能源化学(英文版)

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Preface to the Special Issue on Energy Electrochemistry

Zhongqun Tian, Jun Chen, Yongyao Xia

2018, 27(6): 1516-1516.

摘要 ( 911 )

Energy electrochemistry is one of the key branches of energy chemistry. Its main goal is to develop chemical energy storage devices with high performance, high safety, long life and low cost for wide applications. The key research areas include lithium ion batteries, fuel cells and redox flow batteries, and the key future directions include Li-S batteries, Li-air batteries, all solid-state batteries and batteries for wearable electronics. Recently there have been some significant advances spanning from fundamental discovery to application-specific prototypes in this field. For this reason, J. Energy Chem. organizes this special issue titled "Energy Electrochemistry" to show the recent development and challenges in this field.
This issue contains 16 contributions, with 1 communication, 8 reviews and 7 articles, covering different aspects in fuel cells, ion batteries, lithiumsulfur batteries and etc.
In the communication, Zhuang, Xiao and coworkers (https://doi.org/10.1016/j.jechem.2018.05.009) report a simple method to prepare wide channels bearing hydrocarbon proton exchange membranes with about the 200% improved conductivity for proton exchange membrane fuel cells (PEMFCs). Electrocatalysts are another key component to play vital role in the fuel cells. Liu, Xing and coworkers (https://doi.org/10.1016/j.jechem.2018.01.029) review the recent development of methanol electro-oxidation catalysts for direct methanol fuel cells (DMFCs), which is a promising power source for stationary and portable miniature electric appliances. Xie, Zhang and coworkers (https://doi.org/10.1016/j.jechem.2018.03.015) summarize the recent advances in electrocatalytic conversion of methane to ethylene and methanol. Xing and coworkers (https://doi.org/10.1016/j.jechem.2018.06.008) developed a series of Fe-N-C catalysts from various iron sources, for example ZIF-8, (Fe(acac)₃ and discussed the influence of the Fe morphology and site density on the ORR activity.
The lithium-ion batteries featuring relatively high energy density have long been used to power portable electronics and electrical vehicles. Aqueous lithium-ion battery (ALIB) is one of the most promising stationary power sources for sustainable energy such as wind and solar power. Xia and coworkers (https://doi.org/10.1016/j.jechem.2018.06.004) review the development of cathode, anode and electrolyte for acquiring the desired electrochemical performance of ALIBs. Moreover, electrode materials determine the battery performance. Zhao et al. (https://doi.org/10.1016/j.jechem.2018.01.009) review the recent development of using transition metal sulfides such as copper sulfides, molybdenum sulfides, cobalt sulfides, and iron sulfides as electrode materials for lithium ion batteries. Sun et al. (https://doi.org/10.1016/j.jechem.2018.04.009) report the excellent performance of lithium-ion battery with porous core-shell CoMn₂O₄ microspheres as anode and their conversion reaction mechanism. Chen et al. (https://doi.org/10.1016/j.jechem.2018.06.003) report core-shell structured 1,4-benzoquinone@titanium dioxide (BQ@TiO₂) composite as cathode for lithium batteries, which exhibit high discharge capacity and good cycling performance. Xia and coworkers (https://doi.org/10.1016/j.jechem.2018.01.026) determine the theoretical specific capacity of a new two-dimensional boron material as anode material for lithium-ion batteries using the first principles calculations.
In situ and operando techniques with high spatial and temporal resolution have been developing rapidly for the nondestructive and real time dynamic investigation on the electrochemical reaction mechanism. Yang et al. (https://doi.org/10.1016/j.jechem.2018.03.020) review the application of synchrotron X-ray techniques, including X-ray diffraction (XRD), Pair Distribution Function (PDF), Hard and Soft X-ray absorption spectroscopy (XAS) and X-ray photoelectron spectroscopy (XPS), to the investigation of battery systems. He, Zhou and coworkers (https://doi.org/10.1016/j.jechem.2018.06.007) investigated the lithium storage mechanism of layered LiNi_0.8Co_0.15Al_0.05O₂ during the electrochemical process through in situ X-ray diffraction.
Lithium-sulfur (LiS) battery is considered to be a promising next generation energy storage device with very high theoretical energy density and the natural abundance of sulfur. Guo et al. (https://doi.org/10.1016/j.jechem.2018.04.014) review the physical and chemical confinement of LiPSs and emphasize that synergy of the physical and chemical confinement is the feasible avenue to guide LiS batteries to the practical application. Chen, Wei and coworkers (https://doi.org/10.1016/j.jechem.2018.02.010) report a novel hierarchically porous nitrogen-doped carbon (HPNC) via a combination of salt template (ZnCl₂) and hard template (SiO₂) as sulfur host for Li-S batteries.
Comparing with lithium, sodium is of high overall abundance with even geographical distribution, and low cost. Thus, sodium-ion batteries (SIBs) have attracted increasing attention in the past decades. Zheng, Zhang and coworkers (https://doi.org/10.1016/j.jechem.2018.05.001) review the crystal structure of Na₃V₂(PO₄)₃ (NVP), a typical sodium super ion conductor (NASICON)-based electrode material, and recent approaches to enhance their surface electrical conductivity and intrinsic electrical conductivity. Besides, for the higher energy density Na-based batteries, Lu, Hu and coworkers (https://doi.org/10.1016/j.jechem.2018.03.004) discuss the challenges of Na metal anode, and then summarize several strategies to suppress dendrite growth and improve electrochemical performance, including interface engineering, electrolyte composition, electrode construction, and so on.
The last but not least system is lead-carbon battery (LCB) that is the new generation of lead-acid batteries. It is well known for its superior performance in partial-state-of-charge operation. Lin et al. (https://doi.org/10.1016/j.jechem.2018.03.002) report the novel lead-carbon anode with C/Pb composite, which displays excellent chargedischarge reversibility.
In summary, these outstanding contributions present the cutting-edge research and excellent collection of the field of energy electrochemistry. We would like to sincerely thank the authors for their great efforts in preparing high-quality manuscripts and the expert reviewers for providing constructive comments and helpful suggestions, which contributed substantially to the high scientific level of this issue. We also thank the efficient and professional editorial office of J. Energy Chem. for their tremendous efforts to make this issue such a great success.

