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2020, Vol. 48, No. 9　Online: 2020-09-15

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Promoted CO2 electroreduction over indium-doped SnP3: A computational study Yuefeng Zhang, Wenchao Zhang, Yuezhan Feng, Jianmin Ma 2020, 48(9): 1-6.  DOI: 10.1016/j.jechem.2019.12.025 摘要 ( 5 )   It is generally considered that the hydrogenation of CO2 is the critical bottleneck of the CO2 electroreduction.In this work.with the aid of density functional theory (DFT) calculations.the catalytic hydrogenation of CO2 molecules over Indium-doped SnP3 catalyst were systematically studied.Through doping with indium (In) atom.the energy barrier of CO2 protonation is reduced and OCHO* species could easily be generated.This is mainly due to the p orbital of In exhibits strong hybridization with the p orbital of O.indicating that there is a strong interaction between OCHO* and In-doped SnP3 catalyst.As a result.In-doped SnP3 possesses high-efficiency and high-selectivity for converting CO2 into HCOOH with a low limiting potential of -0.17 V.Our findings will offer theoretical guidance to CO2 electroreduction.

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In-situ electrochemical functionalization of carbon materials for high-performance Li-O2 batteries Jungwon Kang, Jin Min Kim, do Youb Kim, Jungdon Suk, Jaekook Kim, dong Wook Kim, Yongku Kang 2020, 48(9): 7-13.  DOI: 10.1016/j.jechem.2019.12.016 摘要 ( 13 )   The development of effective synthetic routes is important to manifest proper nature of specific materials.In-situ electrochemical functionalization possesses great advantages over conventional routes.especially facile way and leading to reaching elaborate sites of functional group.Here.we demonstrate the preparation of functionalized carbons by in-situ electrochemical reduction in an argon atmosphere for application in low-cost.environmentally benign.and high-performance oxygen-electrodes for non-aqueous Li-O2 batteries.A Li-O2 battery with functionalized carbon shows a high discharge capacity (100 times that of pristine carbon).high power and cycling stability.The outstanding performance is attributed to the high O2 affinity of the functionalized carbon surface that facilitates the formation of soluble and diffusible superoxide intermediates by the reduction of the remaining O2 competing with surface growth for Li2O2 formation.

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Aqueous K-ion battery incorporating environment-friendly organic compound and Berlin green Mingtan Wang, Huaiqing Wang, Huamin Zhang, Xianfeng Li 2020, 48(9): 14-20.  DOI: 10.1016/j.jechem.2019.12.019 摘要 ( 26 )   Aqueous rechargeable metal-ion batteries (ARMBs) hold intrinsic advantages of high safety.low cost and environmental benignity for large scale energy storage technologies.However.the research on aqueous Kion batteries (AKIBs) was hindered by limited materials.Herein.a novel AKIB was reported by employing environment-friendly 1,4,5,8-naphthalenetetracarboxylic dianhydride-derived polyimide (PNTCDA) as anode and Berlin green (FeHCF) as cathode.Both electrodes have high rate performance and excellent capacity retention during cycling.Kinetics researches verify the superior electrochemical property of PNTCDA in saturated KNO3 solution.In-situ XRD of FeHCF demonstrates the unique shift of peak position and negligible distortion of lattice during the insertion/extraction of K+.The AKIB exhibits an attractive energy density of 46.9 Wh/kg and a high capacity retention of 74% in 300 cycles.More importantly.the battery can reach a super-high power of 2079.1 W/kg with an energy density of 24.2 Wh/kg.ranking relatively high among the ARIMs.This system extends the use of polyimide and points a way of AKIBs for grid-scale energy storage.

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Reinventing the mechanism of high-performance Bi anode in aqueous K+ rechargeable batteries Tingting Qin, Xuefeng Chu, Ting Deng, boran Wang, Xiaoyu Zhang, Taowen Dong, Zhengming Li, Xiaofeng Fan, Xin Ge, Zizhun Wang, Peng Wang, Wei Zhang, Weitao Zheng 2020, 48(9): 21-28.  DOI: 10.1016/j.jechem.2019.12.012 摘要 ( 14 )   Increasing attention has been paid to rechargeable aqueous batteries due to their high safety and low cost.However.they remain in their infancy because of the limited choice of available anode materials with high specific capacity and satisfying cycling performance.Bi metal with layered structure can act as an ideal anode material with high capacity;however.the energy storage mechanism has not well elucidated.Herein.we demonstrate that Bi metal enables affording ultra-high specific capacity (254.3 mAh g-1).superior rate capability and a capacity retention of 88.8% after 1600 cycles.Different from the previously-reported redox reaction mechanisms of Bi electrode.efficient (de)alloying of K+ is responsible for its excellent performance.An excellent aqueous Bi battery is fabricated by matching Bi anode with Co(OH)2 cathode in KOH (1 M) electrolyte.Its outstanding performance is quite adequate and competitive for electrochemical energy storage devices.

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Strategies for enhancing conductivity of colloidal nanocrystals and their photoelectronic applications Fen Qiao, Yi Xie 2020, 48(9): 29-42.  DOI: 10.1016/j.jechem.2019.12.022 摘要 ( 5 )   Semiconductor colloidal nanocrystals (NCs) have size- and shape-dependent optoelectronic properties due to the quantum confinement effect.and are considered to be promising optoelectronic materials.Among them.II-VI (CdSe.CdS.CdTe.etc.) and IV-VI (PbSe.PbTe.PbS.etc.) have been widely studied as representative colloidal NCs.However.the surfactant used in its synthesis progress results in the NCs surface covered by an insulating shell.which greatly affects the exciton separation and carrier transport of colloidal NCs-based photovoltaic devices.Therefore.how to design high-efficiency optoelectronic devices by improving the transport performance of carriers has been a great challenge.The key issues in the research of II-VI (CdSe.CdS.CdTe.etc.) and IV-VI (PbSe.PbTe.PbS.etc.) colloidal NCs were summarized.including synthesis strategy.morphology/size adjustment.surface ligand design.improvement of conductivity and their optoelectronic properties.The influence of surface ligands on the stability and dispersion of NCs was firstly introduced.and then strategies of improving electrical conductivity of NCs were discussed.such as ligands exchange.doping.self-assembly and plasmons.which provided a good foundation for the subsequent preparation of optoelectronic devices.The future development direction of NCs optoelectronic devices is expounded from the aspects of materials composition.comprehensive preparation and flexible processing of colloidal NCs.

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Interface electron collaborative migration of Co-Co3O4/carbon dots: Boosting the hydrolytic dehydrogenation of ammonia borane Han Wu, Min Wu, boyang Wang, Xue Yong, Yushan Liu, baojun Li, baozhong Liu, Siyu Lu 2020, 48(9): 43-53.  DOI: 10.1016/j.jechem.2019.12.023 摘要 ( 14 )   Ammonia borane (AB) is an excellent candidate for the chemical storage of hydrogen.However.its practical utilization for hydrogen production is hindered by the need for expensive noble-metal-based catalysts.Herein.we report Co-Co3O4 nanoparticles (NPs) facilely deposited on carbon dots (CDs) as a highly efficient.robust.and noble-metal-free catalyst for the hydrolysis of AB.The incorporation of the multiinterfaces between Co.Co3O4 NPs.and CDs endows this hybrid material with excellent catalytic activity (rB=6816 mLH2 min-1 gCo-1) exceeding that of previous non-noble-metal NP systems and even that of some noble-metal NP systems.A further mechanistic study suggests that these interfacial interactions can affect the electronic structures of interfacial atoms and provide abundant adsorption sites for AB and water molecules.resulting in a low energy barrier for the activation of reactive molecules and thus substantial improvement of the catalytic rate.

