structure at a low temperature owing to both strong H2 spillover of Pd and intimate interac-tion between the encapsulated PdO and LaCoO3. The pure LaCoO3 without PdO was relatively inert to CO2 hydrogenation (CO2 conversion <4%). In contrast, PdO@LaCoO3 exhibited excellent CO2 methanation per-formance with 62.3% CO2 conversion and >99% CH4 selectivity. The characterization results demonstrated that the catalytically active Co2C was in-situ formed by carburization of the extracted Co0 during CO2 methanation for the PdO@LaCoO3 sample. Whereas, the LaCoO3 with surface supported PdO (PdO/LaCoO3) showed a weak interaction and remained a perovskite structure with few Co2C active centers after the catalytic reaction, which was similar to the parent LaCoO3. Accordingly, the PdO/LaCoO3 showed an inferior catalytic performance with 31.8% CO2 conversion and 87.4% CH4 selectivity. Therefore, the designed encapsulation structure of PdO within perovskite is critical to extract metallic NPs from perovskite-type oxides, which has the potential to prepare other integrated nanocatalysts based on perovskite-type oxides.

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Insights into the adsorption/desorption of CO2 and CO on single-atom Fe-nitrogen-graphene catalyst under electrochemical environment Jiejie Li, Jian Liu, BoYang 2021, 53(2): 20-25.  DOI: 10.1016/j.jechem.2020.04.016 Abstract ( 8 )   PDF (5008KB) ( 2 )   Single-atom metal-nitrogen-graphene (M-N-Gra) catalysts are promising materials for electrocatalytic CO2 reduction reaction (CO2RR). However, theoretical explorations on such systems were greatly hindered be-cause of the complexity in modeling solid/liquid interface and electrochemical environment. In the cur-rent work, we investigated two crucial processes in CO2RR, i.e. adsorption and desorption of CO2 and CO at Fe-N4 center, with an explicit aqueous model. We used the ab initio molecular dynamics simulations associated with free energy sampling methods and electrode potential analysis to estimate the energet-ics under electrochemical environment, and found significant difference in aqueous solution compared with the same process in vacuum. The effect of applied electrode potential on the adsorption structures, charge transfer and free energies of both CO2 and CO on Fe-N-Gra was thoroughly discussed. These find-ings bring insights in fundamental understandings of the CO2RR process under realistic conditions, and facilitate future design of efficient M-N-Gra-based CO2RR catalysts.

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Highly active Fe7S8 encapsulated in N-doped hollow carbon nanofibers for high-rate sodium-ion batteries Chengzhi Zhang, Donghai Wei, Fei Wang, Guanhua Zhang, Junfei Duan, Fei Han, Huigao Duan, Jinshui Liu 2021, 53(2): 26-35.  DOI: 10.1016/j.jechem.2020.05.011 Abstract ( 3 )   PDF (9666KB) ( 3 )   Nanostructured iron sulfides are regarded as a potential anode material for sodium-ion batteries in virtue of the rich natural abundance and remarkable theoretical capacity. However, poor rate performance and inferior cycling stability caused by sluggish kinetics and volume swelling represent two main obstacles at present. The previous research mainly focuses on nanostructure design and/or hybridizing with conductive materials. Further boosting the property by adjusting Fe/S atomic ratio in iron sulfides is rarely reported. In this work, Fe7S8 and FeS2 encapsulated in N-doped hollow carbon fibers (NHCFs/Fe7S8 and NHCFs/FeS2) are constructed by a combined chemical bath deposition and subsequent sulfidation treatment. The well-designed NHCFs/Fe7S8 electrode displays a remarkable capacity of 517 mAh g-1 at 2 A g-1 after 1000 cycles and a superb rate capability with a capability of 444 mAh g-1 even at 20 A g-1 in ether-based electrolyte. Additionally, the rate capability of NHCFs/Fe7S8 is superior to that of the contrast NHCFs/FeS2 electrode and also much better than the values of the most previously reported iron sulfide-based anodes. The in-depth mechanism explanation is explained by further experimental analysis and theoretical calculation, revealing Fe7S8 displays improved intrinsic electronic conductivity and faster Na+ diffusion coefficient as well as higher reaction reversibility.

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The impact of having an oxygen-rich microporous surface in carbon electrodes for high-power aqueous supercapacitors Servann Hérou, Maria Crespo Ribadeneyra, Philipp Schlee, Hui Luo, Liviu Cristian Tanase, Christine Robberg, Magdalena Titirici 2021, 53(2): 36-48.  DOI: 10.1016/j.jechem.2020.04.068 Abstract ( 7 )   PDF (12869KB) ( 2 )   The growth of electrical transportation is crucially important to mitigate rising climate change concerns regarding materials supply. Supercapacitors are high-power devices, particularly suitable for public transportation since they can easily store breaking energy due to their high-rate charging ability. Additionally, they can function with two carbon electrodes, which is an advantage due to the abundance of carbon in biomass and other waste materials (i.e., plastic waste). Newly developed supercapacitive nanocarbons display extremely narrow micropores (<0.8 nm), as it increases drastically the capacitance in aqueous electrolytes. Here, we present a strategy to produce low-cost flexible microporous electrodes with extremely high power density (>100 kW kg-1), using fourty times less activating agent than tradi- tionnal chemically activated carbons. We also demonstrate that the affinity between the carbon and the electrolyte is of paramount importance to maintain rapid ionic diffusion in narrow micropores. Finally, this facile synthesis method shows that low-cost and bio-based free-standing electrode materials with reliable supercapacitive performances can be used in electrochemistry.

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Co- and N-doped carbon nanotubes with hierarchical pores derived from metal-organic nanotubes for oxygen reduction reaction Xuewan Wang, Xiuan Xi, Ge Huo, Chenyu Xu, Pengfei Sui, Renfei Feng, Xian-Zhu Fu, Jing-Li Luo 2021, 53(2): 49-55.  DOI: 10.1016/j.jechem.2020.05.020 Abstract ( 3 )   PDF (3981KB) ( 2 )   Biomolecules with a broad range of structure and heteroatom-containing groups offer a great opportu- nity for rational design of promising electrocatalysts via versatile chemistry. In this study, uniform folic acid-Co nanotubes (FA-Co NTs) were hydrothermally prepared as sacrificial templates for highly porous Co and N co-doped carbon nanotubes (Co-N/CNTs) with well-controlled size and morphology. The forma- tion mechanism of FA-Co NTs was investigated and FA-Co-hydrazine coordination interaction together with the H-bond interaction between FA molecules was characterized to be the driving force for growth of one-dimensional nanotubes. Such distinct metal-ligand interaction afforded the resultant CNTs rich Co-Nx sites, hierarchically porous structure and Co nanoparticle-embedded conductive network, thus an overall good electrocatalytic activity for oxygen reduction. Electrochemical tests showed that Co-N/ CNTs-900 promoted an efficient 4e- ORR process with an onset potential of 0.908 V vs. RHE, a limiting current density of 5.66 mA cm-2 at 0.6 V and a H2O2 yield lower than 5%, comparable to that of 20% Pt/C catalyst. Moreover, the catalyst revealed very high stability upon continuous operation and remark- able tolerance to methanol.

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Insights on the mechanism of Na-ion storage in expanded graphite anode Xiaodan Li, Zhibin Liu, Jinliang Li, Hang Lei, Wenchen Zhuo, Wei Qin, Xiang Cai, Kwun Nam Hui, Likun Pan, Wenjie Mai 2021, 53(2): 56-62.  DOI: 10.1016/j.jechem.2020.05.022 Abstract ( 4 )   PDF (8167KB) ( 2 )   Currently, Na-ion battery (NIB) has become one of the most potential alternatives for Li-ion batteries due to the safety and low cost. As a promising anode for Na-ion storage, expanded graphite has attracted con- siderable attention. However, the sodiation-desodiation process is still unclear. In our work, we obtain expanded graphite through slight modified Hummer's method and subsequent thermal treatment, which exhibits excellent cycling stability. Even at a high current density of 1 A g-1, our expanded graphite still remains a high reversible capacity of 100 mA h g-1 after 2600 cycles. Furthermore, we also investigate the electrochemical mechanism of our expanded graphite for Na-ion storage by operando Raman technique, which illuminate the electrochemical reaction during different sodiation-desodiation processes.

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Novel polymer acceptors achieving 10.18% efficiency for all-polymer solar cells Shaorong Huang, Feiyan Wu, Zuoji Liu, Yongjie Cui, Lie Chen, Yiwang Chen 2021, 53(2): 63-68.  DOI: 10.1016/j.jechem.2020.04.075 Abstract ( 5 )   PDF (2783KB) ( 2 )   Polymer acceptors based on extended fused ring p skeleton has been proven to be promising candidates for all-polymer solar cells (all-PSCs), due to their remarkable improved light absorption than the tradi- tional imide-based polymer acceptors. To expand structural diversity of the polymer acceptors, herein, two polymer acceptors PSF-IDIC and PSi-IDIC with extended fused ring p skeleton are developed by copolymerization of 2,20-((2Z,20Z)-((4,4,9,9-tetrahexadecyl-4,9-dihydro-s-indaceno [1,2-b:5,6-b']dithio phene-2,7-diyl)bis(methanylylidene))bis(3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile (IDIC-C16) block with sulfur (S) and fluorine (F) functionalized benzodithiophene (BDT) unit and silicon (Si) atom functionalized BDT unit, respectively. Both polymer acceptors exhibit strong light absorption. The PSF-IDIC exhibits similar energy levels and slightly higher absorption coefficient relative to the PSi-IDIC. After blended with the donor polymer PM6, the functional atoms on the polymer acceptors show quite different effect on the device performance. Both of the acceptors deliver a notably high open circuit voltage (VOC) of the devices, but PSi-IDIC achieves higher VOC than PSF-IDIC. All-PSC based on PM6: PSi-IDIC attains a power conversion efficiency (PCE) of 8.29%, while PM6:PSF-IDIC-based device achieves a much higher PCE of 10.18%, which is one of the highest values for the all-PSCs reported so far. The superior device performance of PM6:PSF-IDIC is attributed to its higher exciton dissociation and charge transport, decreased charge recombination, and optimized morphology than PM6:PSi-IDIC counterpart. These results suggest that optimizing the functional atoms of the side chain provide an effective strategy to develop high performance polymer acceptors for all-PSCs.

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Shorter alkyl chain in thieno[3,4-c]pyrrole-4,6-dione (TPD)-based large bandgap polymer donors - Yield efficient non-fullerene polymer solar cells Jiaji Zhao, Xuelong Huang, Qingduan Li, Shengjian Liu, Ziqiang Fan, Di Zhang, Shanshan Ma, Zhixiong Cao, Xuechen Jiao, Yue-Peng Cai, Fei Huang 2021, 53(2): 69-76.  DOI: 10.1016/j.jechem.2020.04.076 Abstract ( 4 )   PDF (2204KB) ( 2 )   Typically, conjugated polymers are composed of conjugated backbones and alkyl side chains. In this con- tribution, a cost-effective strategy of tailoring the length of alkyl side chain is utilized to design high-performing thieno[3,4-c]pyrrole-4,6-dione (TPD)-based large bandgap polymer donors PBDT-BiTPD (Cv) (v = 48, 52, 56), in which v represents the alkyl side chain length in term of the total carbon number.A combination of light absorption, device, and morphology examinations make clear that the shorter alkyl side chains yield (i) higher crystallinity and more predominant face-on crystallite orientation in their neat and BHJ blend films, (ii) higher charge mobilities (6.7×10-4 cm2 V-1 s-1 for C48 vs. 3.2×10-4cm2 V-1 s-1 for C56), and negligible charge recombination, consequently, (iii) significantly improved fill-factor (FF) and short current (JSC), while almost the same open circuit voltage (VOC) of ca.0.82 V in their corresponding BHJ devices. In parallel, as alkyl side chain lengths decrease from C56 to C48, power conversion efficiencies (PCEs) increased from 7.8% for C56 to 11.1% for C52, and further to 14.1% for C48 in their BHJ solar cells made with a narrow bandgap non-fullerene acceptor Y6. This systematic study declares that shortening the side chain, if providing appropriate solubility in device solution processing solvents, is of essential significance for developing high-performing polymer donors and further improving device photovoltaic performance.

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Cobalt porphyrins supported on carbon nanotubes as model catalysts of metal-N4/C sites for oxygen electrocatalysis Haonan Qin, Yanzhi Wang, Bin Wang, Xiaoguang Duan, Haitao Lei, Xuepeng Zhang, Haoquan Zheng, Wei Zhang, Rui Cao 2021, 53(2): 77-81.  DOI: 10.1016/j.jechem.2020.05.015 Abstract ( 4 )   PDF (6541KB) ( 2 )   Transition-metal based M-N4/C catalysts are appealing for electrocatalytic oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Employing model catalysts, which have well-defined molecular structures and coordination environments, to investigate electrocatalytic performance of M-N4/C sites for ORR and OER is of fundamental significance. Herein, we reported the use of Co tetra (phenyl)porphyrin 1 and Co tetra(pentafluorophenyl)porphyrin 2 as models to probe the role of Co-N4/C sites for oxygen electrocatalysis. We showed that Co porphyrin 1 is more efficient than its struc- tural analogue 2 for oxygen electrocatalysis in alkaline aqueous solutions, indicating that the electron- rich Co-N4/C site is more favored when noncovalently adsorbed on carbon supports. This work inspires rational design of reaction-oriented catalysts for sustainable energy storage and conversion technologies.

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Amorphization activated FeB2 porous nanosheets enable efficient electrocatalytic N2 fixation Ke Chu, Weicong Gu, Qingqing Li, Yaping Liu, Ye Tian, Wuming Liu 2021, 53(2): 82-89.  DOI: 10.1016/j.jechem.2020.05.009 Abstract ( 5 )   PDF (5746KB) ( 2 )   Designing active, robust and cost-effective catalysts for the nitrogen reduction reaction (NRR) is of para- mount significance for sustainable electrochemical NH3 synthesis. Transition-metal diborides (TMB2) have been recently theoretically predicted to be a new class of potential NRR catalysts, but direct exper- imental evidence is still lacking. Herein, we present the first experimental demonstration that amorphous FeB2 porous nanosheets (a-FeB2 PNSs) could be a highly efficient NRR catalyst, which exhibited an NH3 yield of 39.8 lg h-1 mg-1 ( 0.3 V) and a Faradaic efficiency of 16.7% ( 0.2 V), significantly outperforming their crystalline counterpart and most of existing NRR catalysts. First-principle calculations unveiled that the amorphization could induce the upraised d-band center of a-FeB2 to boost d-2π* coupling between the active Fe site and *N2H intermediate, resulting in enhanced *N2H stabilization and reduced reaction barrier. Out study may facilitate the development and understanding of earth-abundant TMB2-based cat- alysts for electrocatalytic N2 fixation.

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Unveiling enzyme-mimetic active intermediate of a bioinspired oxo-MoSx electrocatalyst for aqueous nitrate reduction Yuting Wang, Bin Zhang 2021, 53(2): 90-92.  DOI: 10.1016/j.jechem.2020.05.017 Abstract ( 3 )   PDF (1890KB) ( 2 )

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Enhanced hydrogen evolution reaction in Sr doped BiFeO3 by achieving the coexistence of ferroelectricity and ferromagnetism at room temperature Ji Qi, Huan Liu, Ming Feng, Hang Xu, Haiwei Liu, Chen Wang, Aopei Wang, Weiming Lü 2021, 53(2): 93-98.  DOI: 10.1016/j.jechem.2020.05.003 Abstract ( 4 )   PDF (3195KB) ( 2 )   The perovskite transition metal oxide (TMO) has been considered in electrocatalysis for the modern clean energy technologies as its high electrochemical activity and low cost. The atomic scale engineering to the local stoichiometry of single crystal TMO provides a clue of the relation between electronic structure and catalytic performance. Here we report a hydrogen evolution reaction (HER) activity enhancement ~ 1761% of Bi0.85Sr0.15FeO3 compared to the pure BiFeO3. By the systemic investigation of the Sr doping level of Bi1-xSrxFeO3 (BSFO), it is found that the HER enhancement originates from the improvement of ferromagnetism of BSFO without obvious scarification of the ferroelectricity at the room temperature. The multiple ferroic orderings in BSFO are beneficial for HER activity, which offers the strengthen of hybridization of Fe 3d and O 2p orbitals from the view of ferromagnetism, and the assis- tance of electron drift by spontaneous electric polarization. Our study not only affords the strategy of developing multiple ferroic orderings in TMO, but also facilitates the atomic scale understanding of the improved HER activity.

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Incorporation of layered tin (IV) phosphate in graphene framework for high performance lithium-sulfur batteries Haifeng Yuan, Na Zhang, Leiwu Tian, Lei Xu, Qinjun Shao, Syed Danish Ali Zaidi, Jianping Xiao, Jian Chen 2021, 53(2): 99-108.  DOI: 10.1016/j.jechem.2020.05.028 Abstract ( 3 )   PDF (6097KB) ( 2 )   To anchor the polysulfide and enhance the conversion kinetics of polysulfide to disulfide / sulfide is crit-ical for improving the performance of lithium-sulfur battery. For this purpose, the graphene-supported tin (IV) phosphate (Sn(HPO4)2·H2O, SnP) composites (SnP-G) are employed as the novel sulfur hosts in this work. When compared to the graphene-sulfur and carbon-sulfur composites, the SnP-G-sulfur com- posites exhibit much better cycling performance at 1.0C over 800cycles. Meanwhile, the pouch cell fab- ricated with the SnP-G-sulfur cathodes also exhibits excellent performance with an initial capacity of 1266.6 mAh g-1 (S) and capacity retention of 76.9% after 100cycles at 0.1C. The adsorption tests, density functional theory (DFT) calculations in combination with physical characterizations and electrochemical measurements provide insights into the mechanism of capture-accelerated conversion mechanism of polysulfide at the surface of SnP. DFT calculations indicate that the Li-O bond formed between Li atom (from Li2Sn, n = 1, 2, 4, 6, 8) and O atom (from PO3-OH in SnP) is the main reason for the strong interac- tions between Li2Sn and SnP. As a result, SnP can effectively restrain the shuttle effect and improving the cycling performance of Li-S cell. In addition, by employing the climbing-image nudged elastic band (ci- NEB) methods, the energy barrier for lithium sulfide decomposition (charging reaction) on SnP is proved to decrease significantly compared to that on graphene. It can be concluded that SnP is an effective sulfur hosts acting as dual-functional accelerators for the conversion reactions of polysulfide to sulfide (dis- charging reaction) as well as polysulfide to sulfur (charging reaction).