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Tuning combined steam and dry reforming of methane for "metgas" production: A thermodynamic approach and state-of-the-art catalysts Karam Jabbour 2020, 48(9): 54-91.  DOI: 10.1016/j.jechem.2019.12.017 摘要 ( 29 )   Nowadays.combined steam and dry reforming of methane (CSDRM) is viewed as a new alternative for the production of high-quality syngas (termed as "metgas".H2:CO of 2.0) suitable for subsequent synthesis of methanol.considered as a promising renewable energy vector to substitute fossil fuel resources.Adequate operation conditions (molar feed composition.temperature and pressure) are required for the sole production of "metgas" while achieving high CH4.CO2 and H2O conversion levels.In this work.thermodynamic equilibrium analysis of CSDRM has been performed using Gibbs free energy minimization where;(i) the effect of temperature (range:200-1000℃).(ii) feed composition (stoichiometric ratio as compared to a feed under excess steam or excess carbon dioxide).(iii) pressure (range:1-20 bar) and.(iv) the presence of a gaseous diluent on coke yields.reactivity levels and selectivity towards "metgas" were investigated.Running CSDRM at a temperature of at least 800℃.a pressure of 1 bar and under a feed composition where CO2+H2O/CH4 is around 1.0.are optimum conditions for the theoretical production of "metgas" while minimizing C(s) formation for longer experimental catalytic runs.A second part of this work presents a review of the recent progresses in the design of (principally) Ni-based catalysts along with some mechanistic and kinetic modeling aspects for the targeted CSDRM reaction.As compared to noble metals.their high availability.low cost and good intrinsic activity levels are main reasons for increasing research dedications in understanding deactivation potentials and providing amelioration strategies for further development.Deactivation causes and main orientations towards designing deactivationresistant supported Ni nanoparticles are clearly addressed and analyzed.Reported procedures based on salient catalytic features (i.e..acidity/basicity character.redox properties.oxygen mobility.metal-support interaction) and recently employed innovative tactics (such as confinement within mesoporous systems.stabilization through core shell structures or on carbide surfaces) are highlighted and their impact on Ni0 reactivity and stability are discussed.The final aspect of this review encloses the major directions and trends for improving synthesis/preparation designs of Ni-based catalysts for the sake of upgrading their usage into industrially oriented combined reforming operations.

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Electrophoretically deposited binder-free 3-D carbon/sulfur nanocomposite cathode for high-performance Li-S batteries Sasan Ghashghaie, Samson Ho-Sum Cheng, Jie Fang, Hafiz Khurram Shahzad, Robin Lok-Wang Ma, chi-Yuen Chung 2020, 48(9): 92-101.  DOI: 10.1016/j.jechem.2019.12.015 摘要 ( 4 )   In the present study.the electrophoretic deposition method was successfully applied as a binder-free and scalable approach to deposit carbonaceous nanomaterials on carbon fiber paper (CFP) for cathode applications in Li-S batteries.The microstructural studies of the EPD-CNT film using scanning electron microscopy (SEM) revealed the formation of a crack-free and porous layer of CNTs being uniformly distributed on the CFP surface.The EPD:CFP/CNT/S cathode delivered a capacity around 2.2 times higher than that obtained in the absence of the EPD-CNT film (CFP/S cell) after 50 cycles and a capacity of 935 mAh g-1 after 100 cycles at 0.1 C.The EPD method was then employed to fabricate layer-by-layer structures where the EPD-CNT film was decorated with carbon black particles.The initial capacity as well as the reversible capacity after 100 cycles was further increased by the EPD:CFP/CNT/KB/S layer-by-layer structure to 1473 and 1033 mAh g-1.respectively.indicating effective suppression of the shuttle effect.In addition.the rate performance of CFP/S was improved by depositing the EPD-CNT and EPD-CNT/carbon black architectures on CFP surface.and even further enhanced through the co-deposition of CNT and Pt nanoparticles by EPD.delivering a specific capacity of around 730 mAh g-1 at 1 C.Finally.the cathodes fabricated by EPD were observed to outperform those made by the conventional casting method in terms of cycling performance.internal resistance.and polarization.This difference was ascribed to the non-uniform microstructure of the Cast-CNT film.which resulted in poor interfacial connection between the CNT agglomerates.hindering uniform sulfide/sulfur deposition during cycling.The obtained results suggested that the binder-free C/S nanocomposite cathode made by EPD is key to further enhance the specific capacity and energy density of Li-S batteries.

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Na3.8[Sn0.67Si0.33]0.8Sb0.2S4:A quinary sodium fast ionic conductor for all-solid-state sodium battery Huanhuan Jia, Linfeng Peng, Zhuoran Zhang, Tao An, Jia Xie 2020, 48(9): 102-106.  DOI: 10.1016/j.jechem.2019.12.021 摘要 ( 10 )   Strategy of Sb-substitution is carried out on the template structure Na4Sn0.67M0.33S4 (M=Si.Ge).which affords a series of quinary sulfide-based sodium fast ionic conductors formulated as Na4-x[Sn0.67M0.33]1-xSbxS4 (M=Si.x=0.1.0.2.0.3;M=Ge.x=0.2.).Among them.the highest ambient ionic conductivity (1.75×10-4 S cm-1) is achieved when M=Si and x=0.2.The new fast ionic conductor Na3.8[Sn0.67Si0.33]0.8Sb0.2S4 is isostructural to its structure template Na4Sn0.67Si0.33S4 and thus crystallizes in the space group of I41/acd.It is shown that the incorporation of Sb improves the ionic conductivity.The study of lattice parameters shows that the improvement of the ion conductivity by Sbsubstitution is mainly due to the enlarged crystal lattice.Furthermore.using Na3.8[Sn0.67Si0.33]0.8Sb0.2S4 as solid electrolytes.room temperature all-solid-state sodium battery of Se0.05S0.95@pPAN/Na3Sn is realized.which proves the novel fast ionic conductor a potential candidate to apply in sodium solid state battery.This work not only extends the scope of Na4[Sn0.67Si0.33]S4.the I41/acd space group template.but also deepens the understanding of the lattice size effect on the structure and property relationship by aliovalent substitution.

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Practical fuel cells enabled by unprecedented oxygen reduction reaction on 3D nanostructured electrocatalysts Hong Yuan, Qiang Zhang 2020, 48(9): 107-108.  DOI: 10.1016/j.jechem.2020.01.004 摘要 ( 14 )

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Interface enhanced well-dispersed Co9S8 nanocrystals as an efficient polysulfide host in lithium-sulfur batteries Xue Liu, Qiu He, Hong Yuan, chong Yan, Yan Zhao, Xu Xu, Jia-Qi Huang, Yu-Lun Chueh, Qiang Zhang, Liqiang Mai 2020, 48(9): 109-115.  DOI: 10.1016/j.jechem.2020.01.003 摘要 ( 11 )   The high specific capacity and energy density of lithium-sulfur batteries have attracted strong considerations on their fundamental mechanism and energy applications.However.polysulfide shuttle is still the key issue that impedes the development of Li-S batteries.Exploring nanocrystal hosts for polysulfide immobilization and conversion is a promising way.In this contribution.we have investigated well-dispersed Co9S8 nanocrystals grown on graphene oxide (GO) nanosheets with different degrees of dispersion as cathode host materials for Li-S batteries.The Co9S8-GO composite with 1 wt% GO (GCS1) has an average crystal size of 76 nm and shows the strongest adsorption capability toward lithium polysulfides.When used as the host material for the cathode of Li-S batteries.the GCS1-sulfur composite exhibits an initial specific capacity of ~1000 mAh g-1 at 0.5 C and shows an average decay rate of 0.11% for 500 cycles.This work on the dispersion control of Co9S8 nanocrystals may inspire more investigations on well-dispersed nanocrystal based hosts for Li-S batteries.

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Anion-cation dual doping: An effective electronic modulation strategy of Ni2P for high-performance oxygen evolution Bo Xu, Xiaodong Yang, Qiang Fang, Linbing Du, Yan Fu, Yiqiang Sun, Qisheng Liu, Qingquan Lin, cuncheng Li 2020, 48(9): 116-121.  DOI: 10.1016/j.jechem.2019.12.027 摘要 ( 6 )   Developing of high-performance and low-cost electrocatalysts is of great significance to reduce the overpotential and accelerated the reaction rate of oxygen evolution in water splitting and related energy conversion applications.Herein.Fe.O-dual doped Ni2P (Fe.O-Ni2P) nanoarray is successfully synthesized on carbon cloth demonstrating enhanced electrocatalytic activity and stability for oxygen evolution reaction (OER) under alkaline media.The as-synthesized Fe.O-Ni2P nanoarray exhibits obviously improved OER performance with a low overpotential of 210 mV at 10 mA cm-2 current density and a Tafel slope of 48 mV dec-1.as well as long-term durability.The strong coupling interaction induced changes in electronic structure lead to relatively higher oxidation state and stronger oxidation ability of the Fe.O-Ni2P nanoarray.together with the high electrochemical surface area and good conductivity contribute to the superior OER performance.This work highlights the anion-cation dual doping strategy may be an effective method for fabrication of catalysts relating to energy conversion applications.