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A new trick on an old support: Zr in situ defects-created carbon nitride for efficient electrochemical nitrogen fixation Wenwen Lin, Siyu Yao, Hao Chen, Shenglai Li, Yang Xia, Yuan Yao, Jing Li, Dangguo Cheng, Jie Fu 2021, 53(2): 109-115.  DOI: 10.1016/j.jechem.2020.05.013 Abstract ( 6 )   PDF (4974KB) ( 2 )   Electrochemical nitrogen reduction reaction (NRR) to produce ammonia under ambient conditions is con- sidered as a promising approach to tackle the energy-intensive Haber-Bosch process, but the low Faradaic efficiency and yield of NH3 are still a challenge. Herein, a carbon-vacancies enriched mesoporous g-C3N4 is developed by an in situ Zr doping strategy. The in situ mesoporous-forming mechanism is deeply understood by TPSR to reveal the functions of Zr dopant that pulls C from the precursor of C3N4, resulting the formation of homogeneous mesopores with about 57% of the one C-defective s-triazine ring in C3N4. Due to the defect sites obtained in metal doping synthesis, the RuAu bimetallic supported catalyst (RuAu3/0.3Zr-C3N4) exhibits effective NRR performance with a Faraday efficiency of 11.54% and an NH3 yield of 5.28 1g h-1 mg-1cat at-0.1 V (RHE), which is nearly 10 times higher than that of RuAu3/C3N4 cat- alyst. This work proposes a simple and template-free preparation method for the high defect density meso- porous C3N4, and provides new possibilities of a wide application of mesopore g-C3N4.

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Incorporating multifunctional LiAlSiO4 into polyethylene oxide for high-performance solid-state lithium batteries Yuqi Wu, Xinhai Li, Guochun Yan, Zhixing Wang, Huajun Guo, Yong Ke, Lijue Wu, Haikuo Fu, Jiexi Wang 2021, 53(2): 116-123.  DOI: 10.1016/j.jechem.2020.04.070 Abstract ( 4 )   PDF (4242KB) ( 2 )   High ionic conductivity, good electrochemical stability, and satisfactory mechanical property are the cru- cial factors for polymer solid state electrolytes. Herein, fast ion conductor LiAlSiO4 (LASO) is incorporated into polyethylene oxide (PEO)-based solid-state electrolytes (SSEs). The SSEs containing LASO exhibit enhanced mechanical properties performance compared to pristine PEO-LiTFSI electrolyte. A reduced melting transition temperature of 40.57 °C is enabled by introducing LASO in to PEO-based SSE, which is beneficial to the motion of PEO chain and makes it possible for working at a moderate environment. Coupling with the enhanced motion of PEO, dissociation of the lithium salt, and conducting channel of LASO, the optimized composite polymer SSE exhibits a high ionic conductivity of 4.68 × 10-4, 3.16 × 10-4 and 1.62 × 10-4 S cm-1 at 60, 50 and 40 °C, respectively. The corresponding LiFePO4//Li solid-state battery exhibits high specific capacities of 166, 160 and 139 mAh g-1 at 0.2 C under 60, 40 and 25 °C. In addition, it remains 130 mAh g-1 at 4.0 C, and maintains 91.74% after 500 cycles at 1.0 C under 60 °C. This study provides a simple approach for developing ionic conductor-filled polymer elec-trolytes in solid-state lithium battery application.

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Carbon decorated Li3V2(PO4)3 for high-rate lithium-ion batteries: Electrochemical performance and charge compensation mechanism Manling Ding, Chen Cheng, Qiulong Wei, Yue Hu, Yingying Yan, Kehua Dai, Jing Mao, Jinghua Guo, Liang Zhang, Liqiang Mai 2021, 53(2): 124-131.  DOI: 10.1016/j.jechem.2020.04.020 Abstract ( 3 )   PDF (7841KB) ( 2 )   Fast charging and high-power delivering batteries are highly demanded in mobile electronics, electric vehicles and grid energy storage, but there are full of challenges. The star-material Li3V2(PO4)3 is demonstrated as a promising high-rate cathode material meeting the above requirements. Herein, we report the carbon decorated Li3V2(PO4)3 (LVP/C) cathode prepared via a facile method, which displays a remarkable high-rate capability and long-term cycling performance. Briefly, the prepared LVP/C delivers a high discharge capacity of 122 mAh g-1 (~93% of the theoretical capacity) at a high rate up to 20 C and a superior capacity retention of 87.1% after 1000 cycles. Importantly, by applying a combination of X-ray absorption spectroscopy and full-range mapping of resonant inelastic X-ray scattering, we clearly elucidate the structural and chemical evolutions of LVP upon various potentials and cycle numbers. We show unambiguous spectroscopic evidences that the evolution of the hybridization strength between V and O in LVP/C as a consequence of lithiation/delithiation is highly reversible both in the bulk and on the surface during the discharge-charge processes even over extended cycles, which should be responsible for the remarkable electrochemical performance of LVP/C. Our present study provides not only an effective synthesis strategy but also deeper insights into the surface and bulk electrochemical reaction mechanism of LVP, which should be beneficial for the further design of high-performance LVP electrode materials.

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Amorphous MoS3 enriched with sulfur vacancies for efficient electrocatalytic nitrogen reduction Ke Chu, Haifeng Nan, Qingqing Li, Yali Guo, Ye Tian, Wuming Liu 2021, 53(2): 132-138.  DOI: 10.1016/j.jechem.2020.04.074 Abstract ( 4 )   PDF (4726KB) ( 3 )   Developing low-priced, yet effective and robust catalysts for the nitrogen reduction reaction (NRR) is of vital importance for scalable and renewable electrochemical NH3 synthesis. Herein, we provide the first demonstration of MoS3 as an efficient and durable NRR catalyst in neutral media. The prepared amorphous MoS3 naturally possessed enriched S vacancies and delivered an NH3 yield of 51.7 μg h-1 mg-1 and a Faradaic efficiency of 12.8% at -0.3 V (RHE) in 0.5 M LiClO4, considerably exceeding those of MoS2 and most reported NRR catalysts. Density functional theory calculations unraveled that S vacancies involved in MoS3 played a crucial role in activating the NRR via a consecutive mechanism with a low energetics barrier and simultaneously suppressing the hydrogen evolution reaction.

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3D macropore carbon-vacancy g-C3N4 constructed using polymethylmethacrylate spheres for enhanced photocatalytic H2 evolution and CO2 reduction Xuewen Wang, Qiuchan Li, Lei Gan, Xinfei Ji, Fayun Chen, Xinke Peng, Rongbin Zhang 2021, 53(2): 139-146.  DOI: 10.1016/j.jechem.2020.05.001 Abstract ( 3 )   PDF (4674KB) ( 2 )   Metal-free g-C3N4 is widely used in photocatalytic reactions owing to its suitable band structure. However, it has low specific surface area and insufficient absorbance for visible light, and its photoexcited carriers have high recombination rates. In this study, the 3D macropore C-vacancy g-C3N4 was prepared through a facile one-step route. Polymethylmethacrylate is used as a template to increase the surface reaction sites of g-C3N4 and extend its visible-light range. Compared to unmodified g-C3N4, the H2 production and CO2 reduction rates of the fabricated g-C3N4 significantly improved. The special pore structure significantly improved the light utilization efficiency of g-C3N4 and increased the number of surface-active sites. The introduction of C-vacancy extended the absorption band of visible-light and suppressed the carrier recombination. The newly developed synthesis strategy can improve solar energy conversion efficiency and potentially modifies g-C3N4.

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Stable all-solid-state battery enabled with Li6.25PS5.25Cl0.75 as fast ion-conducting electrolyte Weidong Xiao, Hongjie Xu, Minjie Xuan, Zhiheng Wu, Yongshang Zhang, Xiangdan Zhang, Shijie Zhang, Yonglong Shen, Guosheng Shao 2021, 53(2): 147-154.  DOI: 10.1016/j.jechem.2020.04.062 Abstract ( 6 )   PDF (3477KB) ( 3 )   All-solid-state batteries (ASSB) with lithium anode have attracted ever-increasing attention towards developing safer batteries with high energy densities. While great advancement has been achieved in developing solid electrolytes (SE) with superb ionic conductivity rivalling that of the current liquid technology, it has yet been very difficult in their successful application to ASSBs with sustaining rate and cyclic performances. Here in this work, we have realized a stable ASSB using the Li6.25PS5.25Cl0.75 fast ion-conducting electrolyte together with LiNbO3 coated LiCoO2 as cathode and lithium foil as the anode. The effective diffusion coefficient of Li-ions in the battery is higher than 10-12 cm2 s-1, and the significantly enhanced electrochemical matching at the cathode-electrolyte interface was essential to enable long-term stability against high oxidation potential, with the LCO@LNO/Li6.25PS5.25Cl0.75/Li battery to retain 74.12% capacity after 430 cycles at 100 μA cm-2 and 59.7% of capacity after 800 cycles at 50 μA cm-2, at a high charging cut-off voltage of 4.2 V. This demonstrates that the Li6.25PS5.25Cl0.75 can be an excellent electrolyte for the realization of stable ASSBs with high-voltage cathodes and metallic lithium as anode, once the electrochemical compatibility between cathode and electrolyte can be addressed with a suitable buffer coating.