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Large-scale production of holey graphite as high-rate anode for lithium ion batteries Feng Xiao, Xianghong Chen, Jiakui Zhang, chunmao Huang, Tong Hu, bo Hong, Jiantie Xu 2020, 48(9): 122-127.  DOI: 10.1016/j.jechem.2019.12.026 摘要 ( 60 )

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Polar, catalytic, and conductive CoSe2/C frameworks for performance enhanced S cathode in Li-S batteries Bo Yuan, di Hua, Xingxing Gu, Yu Shen, Li-Chun Xu, Xiuyan Li, bing Zheng, Jiansheng Wu, Weina Zhang, Sheng Li, fengwei Huo 2020, 48(9): 128-135.  DOI: 10.1016/j.jechem.2019.12.020 摘要 ( 4 )   Lithium-sulfur battery (Li-S) is considered as one of the new-generation rechargeable batteries with high performance because of its extremely high theoretical capacity.energy density.environmental harmony and low cost.However.low electrical and ionic conductivity of sulfur.safety concerns and parasitic reaction generated by the dissolved polysulfide species in electrolyte hinder the commercialization of Li-S battery.Herein.we report a polyhedral porous structure comprising of carbon coating metal selenide nanoparticles (CoSe2/C).which could not only host sulfur for Li-S battery owing to its porous and conductive structure.but also mitigate the shuttle phenomenon by polysulfides adsorption and catalytic acceleration of redox kinetics.As a result.a performance enhanced CoSe2/C-S electrode for Li-S battery is achieved.

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Zeolite-assisted etherification of glycerol with butanol for biodiesel oxygenated additives production C.Cannilla, G.Bonura, S.Maisano, L.Frusteri, M.Migliori, G.Giordano, S.Todaro, f.Frusteri 2020, 48(9): 136-144.  DOI: 10.1016/j.jechem.2020.01.002 摘要 ( 13 )   This research was focused on the valorisation of glycerol.exploring the feasibility of an efficient route for oxygenated additives production based on its etherification with bio-butanol.A home-made BEA zeolite sample with a tuneable acidity has been proposed as the catalytic system.being tested in a stirred reactor under different etherification conditions.Although a reaction temperature as high as 200℃ resulted to be beneficial in terms of glycerol conversion (~90%).only by operating at milder conditions the product selectivity to glycerol-ethers can be better controlled.in order to obtain a bio-fuel complying with the requirements for mixing with fossil diesel or biodiesel.without any need of purification from large amount of by-products.A comprehensive identification of all the compounds formed during the reaction was performed by a GC-MS analysis.on the basis of the complex network of consecutive and parallel reaction paths leading not only to the desired ethers.but also to many side products not detected in similar acid-catalyzed reactions in liquid phase and not available in the most used mass-spectra libraries.

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Lithium metal anodes: Present and future Renheng Wang, Weisheng Cui, fulu Chu, feixiang Wu 2020, 48(9): 145-159.  DOI: 10.1016/j.jechem.2019.12.024 摘要 ( 141 )   Commercial lithium-ion (Li-ion) batteries based on graphite anodes are meeting their bottlenecks that are limited energy densities.In order to satisfy the large market demands of smaller and lighter rechargeable batteries.high-capacity metallic Li replacing low-specific-capacity graphite enables the higher energy density in next-generation rechargeable Li metal batteries (LMBs).However.Li metal anode has been suffering from dendritic problems.interfacial side reactions.volume change and low Coulombic efficiency.Therefore.performance enhancements of Li metal anodes are rather important to realize the high energy density characteristic of metallic Li.In this review.the annoying Li dendrite growth.unstable reaction interface and practical application issues of Li metal anodes are summarized and detailedly discussed to understand the current challenges concerning Li metal anodes.For overcoming such remaining challenges.the corresponding strategies and recent advances are covered and categorized.Finally.we discuss future opportunities and perspectives for developing high-performance Li metal anodes.

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Fabrication of multi-shell coated silicon nanoparticles via in-situ electroless deposition as high performance anodes for lithium ion batteries Wen-Feng Ren, Jun-Tao Li, Shao-Jian Zhang, Ai-Ling Lin, You-Hu Chen, Zhen-Guang Gao, Yao Zhou, Li Deng, Ling Huang, Shi-Gang Sun 2020, 48(9): 160-168.  DOI: 10.1016/j.jechem.2020.01.001 摘要 ( 13 )   Si-based materials have been extensively studied because of their high theoretical capacity.low working potential.and abundant reserves.but serious initial irreversible capacity loss and poor cyclic performance resulting from large volume change of Si during lithiation and delithiation processes restrict their widespread application.Herein.we report the preparation of multi-shell coated Si (DS-Si) nanocomposites by in-situ electroless deposition method using Si granules as the active materials and copper sulfate as Cu sources.The ratio of Si and Cu was readily tuned by varying the concentration of copper sulfate.The multi-shell (Cu@CuxSi/SiO2) coating on Si surface promotes the formation of robust and dense SEI films and the transportation of electron.Thus.the obtained DS-Si composites exhibit an initial coulombic efficiency of 86.2%.a capacity of 1636 mAh g-1 after 100 discharge-charge cycles at 840 mA g-1.and an average charge capacity of 1493 mAh g-1 at 4200 mA g-1.This study provides a low-cost and large-scale approach to the preparation of nanostructured Si-metal composites anodes with good electrochemical performance for lithium ion batteries.

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Electro-derived Cu-Cu2O nanocluster from LDH for stable and selective C2 hydrocarbons production from CO2 electrochemical reduction Naveed Altaf, Shuyu Liang, Liang Huang, Qiang Wang 2020, 48(9): 169-180.  DOI: 10.1016/j.jechem.2019.12.013 摘要 ( 7 )   Recently.CO2 conversion by electrochemical tool into value-added chemicals has been considered as one of the most promising strategies to offer sustainable development in energy and environment.In this contribution.we investigated electro-derived composites from Cu-based layered double hydroxide (LDH) for CO2 electrochemical reduction.The Cu-Cu2O based nanocomposite (HPR-LDH) were derived by using electro-strategy from LDH having the stability up to 20 h and selectivity toward C2H4 with faraday efficiency up to 36% by significantly suppressing CH4 and H2 with respect to bulk Cu foil.A highly negative reduction potential derived catalyst (HPR-LDH) maintained long-term stability for the selective production of ethylene over methane.and a small amount of Cu2O was still observed on the catalyst surface after CO2 reduction reaction (CO2RR).Moreover.such unique strategy for electro-derived composite from LDH having small nanoparticles stacked each other grown on layered structure.would provide new insight to improve durability of O-Cu combination catalysts for C-C coupling products during electrochemical CO2 conversion by suppressing HER.The XRD.SEM.ESR.and XPS analyses confirmed that the long-term ethylene selectivity of HPR-LDH is due to the presence of subsurface oxygen.The designed composite catalyst significantly enhances the stability and selectivity.and also decreases the over potential for CO2 electroreduction.We predict that the new designed LDH 2D-derived composites may attract new insight for transition metal and may open up a new direction for known structural properties of selective catalyst synthesis regarding effective CO2 reduction reaction.

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High crystallinity and photovoltaic performance of CsPbI3 film enabled by secondary dimension Min Wu, Keyou Yan, Yong Wang, Xiongwu Kang 2020, 48(9): 181-186.  DOI: 10.1016/j.jechem.2020.01.009 摘要 ( 17 )   The photovoltaic performance of perovskite sloar cells (PSCs) is strongly dependent on the crystallinity.morphorlogy and defects of perovskite films.In the present work.a novel strategy was developed to fabricate the high quality CsPbI3 inorganic perovskite by tuning the growth dynamics of CsPbI3 by pretreatment of fresh CsPbI3 films with phenylethylamine iodide (PEAI).The PEAI can mediate the phase transformation from 1D (DMAPbI3) (DMA:dimethylammonium) to 3D CsPbI3 all-inorganic perovskite films via the PEA2CsPb2I7 of 2D perovskite intermediate phase.resulting in highly crystalline CsPbI3 perovskite films with remarkably enlarged grains and reduced defects.The as-achieved highly crystalline CsPbI3 inorganic perovskite not only exhibited improved phase stability but also significant reduced defects.The perovskite solar cells based on these CsPbI3 thin films exhibited a champion efficiency of 17.08%.much higher than those prepared through posttreatment or direct addition of PEAI into CsPbI3 precursor solution.This work not only developed an effective strategy to prepare high crystalline CsPbI3 film and highly efficient CsPbI3-based all-inorganic PSCs.but also unraveled the mediation mechanism of CsPbI3 by pre-treatment of PEAI.shedding light for further development of high perfomance perovskite-based optoelectronics.

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Nitrogen-rich hierarchically porous carbon foams as high-performance electrodes for lithium-based dual-ion capacitor Yue Chen, Xiaoming Qiu, Li-Zhen Fan 2020, 48(9): 187-194.  DOI: 10.1016/j.jechem.2020.01.024 摘要 ( 4 )   Nitrogen-rich porous carbonaceous materials have shown great potential in energy storage and conversion applications due to their facile fabrication.high electronic conductivity.and improved hydrophilic property.Herein.three-dimensional porous N-rich carbon foams are fabricated through a one-step carbonization-activation method of the commercial melamine foam.and displaying hierarchically porous structure (macro-.meso-.and micro-pores).large surface area (1686.5 m2 g-1).high N-containing level (3.3 at%).and excellent compressibility.The as-prepared carbon foams as electrodes for quasi-solid-state supercapacitors exhibit enhanced energy storage ability with 210 F g-1 and 2.48c at 0.1 A g-1.and 150 F g-1 and 1.77 F cm-2 at 1 A g-1.respectively.Moreover.as an electrode for lithium-based dual-ion capacitor.this distinctive porous carbon also delivers remarkable specific capacitance with 143.6 F g-1 at 0.1 A g-1 and 116.2 F g-1 at 1 A g-1.The simple preparation method and the fascinating electrochemical performance endow the N-rich porous carbon foams great prospects as high-performance electrodes for electrochemical energy storage.

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In/ex-situ Raman spectra combined with EIS for observing interface reactions between Ni-rich layered oxide cathode and sulfide electrolyte Xuelei Li, Huilan Guan, Zhijie Ma, Ming Liang, dawei Song, Hongzhou Zhang, Xixi Shi, chunliang Li, Lifang Jiao, Lianqi Zhang 2020, 48(9): 195-202.  DOI: 10.1016/j.jechem.2020.01.021 摘要 ( 26 )   The interfacial instability between Ni-rich layered oxide cathodes and sulfide electrolytes is a serious problem.leading to poor electrochemical properties of all-solid-state lithium batteries (ASSLB).The chemical/electrochemical side reactions are considered to be the origin of the interfacial deterioration.However.the influence of chemical and electrochemical side reactions on the interfacial deterioration is rarely studied specifically.In this work.the deterioration mechanism of the interface between LiNi0.85-xCo0.15AlxO2 and Li10GeP2S12 is investigated in detail by combining in/ex-situ Raman spectra and Electrochemical Impedance Spectroscopy (EIS).It can be determined that chemical side reaction between LiNi0.8Co0.15Al0.05O2 and Li10GeP2S12 will occur immediately once contacted.and the interfacial deterioration becomes more serious after charge-discharge process under the dual effects of chemical and electrochemical side reactions.Moreover.our research reveals that the interfacial stability and the cycle performance of ASSLB can be greatly enhanced by increasing Al-substitution for Ni in LiNi0.85-xCo0.15AlxO2.In particular.the capacity retention of LiNi0.6Co0.15Al0.25O2 cathode after 200 cycles can reach 81.9%.much higher than that of LiNi0.8Co0.15Al0.05O2 cathode (12.5%@200 cycles).This work gives an insight to study the interfacial issues between Ni-rich layered oxide cathode and sulfide electrolyte for ASSLBs.

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A bifunctional ethylene-vinyl acetate copolymer protective layer for dendrites-free lithium metal anodes Yeru Liang, Ye Xiao, chong Yan, Rui Xu, Jun-Fan Ding, Ji Liang, Hong-Jie Peng, Hong Yuan, Jia-Qi Huang 2020, 48(9): 203-207.  DOI: 10.1016/j.jechem.2020.01.027 摘要 ( 29 )   Lithium metal batteries are strongly considered as one of the most promising candidates for nextgeneration high-performance battery systems.However.the uncontrollable growth of lithium dendrites and the highly reactive lithium metal result in the severe safety risks and the short lifespan for highenergy-density rechargeable batteries.Here.we demonstrate a hydrophobic and ionically conductive ethylene-vinyl acetate (EVA) copolymer layer can not only endow lithium metal anodes with an air-stable and anti-water surface.but also efficiently suppress the lithium-dendrites growth during the electrochemical cycling process.Therefore.the introduction of the EVA copolymer as a bifunctional protection layer simultaneously improves the anti-water/air performance and electrochemical cycling stability of lithium metal anode.

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The electrocatalytic activity of BaTiO3 nanoparticles towards polysulfides enables high-performance lithium-sulfur batteries Hongcheng Gao, Shunlian Ning, Jiasui Zou, Shuang Men, Yuan Zhou, Xiujun Wang, Xiongwu Kang 2020, 48(9): 208-216.  DOI: 10.1016/j.jechem.2020.01.028 摘要 ( 9 )   The slow redox dynamics and dissolution of polysulfides in lithium-sulfur (Li-S) batteries result in poor rate performance and rapid decay of battery capacity.thus limiting their practical application.Ferroelectric barium titanate (BT) nanoparticles have been reported to effectively improve the electrochemical performance of Li-S batteries due to the inherent self-polarization and high adsorption capacity of the BT nanoparticles towards polysulfides.Here in this paper.BT nanoparticles.behave as highly efficient electrocatalyst and demonstrate much higher redox dynamics towards the conversion reaction of polysulfides and Li2S than TiO2.as shown by both electrochemical measurements and density functional theory calculation.The coupling of the sulfur host of the hollow and graphitic carbon flakes (HGCF) and the BT nanoparticles (HGCF/S-BT) enable excellent electrochemical performance of Li-S batteries.delivering a 0.047% capacity decay per cycle in 1000 cycles at 1 C.788 mAh g-1 at 2 C and a reversible capacity of 613 mAh g-1 after 300 cycles at a current density of 0.5 C at a S loading of 3.4 mg cm-2.HGCF/S-BT also shows great promise for practical application in flexible devices as demonstrated on the soft-packaged Li-S batteries.

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Crystallization tailoring of cesium/formamidinium double-cation perovskite for efficient and highly stable solar cells Jianchao Yang, Yu Chen, Weijian Tang, Shubo Wang, Qingshan Ma, Yihui Wu, Ningyi Yuan, Jianning Ding, Wen-Hua Zhang 2020, 48(9): 217-225.  DOI: 10.1016/j.jechem.2020.01.012 摘要 ( 24 )   Achieving high-quality perovskite crystal films is a critical prerequisite in boosting solar cell efficiency and improving the device stability.but the delicate control of nucleation and growth of the perovskite film remains limited success.Herein.a facile but effective strategy has been developed to finely tailor the crystallization of thermally stable cesium/formamidinium (Cs/FA) based perovskite via partially replacing PbI2 with PbCl2 in the precursor solution.The incorporation of chlorine into the perovskite crystal lattice derived from PbCl2 changes the crystallization process and improves the crystal quality.which further results in the formation of larger crystal grains compared to the control sample.The larger crystal grains with high crystallinity lead to reduced grain boundaries.suppressed non-radiative recombination.and enhanced photoluminescence lifetime.Under the optimized conditions.the methylammonium free perovskite solar cells (PSCs) delivers a champion power conversion efficiency (PCE) of 21.30% with an open-circuit voltage as high as 1.18 V.which is one of the highest efficiencies for Cs/FA based PSCs up to now.Importantly.the unencapsulated PSC devices retain more than 95% and 81% of their original PCEs even after long-term (over one year) storage under ambient conditions or 2000 h's thermal aging at 85℃ in a nitrogen atmosphere.respectively.