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Designing N-doped graphene/ReSe2/Ti3C2 MXene heterostructure frameworks as promising anodes for high-rate potassium-ion batteries Zhou Xia, Xiwen Chen, Haina Ci, Zhaodi Fan, Yuyang Yi, Wanjian Yin, Nan Wei, Jingsheng Cai, Yanfeng Zhang, Jingyu Sun 2021, 53(2): 155-162.  DOI: 10.1016/j.jechem.2020.04.071 Abstract ( 6 )   PDF (10856KB) ( 2 )   Developing high-performance anodes for potassium ion batteries (KIBs) is of paramount significance but remains challenging. In the normal sense, electrode materials are prepared by ubiquitous wet chemical routes, which otherwise might not be versatile enough to create desired heterostructures and/or form clean interfacial areas for fast transport of K-ions and electrons. Along this line, rate capability/cycling stability of resulting KIBs are greatly handicapped. Herein we present an all-chemical vapor deposition approach to harness the direct synthesis of nitrogen-doped graphene (NG)/rhenium diselenide (ReSe2) hybrids over three-dimensional MXene supports as superior heterostructure anode material for KIBs. In such an innovative design, 1T′-ReSe2 nanoparticles are sandwiched in between the NG coatings and MXene frameworks via strong interfacial interactions, thereby affording facile K+ diffusion, enhancing overall conductivity, boosting high-power performance and reinforcing structural stability of electrodes. Thus-constructed anode delivers an excellent rate performance of 138 mAh g-1 at 10.0 A g-1 and a high reversible capacity of 90 mAh g-1 at 5 A g-1 after 300 cycles. Furthermore, the potassium storage mechanism has been systematically probed by advanced in situ/ex situ characterization techniques in combination with first principles computations.

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Achieving p-type conductivity in ZnO/Bi0.5Sb1.5Te3 composites Li Yin, Lin Sun, Peng Jiang, Xinhe Bao 2021, 53(2): 163-167.  DOI: 10.1016/j.jechem.2020.04.011 Abstract ( 6 )   PDF (3232KB) ( 3 )

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Nitrogen-doped hierarchically porous carbon spheres for low concentration CO2 capture Yang Li, Jing Wang, Sisi Fan, Fanan Wang, Zheng Shen, Hongmin Duan, Jinming Xu, Yanqiang Huang 2021, 53(2): 168-174.  DOI: 10.1016/j.jechem.2020.05.019 Abstract ( 7 )   PDF (1670KB) ( 3 )   Synthesis of spherical carbon beads with effective CO2 capture capability is highly desirable for large scale application of CO2 sorption, but remains challenging. Herein, a facile and efficient strategy to prepare nitrogen-doped hierarchically porous carbon spheres was developed via co-pyrolyzation of poly(vinylidene chloride) and melamine in alginate gel beads. In this approach, melamine not only serves as the nitrogen precursor, but also acts as a template for the macropores structures. The nitrogen contents in the hierarchically porous carbon spheres reach a high level, ranging from 11.8 wt% to 14.7 wt%, as the melamine amount increases. Owing to the enriched nitrogen functionalities and the special hierarchical porous structure, the carbon spheres exhibit an outstanding CO2 capture performance, with the dynamic capacity of as much as about 7 wt% and a separation factor about 49 at 25 °C in a gas mixture of CO2/N2 (0.5:99.5, v/v).

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Robust S-doped TiO2@N,S-codoped carbon nanotube arrays as free-binder anodes for efficient sodium storage Guangzeng Liu, Man Huang, Zhengchunyu Zhang, Baojuan Xi, Haibo Li, Shenglin Xiong 2021, 53(2): 175-184.  DOI: 10.1016/j.jechem.2020.05.030 Abstract ( 2 )   PDF (6237KB) ( 4 )   Titanium dioxide (TiO2) has been investigated broadly as a stable, safe, and cheap anode material for sodium-ion batteries in recent years. However, the poor electronic conductivity and inherent sluggish sodium ion diffusion hinder its practical applications. Herein, a self-template and in situ vulcanization strategy is developed to synthesize self-supported hybrid nanotube arrays composed of nitrogen/sulfur-codoped carbon coated sulfur-doped TiO2 nanotubes (S-TiO2@NS-C) starting from H2Ti2O5·H2O nanoarrays. The S-TiO2@NS-C composite with one-dimensional nano-sized subunits integrates several merits. Specifically, sulfur doping strongly improves the Na+ storage ability of TiO2@C-N nanotubes by narrowing the bandgap of original TiO2. Originating from the nanoarrays structures built from hollow nanotubes, carbon layer and sulfur doping, the sluggish Na+ insertion/extraction kinetics is effectively improved and the volume variation of the electrode material is significantly alleviated. As a result, the S-TiO2@NS-C nanoarrays present efficient sodium storage properties. The greatly improved sodium storage performances of S-TiO2@NS-C nanoarrays confirm the importance of rational engineering and synthesis of hollow array architectures with higher complexity.

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Reduced Ti-MOFs encapsulated black phosphorus with high stability and enhanced photocatalytic activity Xiao Liu, Peijie Fan, Liangping Xiao, Jian Weng, Qingchi Xu, Jun Xu 2021, 53(2): 185-191.  DOI: 10.1016/j.jechem.2020.05.010 Abstract ( 4 )   PDF (4915KB) ( 2 )   The generation of green hydrogen (H2) energy is of great significance to solve worldwide energy and environmental issues. Reduced Ti based photocatalyst has recently attracted intensive attention due to its excellent photocatalytic activity, while the synthesis of reduced Ti based photocatalysts with high stability is still a great challenge. Here, we report a facile method for synthesis of reduced Ti metal organic frameworks (small amounts of Pt incorporated) encapsulated BP (BP/R-Ti-MOFs/Pt) hybrid nanomaterial with enhanced photocatalytic activity. The strong interaction between Ti and P reduces the valence state of the binding Ti4+ on the BP surface, forming abundant reduced Ti4+ within R-Ti-MOFs/BP. Such reduced Ti4+ render R-Ti-MOFs/BP efficient charge transfer and excellent light absorption capability, thus promote the photocatalytic H2 production efficiency. Furthermore, the Ti-P interaction stabilizes both reduced Ti4+ and BP during the photocatalytic reaction, which greatly enhanced the stability of the obtained BP/R-Ti-MOFs/Pt photocatalyst.

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A magnetic field strategy to porous Pt-Ni nanoparticles with predominant (111) facets for enhanced electrocatalytic oxygen reduction Xiao Lyu, Weina Zhang, Shuang Liu, Xiaoyang Wang, Gen Li, Bowen Shi, Kai Wang, Xin Wang, Qiang Wang, Yi Jia 2021, 53(2): 192-196.  DOI: 10.1016/j.jechem.2020.05.039 Abstract ( 3 )   PDF (2605KB) ( 2 )   For the first time, we developed porous Pt-Ni alloying nanoparticles with predominant (111) facets under intense magnetic fields. Electrochemical analysis revealed that the Pt-Ni alloying nanoparticles obtained at 2 Tesla exhibited a superior catalytic activity and durability for oxygen reduction reaction. This work demonstrated that the imposition of intense magnetic field could be considered as a new approach for developing efficient alloying electrocatalysts with preferential facets.

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Protic ionic liquids/poly(vinylidene fluoride) composite membranes for fuel cell application Isabel Vázquez-Fernández, Mohamed Raghibi, Adnane Bouzina, Laure Timperman, Janick Bigarré, Mérièm Anouti 2021, 53(2): 197-207.  DOI: 10.1016/j.jechem.2020.04.022 Abstract ( 7 )   PDF (6077KB) ( 4 )   Poly(vinylidene fluoride), PVDF, membranes have attracted considerable attention as polymer electrolytes for fuel cells. This study explores the effect of solvent on the spherulite size and the crystallinity of the polymeric membranes. Based on Hansen solubility parameters theory, the mixture of DMC and DMSO was selected among a dozen of solvents for the preparation of PVDF membranes by thermally induced phase separation. The addition of two protic ionic liquids (PILs), bis(2-ethyl hexyl) ammonium hydrogen phosphate [EHNH2][H2PO4], and imidazolium hexanoate [Im][Hex] to PVDF membranes at concentrations (10% < wPIL < 50%) has been investigated by SEM, FTIR, DSC, TGA, EIS, and DMA. The inclusion of ionic liquids into the polymer matrix influences structural parameters (degree of crystallinity and electroactive phases), thermal stability, proton conductivity and mechanical properties of the membranes. The membranes become transparent regardless type of ionic liquid employed. A small amount of ionic liquids increases the degree of crystallinity and facilitates the production of polar β and γ crystals. The proton conductivity mechanism (Grotthuss) is dependent on the ionic liquid structure (due to its self-organization in water) and the content in the PVDF membrane, as well as the membrane water uptake. Different behavior has been observed for the two ionic liquids, which stresses the challenge on selecting an appropriate cation and anion combination. The obtained composite membranes exhibited excellent mechanical performance and reduced elastic modulus, with respect to the pure polymer matrix. These results indicate that PVDF/IL composite membranes have a high potential for PEMFC applications.

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Recent advances in defect electrocatalysts: Preparation and characterization Zhaohui Xiao, Chao Xie, Yanyong Wang, Ru Chen, Shuangyin Wang 2021, 53(2): 208-225.  DOI: 10.1016/j.jechem.2020.04.063 Abstract ( 14 )   PDF (10448KB) ( 5 )   This review briefly summarizes recent progress in defect electrocatalysts, and the synthesis strategies and characterization techniques for defects are systematically discussed. Although challenges in the characterization of defect structures in the electrocatalytic reaction process remain, the dynamic evolution of defect sites is predicted to be helpful for designing and preparing high-performance electrocatalysts for commercial applications. Furthermore, due to an insufficient understanding of the defect-structure-property relationships, future possibilities for the reasonable design of defect electrocatalysts to obtain desirable performance are suggested.

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Mesh-like vertical structures enable both high areal capacity and excellent rate capability Ruyi Chen, Jialu Xue, Yujiao Gong, Chenyang Yu, Zengyu Hui, Hai Xu, Yue Sun, Xi Zhao, Jianing An, Jinyuan Zhou, Qiang Chen, Gengzhi Sun, Wei Huang 2021, 53(2): 226-233.  DOI: 10.1016/j.jechem.2020.05.035 Abstract ( 4 )   PDF (4984KB) ( 2 )   In order to balance electrochemical kinetics with loading level for achieving efficient energy storage with high areal capacity and good rate capability simultaneously for wearable electronics, herein, 2D mesh-like vertical structures (NiCo2S4@Ni(OH)2) with a high mass loading of 2.17 mg cm-2 and combined merits of both 1D nanowires and 2D nanosheets are designed for fabricating flexible hybrid supercapacitors. Particularly, the seamlessly interconnected NiCo2S4 core not only provides high capacity of 287.5 μAh cm-2 but also functions as conductive skeleton for fast electron transport; Ni(OH)2 sheath occupying the voids in NiCo2S4 meshes contributes extra capacity of 248.4 μAh cm-2; the holey features guarantee rapid ion diffusion along and across NiCo2S4@Ni(OH)2 meshes. The resultant flexible electrode exhibits a high areal capacity of 535.9 μAh cm-2 (246.9 mAh g-1) at 3 mA cm-2 and outstanding rate performance with 84.7% retention at 30 mA cm-2, suggesting efficient utilization of both NiCo2S4 and Ni(OH)2 with specific capacities approaching to their theoretical values. The flexible solid-state hybrid device based on NiCo2S4@Ni(OH)2 cathode and Fe2O3 anode delivers a high energy density of 315 μWh cm-2 at the power density of 2.14 mW cm-2 with excellent electrochemical cycling stability.

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Reinforced polysulfide barrier by g-C3N4/CNT composite towards superior lithium-sulfur batteries Xiangliang Wang, Gaoran Li, Minjie Li, Ruiping Liu, Haibo Li, Tengyu Li, Mingzhu Sun, Yirui Deng, Ming Feng, Zhongwei Chen 2021, 53(2): 234-240.  DOI: 10.1016/j.jechem.2020.05.036 Abstract ( 9 )   PDF (3027KB) ( 2 )   The notorious shuttle effect has long been obstructing lithium-sulfur (Li-S) batteries from yielding the expected high energy density and long lifespan. Herein, we develop a multifunctional polysulfide barrier reinforced by the graphitic carbon nitride/carbon nanotube (g-C3N4/CNT) composite toward inhibited shuttling behavior and improved battery performance. The obtained g-C3N4 delivers a unique sponge-like architecture with massive ion transfer pathways and fully exposed active interfaces, while the abundant C-N heteroatomic structures impose strong chemical immobilization toward lithium polysulfides. Combined with the highly conductive agent, the g-C3N4/CNT reinforced separator is endowed with great capability of confining and reutilizing the active sulfur within the cathode, thus contributing to an efficient and stable sulfur electrochemistry. Benefiting from these synergistic attributes, Li-S cells based on g-C3N4/CNT separator exhibit an excellent cyclability with a minimum decay rate of 0.03% per cycle over 500 cycles and decent rate capability up to 2 C. Moreover, a high areal capacity of 7.69 mAh cm-2 can be achieved under a raised sulfur loading up to 10.1 mg cm-2, demonstrating a facile and efficient pathway toward superior Li-S batteries.

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Unraveling and optimizing the metal-metal oxide synergistic effect in a highly active Cox(CoO)1-x catalyst for CO2 hydrogenation Kun Zhao, Marco Calizzi, Emanuele Moioli, Mo Li, Alexandre Borsay, Loris Lombardo, Robin Mutschler, Wen Luo, Andreas Züttel 2021, 53(2): 241-250.  DOI: 10.1016/j.jechem.2020.05.025 Abstract ( 3 )   PDF (2870KB) ( 2 )   The relation between catalytic reactivities and metal/metal oxide ratios, as well as the functions of the metal and the metal oxides were investigated in the CO2 hydrogenation reaction over highly active Cox(CoO)1-x catalysts in operando. The catalytic reactivity of the samples in the CO2 methanation improves with the increased CoO concentration. Strikingly, the sample with the highest concentration of CoO, i.e., Co0.2(CoO)0.8, shows activity at temperatures lower than 200 °C where the other samples with less CoO are inactive. The origins of this improvement are the increased amount and moderate binding of adsorbed CO2 on CoO sites. The derivative adsorption species are found to be intermediates of the CH4 formation. The metallic Co functions as the electronically catalytic site which provides electrons for the hydrogenation steps. As a result, an abundant amount of CoO combined with Co is the optimal composition of the catalyst for achieving the highest reactivity for CO2 hydrogenation.

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Amorphous nickel-cobalt bimetal-organic framework nanosheets with crystalline motifs enable efficient oxygen evolution reaction: Ligands hybridization engineering Yang Li, Zhonggui Gao, Huiming Bao, Binghui Zhang, Cong Wu, Chunfu Huang, Zilu Zhang, Yunyun Xie, Hai Wang 2021, 53(2): 251-259.  DOI: 10.1016/j.jechem.2020.05.002 Abstract ( 4 )   PDF (7480KB) ( 2 )   Development of high-efficiency and low-cost electrocatalyst for oxygen evolution reaction (OER) is very important for use at alkaline water electrolysis. Metal-organic frameworks (MOF) provide a rich platform for designing multi-functional materials due to their controllable composition and ultra-high surface area. Herein, we report our findings in the development of amorphous nickel-cobalt bimetal-organic framework nanosheets with crystalline motifs via a simple “ligands hybridization engineering” strategy. These complexes' ligands contain inorganic ligands (H2O and NO3-) and organic ones, hexamethylenetetramine (HMT). Further, we investigated a series of mixed-metal with multi-ligands materials as OER catalysts to explore their possible advantages and features. It is found that the Ni doping is an effective approach for optimizing the electronic configuration, changing lattice ordering degree, and thus enhancing activities of HMT-based electrocatalysts. Also, the crystalline-amorphous boundaries of various HMT-based electrocatalyst can be easily controlled by simply changing amounts of Ni-precursor added. As a result, the optimized ultrathin (Co, 0.3Ni)-HMT nanosheets can reach a current density of 10 mA cm-2 at low overpotential of 330 mV with a small Tafel slope of 66 mV dec-1. Our findings show that the electronic structure changes induced by Ni doping, 2D nanosheet structure, and MOF frameworks with multi-ligands compositions play critical roles in the enhancement of the kinetically sluggish electrocatalytic OER. The present study emphasizes the importance of ligands and active metals via hybridization for exploring novel efficient electrocatalysts.

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Amorphous 3D pomegranate-like NiCoFe nanoassemblies derived by bi-component cyanogel reduction for outstanding oxygen evolution reaction Zi-Juan Wang, Mi-Xue Jin, Lu Zhang, Ai-Jun Wang, Jiu-Ju Feng 2021, 53(2): 260-267.  DOI: 10.1016/j.jechem.2020.05.026 Abstract ( 5 )   PDF (5580KB) ( 1 )   As a representative type of self-supported templates, cyano-bridged cyanogels provide ideal plateaus for synthesis of three-dimensional (3D) nanostructures. Herein, 3D pomegranate-like Fe-doped NiCo nanoassemblies (3D PG-NiCoFe NAs) were synthesized via facile one-step bi-component cyanogel reduction with NaBH4 as the reducing agent. Specifically, the influence of the incorporated Fe amount was carefully investigated by finely adjusting the feeding molar ratios of the Ni/Co/Fe atoms in the precursors. By virtue of the unique structure and enriched oxygen vacancies originated from well-modulated electronic structures, the 3D PG-NiCoFe-211 NAs exhibited outstanding electrocatalytic performances for oxygen evolution reaction (OER) in alkaline solution, outperforming commercial RuO2 catalyst. The current incorporation of foreign metal atom into host material provides some valuable insights into design and synthesis of metal-based nanocatalysts for constructing practical water splitting devices.