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Ni0.85Se hexagonal nanosheets as an advanced conversion cathode for Mg secondary batteries Dong Chen, Jingwei Shen, Xue Li, Shun-an Cao, Ting Li, Wei Luo, fei Xu 2020, 48(9): 226-232.  DOI: 10.1016/j.jechem.2020.01.018 摘要 ( 8 )   Mg secondary batteries are promising scalable secondary batteries for next-generation energy storage.However.Mg-storage cathode materials are greatly demanded to construct high-performance Mg batteries.Electrochemical conversion reaction provides plenty of cathode options.and strategy for cathode selection and performance optimization is of special significance.In this work.Ni0.85Se with nanostructures of dispersive hexagonal nanosheets (D-Ni0.85Se) and flower-like assembled nanosheets (F-Ni0.85Se) is synthesized and investigated as Mg-storage cathodes.Compared with F-Ni0.85Se.D-Ni0.85Se delivers a higher specific capacity of 168 mAh g-1 at 50 mA g-1 as well as better rate performance.owing to its faster Mg2+ diffusion and lower resistance.D-Ni0.85Se also exhibits a superior cycling stability over 500 cycles.An investigation on mechanism indicates an evolution of Ni0.85Se towards NiSe with cycling.and the Mg-storage reaction occurs between NiSe and metallic Ni0.The present work demonstrates that advanced conversion-type Mg battery cathode materials could be constructed by soft selenide anions.and the electrochemical properties could be manipulated by rational material morphology optimization.

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Few-layer Ti3C2Tx MXene delaminated via flash freezing for high-rate electrochemical capacitive energy storage Xianli Wang, Liubing Dong, Wenbao Liu, Yongfeng Huang, Xuechao Pu, Jinjie Wang, feiyu Kang, Jia Li, chengjun Xu 2020, 48(9): 233-240.  DOI: 10.1016/j.jechem.2020.01.006 摘要 ( 15 )   Few-layer Ti3C2Tx MXene is synthesized from multi-layered Ti3C2Tx via a flash freezing-assisted delamination process.During the flash freezing process.the water molecules in the interlayers of multi-layered MXene are induced to rearrange and produce volume expansion.thus notably expand the MXenes' interlayer distance to form few-layer MXene.The synthesized few-layer Ti3C2Tx MXene nanosheets display a very small thickness (less than 5 Ti3C2 atom-layers) and expanded interlayer spacing.Consequently.the few-layer Ti3C2Tx exhibits enhanced capacitance (255 F g-1 vs.177 F g-1 for the multi-layered Ti3C2Tx) and significantly optimized rate capability (150 F g-1 at 200 mV s-1 vs.25 F g-1 for the multi-layered Ti3C2Tx).because redox-active sites in the few-layer MXene are easily accessible to electrolyte ions.Moreover.an asymmetric supercapacitor is constructed using the few-layer Ti3C2Tx negative electrode and an activated carbon fiber positive electrode.The asymmetric supercapacitor presents a high energy density of 17.9 Wh kg-1 and a high power density of 14 kW kg-1.which is inseparable from its wide voltage window of 1.4 V and the good rate performance of the few-layer Ti3C2Tx MXene electrode.Overall.the flash freezing-assist delamination provides an effective and environmental-friendly strategy to synthesize few-layer MXene materials for high-rate electrochemical energy storage.

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A new phosphidation route for the synthesis of NiPx and their cocatalytic performances for photocatalytic hydrogen evolution over g-C3N4 Ziqun Wang, Longfeng Li, Mingzhu Liu, Tifang Miao, Xiangju Ye, Sugang Meng, Shifu Chen, Xianliang Fu 2020, 48(9): 241-249.  DOI: 10.1016/j.jechem.2020.01.017 摘要 ( 17 )   Ni-based phosphides (NiPx) composed of earth-abundant elements are promising cocatalysts to replace noble metals for photocatalytic H2 evolution reaction (HER).A safe.energy-saving.and compositioncontrollable synthesis of NiPx is still highly desired.A facile and mild solvothermal process was developed for the first time for selective synthesis of a series of NiPx.including Ni.Ni12P5.Ni2P/Ni12P5.Ni/Ni2P and Ni2P.through controlling the dosage of NaBH4 and NaH2PO2.The phosphidation process was mainly composed of (1) a sequential reduction of Ni2+ to Ni0 and (H2PO2)-to P (around the formed Ni0) triggered by NaBH4.and (2) a final phosphidation between Ni0 and the in situ generated P atoms.The photocatalytic HER performance of g-C3N4 can be substantially improved with the decoration of NiPx (3 wt%) as the separation of photoinduced charge carriers can be promoted and some active sites with low over-potential for HER can be introduced.The cocatalytic efficiency of NiPx is mainly determined by P content.Ni2P with a high ratio of P consequently exhibits the highest HER performance (215.1 μmol g-1 h-1).which is almost six times higher than that of the pristine g-C3N4 (35.6 μmol g-1 h-1).Thus.as for the cocatalyst based on Ni phosphides.Ni2P is the preferable crystal phase and more efforts should be devoted to Ni2P to further optimize its structure.texture.and morphology in future works.

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High performance room temperature all-solid-state Na-SexS battery with Na3SbS4-coated cathode via aqueous solution Ziqi Zhang, Haonan Cao, Meng Yang, Xinlin Yan, chuang Yu, di Liu, Long Zhang 2020, 48(9): 250-258.  DOI: 10.1016/j.jechem.2020.01.014 摘要 ( 16 )   All-solid-state (ASS) Na-S batteries are promising for large-scale energy storage because of the incombustible solid electrolyte and avoiding the dissolution of intermediates.However.the poor contact between the active material and the solid electrolyte in the positive electrode leads to poor electrochemical performance.Here.we report an aqueous solution approach to fabricate Na3SbS4-coated SexS-based active materials for a Na-S battery working at room temperature.Compared with the Na3SbS4 and SexS mixed cathode.the coated cathode achieves significantly improved Na-ion diffusion kinetics and reduced impedance resistance.Additionally.the nanoparticle coating sustains the volume expansion of the cathode during cycling.The resulting batteries deliver an intensively enhanced specific capacity at various rates.Regardless of the mass loading.the Na3SbS4-coated cathode maintains a decent reversible capacity for the long-term discharge/charge cycling.The best battery achieves an initial discharge capacity of 509 mAh g-1 at a current density of 437.4 mA g-1 and capacity retention of 98.9% for 100 cycles.To the best of our knowledge.this is one of the best room temperature ASS Na-S battery so far.This work demonstrates that Na3SbS4 is very promising for the cathode coating purpose for ASS Na-S batteries.

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Bronze TiO2 as a cathode host for lithium-sulfur batteries Wenjing Dong, di Wang, Xiaoyun Li, Yuan Yao, Xu Zhao, Zhao Wang, Hong-En Wang, Yu Li, Lihua Chen, dong Qian, bao-Lian Su 2020, 48(9): 259-266.  DOI: 10.1016/j.jechem.2020.01.022 摘要 ( 37 )   Lithium-sulfur batteries (LSBs) are very promising for large-scale electrochemical energy storage.However.dissolution and shuttling of lithium polysulfides (LiPSs) intermediates have severely affected their overall electrochemical properties and limited their practical application.Designing polar cathode hosts that can effectively bind LiPSs and simultaneously promote their redox conversion is crucial for realizing high-performance LSBs.Herein.we report bronze TiO2 (TiO2-B) nanosheets (~5 nm in thickness) chemically bonded with carbon as a novel multifunctional cathode host for advanced LSBs.Experimental observation and first-principles density functional theory (DFT) calculations reveal that the TiO2-B with exposed (100) plane and Ti3+ ions exhibited high chemical affinity toward polysulfides and effectively confined them at surface.Meantime.Ti3+ ions and interface coupling with carbon promoted electronic conductivity of the composite cathode.leading to enhanced redox conversion kinetics of LiPSs during charge/discharge.Consequently.the as-assembled TiO2-B/S cathode manifested high capacity (1165 mAh/g at 0.2 C).excellent rate capability (244 mAh/g at 5 C) and outstanding cyclability (572 mAh/g over 500 cycles at 0.2 C).This work sheds insights on rational design and fabrication of novel functional electrode materials for beyond Li-ion batteries.