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Niobium oxyphosphate nanosheet assembled two-dimensional anode material for enhanced lithium storage Bo Wen, Ruiting Guo, Xiong Liu, Wen Luo, Qiu He, Chaojiang Niu, Jiashen Meng, Qi Li, Yan Zhao, Liqiang Mai 2021, 53(2): 268-275.  DOI: 10.1016/j.jechem.2020.05.004 Abstract ( 5 )   PDF (3869KB) ( 2 )   The development of high-capacity and high-rate anodes has become an attractive endeavor for achieving high energy and power densities in lithium-ion batteries (LIBs). Herein, a new-type anode material of reduced graphene oxide (rGO) supported niobium oxyphosphate (NbOPO4) nanosheet assembled two-dimensional composite material (NbOPO4/rGO) is firstly fabricated and presented as a promising high-performance LIB anode material. In-depth electrochemical analyses and in/ex situ characterizations reveal that the intercalation-conversion reaction takes place during the first discharge process, followed by the reversible redox process between amorphous NbPO4 and Nb which contributes to the reversible capacity in the subsequent cycles. Meanwhile, the lithiation-generated Li3PO4, behaving as a good lithium ion conductor, facilitates ion transport. The rGO support further regulates the structural and electron/ion transfer properties of NbOPO4/rGO composite compared to neat NbOPO4, resulting in greatly enhanced electrochemical performances. As a result, NbOPO4/rGO as a new-type LIB anode material achieves a high capacity of 502.5 mAh g-1 after 800 cycles and outstanding rate capability of 308.4 mAh g-1 at 8 A g-1. This work paves the way for the deep understanding and exploration of phosphate-based high-efficiency anode materials for LIBs.

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Reaction mechanism and additional lithium storage of mesoporous MnO2 anode in Li batteries Jaesang Yoon, Woosung Choi, Taewhan Kim, Hyunwoo Kim, Yun Seok Choi, Ji Man Kim, Won-Sub Yoon 2021, 53(2): 276-284.  DOI: 10.1016/j.jechem.2020.05.029 Abstract ( 3 )   PDF (5786KB) ( 2 )   Nanostructured transition metal oxides, employed as anode materials for lithium-ion batteries, exhibit a higher capacity than the theoretical capacity based on the conversion reaction. To date, the reasons behind this phenomenon are unclear. For the one-step evolution of anode material for lithium-ion batteries, it is essential to understand the lithium storage reaction mechanism of the anode material. Herein, we provide a detailed report on the lithium storage and release mechanism of MnO2, using synchrotron-based X-ray techniques. X-ray diffraction and X-ray absorption spectroscopy results indicate that during the first discharge, MnO2 is reduced in the order of MnO2 → LixMnO2 (1<X<2) → MnO → Mn metal, followed by a reversible reaction between Mn metal and Mn3O4. Furthermore, soft X-ray absorption spectroscopy results indicate that additional reversible formation-decomposition of the electrolyte-derived surface layer occurs and contributes to the reversible capacity of MnO2 after the first discharge. These findings contribute to further understanding of the reaction mechanism and additional lithium storage of MnO2 and suggest practical strategies for developing high energy density anode materials for next-generation Li batteries.

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Degradation diagnosis of lithium-ion batteries using AC impedance technique in fixing the state of charge of an electrode Keisuke Ando, Tomoyuki Matsuda, Daichi Imamura 2021, 53(2): 285-289.  DOI: 10.1016/j.jechem.2020.04.072 Abstract ( 6 )   PDF (707KB) ( 4 )

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Recent advances in spinel-type electrocatalysts for bifunctional oxygen reduction and oxygen evolution reactions Xiao-Meng Liu, Xiaoyang Cui, Kamran Dastafkan, Hao-Fan Wang, Cheng Tang, Chuan Zhao, Aibing Chen, Chuanxin He, Minghan Han, Qiang Zhang 2021, 53(2): 290-302.  DOI: 10.1016/j.jechem.2020.04.012 Abstract ( 12 )   PDF (11411KB) ( 5 )   The demand for efficient and environmentally-benign electrocatalysts that help availably harness the renewable energy resources is growing rapidly. In recent years, increasing insights into the design of water electrolysers, fuel cells, and metal-air batteries emerge in response to the need for developing sustainable energy carriers, in which the oxygen evolution reaction and the oxygen reduction reaction play key roles. However, both reactions suffer from sluggish kinetics that restricts the reactivity. Therefore, it is vital to probe into the structure of the catalysts to exploit high-performance bifunctional oxygen electrocatalysts. Spinel-type catalysts are a class of materials with advantages of versatility, low toxicity, low expense, high abundance, flexible ion arrangement, and multivalence structure. In this review, we afford a basic overview of spinel-type materials and then introduce the relevant theoretical principles for electrocatalytic activity, following that we shed light on the structure-property relationship strategies for spinel-type catalysts including electronic structure, microstructure, phase and composition regulation, and coupling with electrically conductive supports. We elaborate the relationship between structure and property, in order to provide some insights into the design of spinel-type bifunctional oxygen electrocatalysts.

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Fe, V-co-doped C2N for electrocatalytic N2-to-NH3 conversion Zengxi Wei, Jian He, Yulu Yang, Zhenhai Xia, Yuezhan Feng, Jianmin Ma 2021, 53(2): 303-308.  DOI: 10.1016/j.jechem.2020.04.014 Abstract ( 4 )   PDF (7021KB) ( 3 )   Designing providential catalyst is the key to drive the electrochemical nitrogen reduction reactions (NRR), which is referring to multiple intermediates and products. By means of density functional theory (DFT) calculations, we studied heteronuclear bi-atom electrocatalyst (HBEC) for NRR. Our results revealed that compared to homonuclear bi-atom electrocatalyst (Fe2@C2N, V2@C2N), Fe, V-co-doped C2N (FeV@C2N) had a smaller limiting potential of -0.17 V and could accelerate N2-to-NH3 conversion through the enzymatic pathway of NRR. Importantly, N-N bond length monotonically increases with increasing the Bader charges of adsorbed N2 molecule but decreases with increasing the Bader charge difference of two adsorbed N atoms. Additionally, the FeV@C2N could suppress the production of H2 by the preferential adsorption and reduction of N2 molecule. Thus, the as-designed HBEC may have the outstanding electrochemical NRR performance. This work opens a new perspective for NRR by HBECs under mild conditions.

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Plasmonic CsPbBr3-Au nanocomposite for excitation wavelength dependent photocatalytic CO2 reduction Jin-Feng Liao, Ya-Ting Cai, Jun-Yan Li, Yong Jiang, Xu-Dong Wang, Hong-Yan Chen, Dai-Bin Kuang 2021, 53(2): 309-315.  DOI: 10.1016/j.jechem.2020.04.017 Abstract ( 4 )   PDF (11901KB) ( 2 )   The optoelectronic performance of CsPbBr3 nanocrystal (NC) has been dramatically limited by the severe charge carrier recombination and its narrow light absorption range, which are anticipated to be resolved via coupling with plasmonic Au nanoparticle (NP). In view of this, CsPbBr3-Au nanocomposite is fabricated and further employed as a concept model to study the electronic interaction between perovskite NC and Au NP for the first time. It has been found that the excitation-wavelength dependent carrier transfer behavior exists in CsPbBr3-Au nanocomposite. Upon illumination with visible light (λ >420 nm), photo-generated electrons in CsPbBr3 can inject into Au with an electron injection rate and efficiency of 2.84 × 109 s-1 and 78%, respectively. The boosted charge separation is further translated into a 3.2-fold enhancement in CO2 photocatalytic reduction activity compared with pristine CsPbBr3. On the other hand, when solely exciting Au NP with longer wavelength light (λ >580 nm), the localized surface plasmon resonance (LSPR) induced hot electrons in Au NPs can transfer to CsPbBr3 NC and further participate in photocatalytic reaction towards CO2 reduction. The present study provides new insights into preparing plasmonic nanostructure to enhance the performance of perovskite based optoelectronic devices.

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Influence of interlayer water molecules in Ni-based catalysts for oxygen evolution reaction Liutao Huang, Lei Yang, Siwei Guo, Yang Li, Lihua Zhao, Lifang Jiao 2021, 53(2): 316-322.  DOI: 10.1016/j.jechem.2020.05.042 Abstract ( 2 )   PDF (9373KB) ( 1 )   Nickel-iron layered double hydroxides (NiFe LDHs) have been identified as one of the best promising electrocatalysts-candidates for oxygen evolution reaction (OER). However, the catalytic activity effected by interlayer water molecules is ignored and rarely reported. Herein, Ni(OH)2, NiFe LDHs vertically aligned Ni foam are designed for OER. As a contrast, the corresponding electrocatalysts with the removal of the interlayer water molecules (Ni(OH)2-AT, NiFe LDHs-AT) are developed to probe into the influence of the interlayer water molecules towards OER. As expected, NiFe LDH nanoplates exhibit excellent catalytic performance and durability for water electrolysis in alkaline conditions with lower overpotential and smaller Tafel slope compared to those of NiFe LDHs-AT, which are influenced mainly by stability of crystal structure due to the existence of interlayer water molecules. The discovery opens up a similar pathway by controlling the amount of water molecules to boost catalytic performance for studying other electrocatalysts with heteroatom dopant.