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A novel permselective organo-polysulfides/PVDF gel polymer electrolyte enables stable lithium anode for lithium-sulfur batteries Yan-Qiu Shen, fang-Lei Zeng, Xin-Yu Zhou, An-bang Wang, Wei-kun Wang, Ning-Yi Yuan, Jian-Ning Ding 2020, 48(9): 267-276.  DOI: 10.1016/j.jechem.2020.01.016 摘要 ( 23 )   Lithium-sulfur (Li-S) battery can satisfy the need of the future power battery market because of its high energy density.but the hidden dangers caused by lithium anode have seriously hindered their commercialization.Herein.an innovative gel polymer electrolyte (GPE) composed of polyvinylidene fluoride (PVDF) and organo-polysulfide polymer (PSPEG) is proposed.which could be used in semisolid-state Li-S batteries for protection of Li anodes.Particularly.organo-polysulfide polymer could chemically/electrochemically generate both inorganic and organic components simultaneously in-situ once contacting fresh Li metal surface and/or during discharging processes.And these inorganic/organic components could participate in the formation of the SEI layer and finally constitute a stable and flexible hybrid SEI layer on the surface of Li metal anode.Moreover.the organic components were permselective to lithium ions against anions.Therefore.PVDF/PSPEG GPE ensures the ideal chemical and electrochemical properties for Li-S batteries.Our work demonstrates an effective solution to solve the problems about Li anodes and contributes to the development of the safe Li metal batteries.

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Full-faradaic-active nitrogen species doping enables high-energy-density carbon-based supercapacitor Wei Wei, Zhangjing Chen, Yan Zhang, Jian Chen, Liu Wan, cheng Du, Mingjiang Xie, Xuefeng Guo 2020, 48(9): 277-284.  DOI: 10.1016/j.jechem.2020.02.011 摘要 ( 11 )   Nitrogen doping is usually adopted in carbon based supercapacitor to enhance its relatively low energy density by providing extra pseudocapacity.However.the improvement of energy density is normally limited because the content of the introduced nitrogen species is not high and meanwhile only part of them is electrochemically active.Herein.we designed and fabricated a class of hierarchical nitrogen-rich porous carbons (HNPCs) possessing not only very high nitrogen content (up to 21.7 atom%) but also fully electrochemically active nitrogen species (i.e..pyridinic N.pyrrolic N and oxidized N).Especially.in the synthesis of HNPCs.graphitic carbon nitride (g-C3N4) was used in situ not only as a nitrogen source but also as a catalyst to facilitate the polymerization of phenol and formaldehyde (as carbon precursor) and as a template to create the hierarchical porous structure.As electrodes for aqueous symmetric supercapacitor.the HNPCs with full faradaic-active nitrogen functionalities exhibit excellent supercapacitor performance:high energy density of 36.8 Wh/kg at 2.0 kW/kg (maintaining 25.7 Wh/kg at 38 kW/kg).superior rate capability with 78% capacitance retention from 1.0 to 20 A/g and excellent cycling stability with over 95% capacitance retention after 10 000 cycles.indicating their promising application potential in electrochemical energy storage.This novel carbon material with high-content and full electrochemically active nitrogen species may find extensive potential applications in the energy storage/conversion.catalysis.adsorption.and so on.

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Implanting a preferential solid electrolyte interphase layer over anode electrode of lithium ion batteries for highly enhanced Li+ diffusion properties Ye Kyu Kim, Yoongon Kim, Jaejin Bae, Hyunwoo Ahn, Yuseong Noh, Hyunsu Han, Won Bae Kim 2020, 48(9): 285-292.  DOI: 10.1016/j.jechem.2020.02.026 摘要 ( 13 )   The lithium-ion batteries are recognized as the most promising energy storage system.but it still does not meet the power requirements of electric vehicle batteries owing to low volumetric energy density with the traditional graphite electrode system.In this study.we report the development of a novel electrode system fabricated by implantation of a solid electrolyte interphase (SEI) layer on the graphite surface.The SEI-implanted graphite electrode is made using a lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)-based electrolyte and cycled with a lithium tetrafluoroborate LiBF4-based electrolyte.This new electrode system shows significantly enhanced electrochemical properties owing to the rapid and efficient diffusion of Li ions through the SEI layer between the electrolyte and electrode.This graphite electrode with its pre-formed SEI layer achieves a reversible capacity of 357 mAh g-1 at 0.5 C after 50 cycles.which is significantly higher than that of commercial lithium-ion battery systems constructed with LiPF6 (312 mAh g-1).The resulting unique electrode system could present a new avenue in SEI research for highperformance lithium-ion batteries.

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Anthradithiophene based hole-transport material for efficient and stable perovskite solar cells Guohua Wu, Yaohong Zhang, Ryuji Kaneko, Yoshiyuki Kojima, Ashraful Islam, Kosuke Sugawa, Joe Otsuki, Shengzhong Liu 2020, 48(9): 293-298.  DOI: 10.1016/j.jechem.2020.02.021 摘要 ( 39 )   A novel hole-transport material (HTM) based on an anthradithiophene central bridge named BTPA-7 is developed.In comparison to spiro-OMeTAD (2,2',7,7'-tetrakis-(N,N-di-p-methoxyphenylamine)-9,9'-spirobifluorene).the synthetic steps of BTPA-7 are greatly reduced from 6 to 3 and the synthetic cost of BTPA-7 is nearly a half that of spiro-OMeTAD.Moreover.BTPA-7 exhibits a relatively lower conductivity but higher hole mobility and higher glass transition temperature (Tg) than spiro-OMeTAD.Compared with the photovolatic performance for spiro-OMeTAD.FA0.85MA0.15PbI3 and MAPbI3 PSC devices based on BTPA-7 exhibit slightly lower PCEs with the values of 17.58% (18.88% for spiro-OMeTAD) and 11.90% (13.25% for spiro-OMeTAD).respectively.Nevertheless.a dramatically higher Jsc of PSC based on BTPA-7 is achieved.which arises from the higher hole mobility of BTPA-7.In addition.the relatively hydrophobic character of BTPA-7 eventually enhances the PSC device stability.Lower cost.higher hole mobility.higher Tg.satisfactory photovoltaic performance.and superior device stability of BTPA-7 can be utilized as a substitute for sp

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Insights into interfacial speciation and deposition morphology evolution at Mg-electrolyte interfaces under practical conditions Zihao Song, Zhonghua Zhang, Aobing Du, Shamu Dong, Guicun Li, Guanglei Cui 2020, 48(9): 299-307.  DOI: 10.1016/j.jechem.2020.02.019 摘要 ( 12 )   Rechargeable magnesium (Mg) battery technologies show the promise of low cost.less safety concerns and relatively higher energy density.Interrogating the critical issues on the Mg stripping/plating performance as well as the Mg metal anode-electrolyte interfacial chemistry is one great importance under the practical areal capacity and rate conditions.In this work.we systematically investigate the electrochemistry of Mg stripping/plating processes within four distinctive Mg-ion electrolytes and the Mg anodeelectrolyte interfacial chemistry under practical conditions.Electrochemical results show that the cycle life of Mg//Cu asymmetric cells using these above electrolytes is significantly shortened (less than 10 cycles) when tested at a practical areal capacity of 10 mAh cm-2.Further optical and electron microscopic analyses reveal that the gradual growth of the Mg deposits is susceptible to detachment from the copper substrate.where the initial nucleation process might occur.In spite of showing an interconnected particle-like morphology.the Mg deposits could easily penetrate the porous separator.leading to cell failure.The co-deposition of metallic Al is revealed from surface region to bulk.while the Cl-containing species exist in the near surface of Mg deposits.Our work not only highlights the critical impacts of areal capacity on the performances of Mg stripping/plating process.but calls for further efforts to eliminating the safety concerns of Mg anode under practical conditions.

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Metal-free carbocatalysis for electrochemical oxygen reduction reaction: Activity origin and mechanism Yuhang Li, Yexiang Tong, feng Peng 2020, 48(9): 308-321.  DOI: 10.1016/j.jechem.2020.02.027 摘要 ( 15 )   Although scientists have conducted long-term and extensive studies on oxygen reduction reaction (ORR) catalyzed by metal-free carbon materials.they mainly have focused on the preparation and properties of various doped carbon materials.There is still a lack of systematic scientific guidance on the relationship between the surface structure regulation and activity of carbon-based catalysts.In this review.some of electrochemical and computational fundamental concepts about ORR are concisely summarized.The effects of edge defect and nonmetallic doping of carbon materials on ORR behavior and mechanism have been reviewed.and activity origin identification and intermediate conversion mechanism have been discussed.The outlooks for future researches on metal-free ORR electrocatalysis are suggested.

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Co-doped graphene edge for enhanced N2-to-NH3 conversion Zengxi Wei, Yuezhan Feng, Jianmin Ma 2020, 48(9): 322-327.  DOI: 10.1016/j.jechem.2020.02.014 摘要 ( 5 )   N2 fixation in atmosphere is an important issue in modern chemistry.Designing an ideal electrochemical nitrogen reduction reaction (NRR) catalyst to overcome the sluggish reaction kinetic and ultralow selectivity is still the significant challenge.Herein.we screened the potential catalyst to accelerate N2 fixation by designing the single transition metal (TM) atoms (Ti.V.Cr.Mn.Fe.Co.Ni.Cu.Zn.Mo.W.Ru and Rh) supported on the edge of graphene.Our calculations revealed that the Co atom supported on the graphene edge could selectively stabilize *N2H species and destabilize *NH2 species.leading to the highest catalytic activity and selectivity for N2 fixation at the ambient conditions.In addition.the enzymatic mechanism of eNNR have the lowest overpotential of 0.72 V.This theoretical work will give a new perspective to design an available catalyst for NRR.

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Fe-doped CoP core-shell structure with open cages as efficient electrocatalyst for oxygen evolution Jing-Yi Xie, Zi-Zhang Liu, Jia Li, Lei Feng, Min Yang, Yu Ma, da-Peng Liu, Lei Wang, Yong-Ming Chai, bin Dong 2020, 48(9): 328-333.  DOI: 10.1016/j.jechem.2020.02.031 摘要 ( 16 )   Developing a facile approach based on transition metal-based Prussian blue (PB) and its analogues (PBAs) with core-shell nanostructure is a very promising choice for constructing cost-effective electrocatalysts for oxygen evolution reaction (OER).Herein.a bimetallic core-shell structure with open cages of Fe-doped CoP (Fe-CoP cage) has been synthesized using CoFe-PBA cage-4 as precursor through a facile hydrothermal method and following phosphating process.Interestingly.there is an open hole in each face center of Fe-CoP cage.which suggests the more exposure of active sites for OER.Electrochemical measurements show that Fe-CoP cage can afford a current density of 10 mA cm-2 at a low overpotential (300 mV).which is better than that of RuO2.The excellent performance can be attributed to Fe doping composition and unique open-cage core-shell structure.The synergistic effect derived from bimetallic active for OER has been discussed.And its great catalytic stability has been evaluated via 1000 cycles of CV and chronoamperometry measurement.This work provides a potential method to design multiple transitional metal-doping electrocatalysts with complex framework derived from PBAs for water splitting.

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Comprehensively-modified polymer electrolyte membranes with multifunctional PMIA for highly-stable all-solid-state lithium-ion batteries Lehao Liu, Jinshan Mo, Jingru Li, Jinxin Liu, Hejin Yan, Jing Lyu, bing Jiang, Lihua Chu, Meicheng Li 2020, 48(9): 334-343.  DOI: 10.1016/j.jechem.2020.02.033 摘要 ( 17 )   Polyethylene oxide (PEO)-based electrolytes have obvious merits such as strong ability to dissolve salts (e.g..LiTFSI) and high flexibility.but their applications in solid-state batteries is hindered by the low ion conductance and poor mechanical and thermal properties.Herein.poly(m-phenylene isophthalamide) (PMIA) is employed as a multifunctional additive to improve the overall properties of the PEO-based electrolytes.The hydrogen-bond interactions between PMIA and PEO/TFSI-can effectively prevent the PEO crystallization and meanwhile facilitate the LiTFSI dissociation.and thus greatly improve the ionic conductivity (two times that of the pristine electrolyte at room temperature).With the incorporation of the high-strength PMIA with tough amide-benzene backbones.the PMIA/PEO-LiTFSI composite polymer electrolyte (CPE) membranes also show much higher mechanical strength (2.96 MPa).thermostability (419℃) and interfacial stability against Li dendrites (468 h at 0.10 mA cm-2) than the pristine electrolyte (0.32 MPa.364℃ and short circuit after 246 h).Furthermore.the CPE-based LiFePO4/Li cells exhibit superior cycling stability (137 mAh g-1 with 93% retention after 100 cycles at 0.5 C) and rate performance (123 mAh g-1 at 1.0 C).This work provides a novel and effective CPE structure design strategy to achieve comprehensively-upgraded electrolytes for promising solid-state battery applications.

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There is plenty of space in the MXene layers: The confinement and fillings Ming Lu, Wenjuan Han, Haibo Li, Wei Zhang, bingsen Zhang 2020, 48(9): 344-363.  DOI: 10.1016/j.jechem.2020.02.032 摘要 ( 53 )   MXenes have emerged as a new kind of 2D transition metal carbides.nitrides and carbonitrides.Origined from the unique 2D structure with a luxuriant combination of elements.MXenes drive a series of the investigations related to energy storage and conversion.biometrics and sensing.lighting.purification and separation.For 2D layered MXene materials.the interspacing confined by the independent MXenes layers affords a distinct confinement space.which is similar to a nanoreactor that can be utilized for the storage of ions.nanoparticles.nanowires.and the materials with 2D or 3D structure.These fillings confined by MXene layers afford new opptunities for achieving improved properties and performance via complementary natural features.further the synergistic effect.Herein.we summarize the recent reports concerning with the confinded MXenes spacing and the fillings.The modification of interlayer distance lead by the intercalants were explored.We expect that our review may offer the route for a series of ongoing studies to address the MXenes.

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Attapulgite nanorods assisted surface engineering for separator to achieve high-performance lithium-sulfur batteries Wenhao Sun, Xiaogang Sun, Naseem Akhtar, chengming Li, Weikun Wang, Anbang Wang, Kai Wang, Yaqin Huang 2020, 48(9): 364-374.  DOI: 10.1016/j.jechem.2020.02.030 摘要 ( 4 )   Lithium-sulfur (Li-S) batteries have been recognized as one of the most promising candidates for nextgeneration portable electronic devices.owing to their extremely high energy density and low cost.However.the dissolution of lithium polysulfides (LiPSs) and consequent "shuttle effect" seriously hinder the practical deployment of Li-S batteries.Herein.multi-metal oxide nanorods named attapulgite are proposed as multifunctional ionic sieve to immobilize LiPSs and further promote the regulation of LiPSs.Attapulgite.consisting of Al.Mg.Fe.Si and O ions.possesses more polar sites to immobilize LiPSs in comparison with single metal oxides.In addition.the catalytic nature (Fe ions) of attapulgite avails the LiPSs conversion reaction.which is further confirmed by the linear sweep voltammetry and electrochemical impedance spectroscopy.Benefited from the synergistic effect of multi-metal oxide and conductive carbon.the Li-S battery with the modified separator delivers remarkable discharge capacities of 1059.4 mAh g-1 and 792.5 mAh g-1 for the first and 200th cycle at 0.5 C.respectively.The work presents an effective way to improve the electrochemical performance of Li-S batteries by employing attapulgite nanorods assisted separator surface engineering.

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Slurry-like hybrid electrolyte with high lithium-ion transference number for dendrite-free lithium metal anode Hewei Xu, Ying He, Zibo Zhang, Junli Shi, Pingying Liu, Ziqi Tian, Kan Luo, Xiaozhe Zhang, Suzhe Liang, Zhaoping Liu 2020, 48(9): 375-382.  DOI: 10.1016/j.jechem.2020.02.009 摘要 ( 12 )   Lithium metal anode is regarded as the ultimate choice for next-generation energy storage systems.due to the lowest negative electrochemical potential and super high theoretical specific capacity.However.the growth of lithium dendrite during the cycling process is still one of the most critical bottlenecks for its application.In this work.a slurry-like hybrid electrolyte is proposed towards the application for lithium metal anode.which is composed of a liquid electrolyte part and a nanometric silane-Al2O3 particle part.The hybrid electrolyte shows high ionic conductivity (3.89×10-3 S cm-1 at 25℃) and lithium-ion transference number (0.88).Especially.the resistance of hybrid electrolyte decreases compared to that of liquid electrolyte.while the viscosity of hybrid electrolyte increases.It is demonstrated that the hybrid electrolyte can effectively suppress the growth of lithium dendrite.Stable cycling of Li/Li cells at a current density up to 1 mA cm-2 is possible.The hybrid electrolyte helps to uniform the lithium ion flux inside the battery and partly comes from the formation of a rigid and highly conductive hybrid interfacial layer on the surface of lithium metal.This work not only provides a fresh way to stabilize lithium metal anode but also sheds light on further research for electrolyte optimization and design of lithium metal battery system.