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In situ Raman spectroscopy reveals the mechanism of titanium substitution in P2-Na2/3Ni1/3Mn2/3O2: Cathode materials for sodium batteries Xiao-Bin Zhong, Chao He, Fan Gao, Zhong-Qun Tian, Jian-Feng Li 2021, 53(2): 323-328.  DOI: 10.1016/j.jechem.2020.05.018 Abstract ( 3 )   PDF (4488KB) ( 4 )   Layered P2-Na2/3Ni1/3Mn2/3O2 is a promising cathode material. It exhibits a high capacity and suitable operating voltage and undergoes a phase transition from P2 to O2 during charge/discharge. Researchers have used Ti substitution to improve the cathode, yet the chemical principles that underpin elemental substitution and functional improvement remain unclear. To clarify these principles, we used in situ Raman spectroscopy to monitor chemical changes in P2-Na2/3Ni1/3Mn1/3Ti1/3O2 and P2-Na2/3Ni1/3Mn2/3O2 during charge/discharge. Based on the change in the A1g and Eg peaks during charge/discharge, we concluded that Ti substitution compressed the transition metal layer and expanded the planar oxygen layer in the unit cell. Titanium stabilized the P2 phase structure, which improved the cycling stability of P2-NaNMT. Our results provide clear theoretical support for future research on modifying electrodes by elemental substitution.

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Catalytic hydrotreatment of humins into cyclic hydrocarbons over solid acid supported metal catalysts in cyclohexane Junmin Sun, Hai Cheng, Yao Zhang, Yinmin Zhang, Xunfeng Lan, Yongfeng Zhang, Qineng Xia, Daqian Ding 2021, 53(2): 329-339.  DOI: 10.1016/j.jechem.2020.05.034 Abstract ( 6 )   PDF (2573KB) ( 2 )   Humins are common undesirable sideproducts during many acid-catalyzed reactions in renewable biomass platform conversion. However, few studies have been reported to the efficient utilization of humins. For the first time, the selective catalytic conversion of biomass-derived humins into cyclic hydrocarbons with high conversion rate and selectivity is presented using a home-made Ru/W-P-Si-O bifunctional catalyst. The multistage polymerization structure of humins was studied through controlled experiments. Results show that the C-C bond network can be efficiently depolymerized at a mild reaction temperature of 340-380 °C, catalyzed by the cooperative catalysis of nano-Ru particles and porous strong Lewis solid acid. Particularly, 95.4% conversion of humins was achieved under the optimal condition with up to 88.3% yield of cyclic hydrocarbons. The detailed composition after liquefaction was also analyzed. This study paves the way for the efficient production of cyclic and aromatic hydrocarbons from furan-derived humin polymer through Lewis acid-catalyzed Diels-Alder reactions between furan rings.

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A strategy to achieve high loading and high energy density Li-S batteries Fei Yin, Qi Jin, Hong Gao, XiTian Zhang, ZhiGuo Zhang 2021, 53(2): 340-346.  DOI: 10.1016/j.jechem.2020.05.014 Abstract ( 3 )   PDF (2244KB) ( 2 )   Lithium-sulfur (Li-S) batteries are one of the most promising rechargeable storage devices due to the high theoretical energy density. However, the low areal sulfur loading impedes their commercial development. Herein, a 3D free-standing sulfur cathode scaffold is rationally designed and fabricated by coaxially coating polar Ti3C2Tx flakes on sulfur-impregnated carbon cloth (Ti3C2Tx@S/CC) to achieve high loading and high energy density Li-S batteries, in which, the flexible CC substrate with highly porous structure can accommodate large amounts of sulfur and ensure fast electron transfer, while the outer-coated Ti3C2Tx can serve as a polar and conductive protective layer to further promote the conductivity of the whole electrode, achieve physical blocking and chemical anchoring of lithium-polysulfides as well as catalyze their conversion. Due to these advantages, at a sulfur loading of 4 mg cm-2, Li-S cells with Ti3C2Tx@S/CC cathodes can deliver outstanding cycling stability (746.1 mAh g-1 after 200 cycles at 1 C), superb rate performance (866.8 mAh g-1 up to 2 C) and a high specific energy density (564.2 Wh kg-1 after 100 cycles at 0.5 C). More significantly, they also show the commercial potential that can compete with current lithium-ion batteries due to the high areal capacity of 6.7 mAh cm-2 at the increased loading of 8 mg cm-2.

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Reversible potassium storage in ultrafine CFx: A superior cathode material for potassium batteries and its mechanism Hongjun Yue, Huixin Chen, Chen Zhao, Zhiming Zheng, Ke Zhou, Qiaobao Zhang, Guiming Zhong, Can-Zhong Lu, Yong Yang 2021, 53(2): 347-353.  DOI: 10.1016/j.jechem.2020.05.024 Abstract ( 3 )   PDF (2861KB) ( 2 )   Current studies of cathodes for potassium batteries (PBs) mainly focus on the intercalation-type materials. The conversion-type materials that possess much higher theoretical capacities are rarely discussed in previous literatures. In this work, carbon fluoride (CFx) is reported as a high capacity conversion-type cathode for PBs for the first time. The material delivers a remarkable discharge capacity of >250 mAh g-1 with mid-voltage of 2.6 V at 20 mA g-1. Moreover, a highly reversible capacity of around 95 mAh g-1 is achieved at 125 mA g-1 and maintained for 900 cycles, demonstrating its excellent cycling stability. The mechanism of this highly reversible conversion reaction is further investigated by nuclear magnetic resonance spectra, X-ray diffraction, and transmission electron microscopy studies. According to the analyses, the C-F bond in the cycled material is different from that in the pristine state, which presents relatively higher reversibility. This finding offers important insights for further improving the performance of the CFx. This work not only demonstrates the CFx as a high performance cathode for PBs, but also paves a new avenue of exploring conversion-type cathodes for high energy density PBs.

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A perspective on graphene for supercapacitors: Current status and future challenges Feng Su, Zhong-Shuai Wu 2021, 53(2): 354-357.  DOI: 10.1016/j.jechem.2020.05.041 Abstract ( 5 )   PDF (2307KB) ( 3 )

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Carambola-like metal-organic frameworks for high-performance electrocatalytic oxygen evolution reaction Zhi Gao, Longhui Xiao, Xuemin Su, Xiangqing He, Yi Yu, Xinhui Huang, Feng Luo 2021, 53(2): 358-363.  DOI: 10.1016/j.jechem.2020.05.023 Abstract ( 6 )   PDF (4750KB) ( 2 )

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Melamine-assisted pyrolytic synthesis of bifunctional cobalt-based core-shell electrocatalysts for rechargeable zinc-air batteries Jiqing Jiao, Yuan Pan, Bin Wang, Wenjuan Yang, Shoujie Liu, Chao Zhang 2021, 53(2): 364-371.  DOI: 10.1016/j.jechem.2020.05.032 Abstract ( 3 )   PDF (5611KB) ( 2 )   Designing a highly active- and stable non-noble metal bifunctional oxygen catalyst for rechargeable Zn-air battery remains a great challenge. Herein, we develop a facile and melamine-assisted-pyrolysis (MAP) strategy for the synthesis of core-shell Co-based electrocatalysts@N-doped carbon nanotubes (Co@CNTs) derived from metal-organic frameworks. The Co@CNTs exhibited excellent bifunctional electrocatalytic performance for both oxygen evolution and reduction. DFT calculations demonstrated that the Gibbs free energy of the rate-determining step was small enough to improve ORR activities. As a result, a Zn-air battery assembled with Co@CNTs proves a lager power density, low voltage gap between charge-discharge and excellent stability. Thus, this work offers a facile strategy to realize the synthesis of non-noble metal electrocatalyst for Zn-air battery materials with high electrochemical performance.

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Dual interfacial engineering for efficient Cs2AgBiBr6 based solar cells Tao Luo, Yalan Zhang, Xiaoming Chang, Junjie Fang, Tianqi Niu, Jing Lu, Yuanyuan Fan, Zicheng Ding, Kui Zhao, ShengzhongLiu 2021, 53(2): 372-378.  DOI: 10.1016/j.jechem.2020.05.016 Abstract ( 4 )   PDF (3708KB) ( 4 )   The emerging lead-free halide double perovskite solar cells have attracted widespread attentions due to their long-term stability and non-toxicity, but suffer from the low device performance. One efficiency-limiting factor is the improper contacts between the halide double perovskite and anode/cathode electrodes. Here, we improve the efficiency and stability of the bismuth-halide double perovskite based solar cells by a synergistic interface design for both electron and hole transport layers (ETL/HTL). The results show that the modification of the TiO2 ETL with a thin hydrophobic C60 layer and replacement of the lithium-doped small molecule HTL with an un-doped conjugated polymer lead to higher surface quality of perovskite film and better energy-level alignment at the contacts. As a result, the optimized device shows reduced trap density, suppressed charge recombination and enhanced charge extraction, leading to an increase of 69% in device efficiency. In addition, the device also exhibits superior stability in ambient environment, heat stress and light bias after interface optimization. This work provides an efficient strategy for the device optimization of the emerging lead-free perovskite solar cells.

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Growth mechanisms for spherical Ni0.815Co0.15Al0.035(OH)2 precursors prepared via the ammonia complexation precipitation method Xi Yang, Xuesong Huang, Hancheng Shi, Peng Dong, Ding Wang, Jianguo Duan, Yingjie Zhang 2021, 53(2): 379-386.  DOI: 10.1016/j.jechem.2020.05.049 Abstract ( 3 )   PDF (4790KB) ( 2 )   The microstructures of precursors strongly affect the electrochemical performance of Ni-rich layer-structured cathode materials. In this study, the growth behaviour of Ni0.815Co0.15Al0.035(OH)2 (NCA) prepared via the ammonia complexation precipitation method in a 50-L-volume continuously stirred tank reactor (CSTR) is studied in detail. The growth of Ni(OH)2-based hydroxide can be divided into a nucleation process, an agglomeration growth process, a process in which multiple growth mechanisms coexist, and an interface growth process over time, while the inner structure of the CSTR can be divided into a nucleation zone, a complex dissolution zone, a growth zone, and a maturation zone. The concentration of ammonium ions affects the growth habit of the primary crystal significantly due to its specific adsorption on the electronegative crystal plane. When the ammonia concentration is <1.5 mol L-1 at 60 °C at pH = 11.5, the precursors grow preferentially along the (1 0 1) crystal plane, whereas they grow preferentially along the (0 0 1) crystal plane when the concentration is >2.0 mol L-1. The LiNi0.815Co0.15Al0.035O2 materials inherit the grain structure of the precursor. Materials prepared from precursors with (1 0 1) preferential primary particles show a higher specific capacity and better rate performance than those that were prepared from (0 0 1) preferential primary particles, but the latter realize a better cycling performance than the former.

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Nb2CTx MXene: High capacity and ultra-long cycle capability for lithium-ion battery by regulation of functional groups Jiabao Zhao, Jing Wen, Junpeng Xiao, Xinzhi Ma, Jiahui Gao, Lina Bai, Hong Gao, Xitian Zhang, Zhiguo Zhang 2021, 53(2): 387-395.  DOI: 10.1016/j.jechem.2020.05.037 Abstract ( 5 )   PDF (5397KB) ( 2 )   MXenes are well known for their potential application in supercapacitors due to their high-rate intercalation pseudocapacitance and long cyclability. However, the reported low capacity of pristine MXenes hinders their practical application in lithium-ion batteries. In this work, a robust strategy is developed to control the functional groups of Nb2CTx MXene. The capacity of pristine Nb2CTx MXene can be significantly increased by Li+ intercalation and surface modification. The specific capacity of the treated Nb2CTx is up to 448 mAh g-1 at 0.05 A g-1, and at a large current density of 2 A g-1 remains a high reversible capacity retention rate of 75% after an ultra-long cycle of 2000 cycles. These values exceed most of the reported pristine MXenes (including the most studied Ti3C2Tx) and carbon-based materials. It demonstrates that this strategy has great help to improve the electrochemical performance of pristine MXene, and the results enhance the promise of MXenes in the application of lithium-ion batteries.

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Advanced metal-organic frameworks for aqueous sodium-ion rechargeable batteries Dongkyu Choi, Seonguk Lim, Dongwook Han 2021, 53(2): 396-406.  DOI: 10.1016/j.jechem.2020.07.024 Abstract ( 10 )   PDF (3715KB) ( 4 )   Inexpensive and abundant sodium resources make energy storage systems using sodium chemistry promising replacements for typical lithium-ion rechargeable batteries (LIBs). Fortuitously, aqueous sodium-ion rechargeable batteries (ASIBs), which operate in aqueous electrolytes, are cheaper, safer, and more ionically conductive than batteries that operate in conventional organic electrolytes; furthermore, they are suitable for grid-scale energy storage applications. As electrode materials for storing Na+ ions in ASIBs, a variety of multifunctional metal-organic frameworks (MOFs) have demonstrated great potential in terms of having porous 3D crystal structures, compatibility with aqueous solutions, long cycle lives (≥1000 cycles), and ease of synthesis. The present review describes MOF-derived technologies for the successful application of MOFs to ASIBs and suggests future challenges in this area of research based on the current understanding.

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Hot Debate on Perovskite Solar Cells: Stability, Toxicity, High-Efficiency and Low Cost Zhou Yang, Hui Wang, Min Huang, Yang Liu, Qunbo Lv, Fang Lv, Xiaodan Zhang, Ying Zhao, ShengzhongLiu 2021, 53(2): 407-411.  DOI: 10.1016/j.jechem.2020.04.028 Abstract ( 3 )   PDF (1138KB) ( 2 )

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Porous conductive interlayer for dendrite-free lithium metal battery Hui Liu, Daichong Peng, Tianye Xu, Kedi Cai, Kening Sun, Zhenhua Wang 2021, 53(2): 412-418.  DOI: 10.1016/j.jechem.2020.07.030 Abstract ( 5 )   PDF (6306KB) ( 2 )   Lithium (Li) metal, possessing ultrahigh theoretical capacity and the lowest electrode potential, is regarded as a promising new generation anode material. However, the uncontrollable growth of Li dendrites during cycling process gives rise to problems as capacity decay and short circuit, suppressing the cycling and safety performances of Li metal battery. In this contribution, porous conductive interlayer (PCI), composed of carbon nanofibers (CNFs) and polyisophthaloyl metaphenylene diamine (PMIA), is developed to suppress Li dendrites and stabilize Li metal anode. PCI possesses the excellent conductive ability of CNFs and the preeminent mechanical properties of PMIA at the same time. When Li metal contacts with PCI during cycling process, an equipotential surface forms on their interface, which eliminates the tip effect on Li anode and homogenizes Li-ions flux in combination with the uniform porous structure of PCI. Employed PCI, the Li|Cu cell exhibits a remarkable cycling stability with a high average Coulombic efficiency of 97.5% for 100 cycles at 0.5 mA cm-2. And the Li|LiFePO4 cell exhibits improved rate capability (114.7 mAh g-1 at 5.0 C) and enhanced cycling performance (78.9% capacity retention rate over 500 cycles at 1.0 C). This work provides a fresh and effective solving strategy for the problem of dendrites in Li metal battery.

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Amines modulation and passivation yields record perovskite optoelectronic devices Wenhuai Feng, Wu-Qiang Wu, Liming Ding 2021, 53(2): 419-421.  DOI: 10.1016/j.jechem.2020.07.052 Abstract ( 6 )   PDF (1258KB) ( 2 )

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Carbon hybrid with 3D nano-forest architecture in-situ catalytically constructed by CoFe alloy as advanced multifunctional electrocatalysts for Zn-air batteries-driven water splitting Shuguang Wang, Jie Wang, Xin Wang, Long Li, Jinwen Qin, Minhua Cao 2021, 53(2): 422-432.  DOI: 10.1016/j.jechem.2020.07.045 Abstract ( 3 )   PDF (7370KB) ( 1 )   Rational design and facile synthesis of non-noble materials as the effective multifunctional electrocatalysts are still challenging. Herein, a self-catalytically grafted growth approach is developed to construct carbon hybrid with three-dimensional (3D) nano-forest architecture via controlled pyrolysis of metal-polymer nanofiber precursor and melamine. The metal-polymer nanofibers act as the matrix, and melamine is used as the initiator for orientated growth of one-dimensional (1D) N-doped carbon nanotubes (N-CNTs) on carbon nanofibers. The as-prepared CoFe-N-CNTs/CNFs-900 possesses unique structure and component advantages in terms of 3D structure, special synapse-like structure, porous feature, high-level N doping and bimetallic active components, which endow the material with structural stability, high mass/electron transport ability and large active sur-/interfaces. Benefiting from the integrated effects of all the above factors, CoFe-N-CNTs/CNFs were successfully applied to overall water splitting and Zn-air batteries. It is believed that this integrated design methodology can be extended to prepare other M-N-C materials for energy-related electrochemical reactions.

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Writing ink-promoted synthesis of electrodes with high energy storage performance: A review Yi Feng, Jingqiu Li, Rongrong Tian, Jianfeng Yao 2021, 53(2): 433-440.  DOI: 10.1016/j.jechem.2020.05.031 Abstract ( 4 )   PDF (3377KB) ( 2 )   As the low-cost commercial product, writing inks (pen ink and Chinese ink) have attracted great attention to fabricate electrochemical electrodes for supercapacitors (SCs) and batteries. Due to the conductive nature deriving from graphitic carbon nanoparticles in ink and strong adhesion, ink can be easily coated onto support to enhance the conductivity, form a porous layer facilitating electrolyte ion diffusion, increase the specific surface area and function as binder and dispersant for other active materials. In this review, the beneficial features of pen ink and Chinese ink are summarized and how these features favor the electrochemical performance is discussed in details. And then, ways to coat ink onto support are described, giving a clear understanding of recent process in this area. Finally, the current challenges and outlook of ink-based electrode are discussed, aiming to offer some basic knowledge and promote wide application and future study of pen ink and Chinese ink in electrochemistry.