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Skin care design for lithium metal protection with cosmetics introduction Yurong Tu, Qingtao Ma, Aoxuan Wang, Xinyue Zhang, Guojie Li, Jiayan Luo, Xingjiang Liu 2020, 48(9): 383-389.  DOI: 10.1016/j.jechem.2020.01.036 摘要 ( 9 )   Lithium metal anode (LMA) is the ultimate "Holy Grail" electrode for next generation high-energy-density batteries.Nevertheless.its instinct high reactivity is a formidable challenge and has intensified side reactions.destabilized the electrode/electrolyte interface and restricted the operating conditions strictly.thus hampering its practical application.Here.we "make up" the Li metal (M-Li) by constructing vaselinecoated layer by a simple dip-coating or casting method.With the chemically stable and hydrophobic vaseline protective layer.the stability of Li towards humid and corrosive atmosphere has been greatly improved.The M-Li guaranteed stable and prolonged cycling life after the anode suffering from corrosion in moist air (relative humidity ~65%) or corrosive electrolyte (with 10,000 ppm H2O or S) both in symmetric cells and LiFePO4 full cells.This work illustrates a convenient.economic.and industrial applicable method for stable LMA.

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Oxygen-deficient titanium dioxide supported cobalt nano-dots as efficient cathode material for lithium-sulfur batteries You Li, Xiao Zhang, Guihua Liu, Ashton Gerhardt, Katelyn Evans, Aizhong Jia, Zisheng Zhang 2020, 48(9): 390-397.  DOI: 10.1016/j.jechem.2020.02.028 摘要 ( 13 )   Lithium sulfur (Li-S) batteries demonstrate great promise for efficient energy storage systems once the lithium polysulfide (LPS) shuttling and sluggish redox kinetics can be well addressed.Herein.we developed a sea urchin-structured oxygen-deficient titanium dioxide semiconductor anchored with cobalt nano-dots (Co@TiO2-x) as a high-performance multifunctional sulfur host material for Li-S batteries.The sea urchin-structured Co@TiO2-x offers strong structural stability and strengthened chemical interaction towards LPS.Meanwhile.the incorporation of Co nano-dots into TiO2 leads to increased oxygen vacancies.which augments the electrical conduction and benefits LPS conversion acceleration as well.As a result.the oxygen vacancy-rich Co@TiO2-x composite exhibits excellent conductivity.strong LPS confinement and promoted sulfur electrochemical kinetics.rendering enhanced LPS shuttling inhibition and rapid redox reaction.Attributed to these features.the Co@TiO2-x/S cathode exhibits a discharge capacity of 803 mAh g-1 at 1 C and a good cyclic stability upon 500 cycles with a low capacity fading rate of 0.07% per cycle.This synergistic design of conductive multifunctional LPS barrier is also promising to enlighten the material engineering in other energy storage applications.

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Design and modulation principles of molybdenum carbide-based materials for green hydrogen evolution Jing-Qi Chi, Min Yang, Yong-Ming Chai, Zhi Yang, Lei Wang, bin Dong 2020, 48(9): 398-423.  DOI: 10.1016/j.jechem.2020.02.013 摘要 ( 14 )   The green production of hydrogen from electrocatalytic water splitting is an important base and promising direction for the future of the large-scale application of hydrogen energy.The key of green hydrogen evolution depends on the development of low-cost and highly active electrocatalysts.Molybdenum carbides (MoxC).as a typical of earth-abundant transition-metal material.have accumulated great attention due to their low cost.earth abundance.electrical conductivity.similar d-band state to Pt.and regulated morphology/electronic structures.In this paper.recent researches focusing on MoxC for efficient HER in a wide pH range are summarized from respects of modulation of unique morphology.electronic structure.and electrode interface step by step.Briefly.modulation of morphology influence the apparent activity of catalyst.modulation of electronic structure of active sites by heteroatom doping and designing heterointerface boost intrinsic HER kinetics.and modulation of electrode interface via hybridization of MoxC structures with carbon materials can ensure the fast electron transfer and boost the activity.Besides the above methods discussed.perspective and challenges of designing MoxC as the substitute of Pt-based electrocatalyst for practical hydrogen generation in a wide pH range are pointed out.

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The evolution and failure mechanism of lithium metal anode under practical working conditions Jia Liu, Hong Yuan 2020, 48(9): 424-425.  DOI: 10.1016/j.jechem.2020.02.047 摘要 ( 11 )

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Vacancy defect modulation in hot-casted NiOx film for efficient inverted planar perovskite solar cells Aili Wang, Zhiyuan Cao, Jianwei Wang, Shurong Wang, chengbo Li, Nuo Li, Lisha Xie, Yong Xiang, Tingshuai Li, Xiaobin Niu, Liming Ding, feng Hao 2020, 48(9): 426-434.  DOI: 10.1016/j.jechem.2020.02.034 摘要 ( 33 )   Nickel oxide (MoxC) has exhibited great potential as an inorganic hole transport layer (HTL) in perovskite solar cells (PSCs) due to its wide optical bandgap and superior stability.In this study.we have modulated the Ni2+ vacancies in MoxC film by controlling deposition temperature in a hot-casting process.resulting the change of coordination structure and charge state of MoxC.Moreover.the change of the HOMO level of MoxC makes it more compatible with perovskite to decrease energy losses and enhance hole carrier injection efficiency.Besides.the defect modulation in the electronic structure of MoxC is beneficial for increasing the electrical conductivity and mobility.which are considered to achieve the balance of charge carrier transport and avoid charge accumulation at the interface between perovskite and HTL effectively.Both experimental analyses and theoretical calculations reveal the increase of nickel vacancy defects change the electronic structure of MoxC by increasing the ratio of Ni3+/Ni2+ and improving the p-type characteristics.Accordingly.an optimal deposition temperature at 120℃ enabled a 36.24% improvement in the power conversion efficiency compared to that deposited at room temperature (25℃).Therefore.this work provides a facile method to manipulate the electronic structure of MoxC to improve the charge carrier transport and photovoltaic performance of related PSCs.

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Construction of robust coupling interface between MoS2 and nitrogen doped graphene for high performance sodium ion batteries Yun Qiao, Jiawei Wu, Xiaoguang Cheng, Yudong Pang, Zhansheng Lu, Xiangdong Lou, Qingling Li, Jin Zhao, Shuting Yang, Yang Liu 2020, 48(9): 435-442.  DOI: 10.1016/j.jechem.2020.02.012 摘要 ( 11 )   As a layered inorganic material.MoS2 has recently attracted intensive attention as anode for sodium ion batteries (SIBs).However.this anode is plagued with low electronic conductivity.serious volume expansion and sluggish kinetics.resulting in capacity fading and poor rate performance.Herein.we develop an interface engineering strategy to substantially enhance the sodium storage performance of MoS2 by incorporating layered MoS2 into three dimensional N-doped graphene scaffold.The strong coupling-interface between MoS2 and N-doped graphene scaffold can not only stabilize the MoS2 structure during sodium insertion/extraction processes.but also provide plenty of anchor sites for additional surface sodium storage.The 3D MoS2@N-doped graphene composite as anode for SIBs performs an outstanding specific capacity of 667.3 mA h g-1 at 0.2 A g-1.a prolonged stability with a capacity retention of 94.4% after 140 cycles and excellent rate capability of 445 mA h g-1 even at a high rate of 10 A g-1.We combined experiment and theoretical simulation to further disclose the interaction between MoS2 and N-doped graphene.adsorption and diffusion of sodium on the composite and the corresponding sodium storage mechanism.This study opens a new door to develop high performance SIBs by introducing the interface engineering technique.