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Water induced phase segregation in hydrocarbon proton exchange membranes

Kangjie Lyu, Yanqiu Peng, Li Xiao, Juntao Lu, Lin Zhuang

2018, 27(6): 1517-1520. DOI: 10.1016/j.jechem.2018.05.009

摘要 ( 1412 )

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Proton exchange membranes (PEMs) are a key material for proton exchange membrane fuel cells (PEM-FCs). Non-fluorinated hydrocarbon PEMs are low-cost alternatives to Nafion, but limited by the low proton conductivity, because of the weak phase segregation structure and narrow ion-transport channels. Various efforts have been taken to improve the performance of hydrocarbon PEMs, but mostly with complex methodologies. Here we demonstrate a simple, yet very efficient method to create phase segregation structure inside a typical hydrocarbon PEM, sulfonated poly(ether ether ketone) (SPEEK). By simply adding appropriate amounts of water into the DMF solvent, the resulting SPEEK membrane exhibits widened ion-transport channels, with the phase size of 2.7 nm, as indicated by both molecular dynamic (MD) simulations and transmission electron microscope (TEM) observations, and the proton conductivity is thus improved by 200%. These findings not only further our fundamental understanding of hydrocarbon PEMs, but are also valuable to the development of low-cost and practical fuel cell technologies.

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The development in aqueous lithium-ion batteries

Duan Bin, Yunping Wen, Yonggang Wang, Yongyao Xia

2018, 27(6): 1521-1535. DOI: 10.1016/j.jechem.2018.06.004

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To meet the growing energy demands, it is urgent for us to construct grid-scale energy storage system than can connect sustainable energy resources. Aqueous Li-ion batteries (ALIBs) have been widely investigated to become the most promising stationary power sources for sustainable energy such as wind and solar power. It is believed that advantages of ALIBs will overcome the limitations of the traditional organic lithium battery in virtue of the safety and environmentally friendly aqueous electrolyte. In the past decades, plentiful works have been devoted to enhance the performance of different types of ALIBs. In this review, we discuss the development of cathode, anode and electrolyte for acquiring the desired electrochemical performance of ALIBs. Also, the main challenges and outlook in this field are briefly discussed.

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The application of nanostructured transition metal sulfides as anodes for lithium ion batteries

Jinbao Zhao, Yiyong Zhang, Yunhui Wang, He Li, Yueying Peng

2018, 27(6): 1536-1554. DOI: 10.1016/j.jechem.2018.01.009

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With wide application of electric vehicles and large-scale in energy storage systems, the requirement of secondary batteries with higher power density and better safety gets urgent. Owing to the merits of high theoretical capacity, relatively low cost and suitable discharge voltage, much attention has been paid to the transition metal sulfides. Recently, a large amount of research papers have reported about the application of transition metal sulfides in lithium ion batteries. However, the practical application of transition metal sulfides is still impeded by their fast capacity fading and poor rate performance. More well-focused researches should be operated towards the commercialization of transition metal sulfides in lithium ion batteries. In this review, recent development of using transition metal sulfides such as copper sulfides, molybdenum sulfides, cobalt sulfides, and iron sulfides as electrode materials for lithium ion batteries is presented. In addition, the electrochemical reaction mechanisms and synthetic strategy of transition metal sulfides are briefly summarized. The critical issues, challenges, and perspectives providing a further understanding of the associated electrochemical processes are also discussed.

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Recent progress on confinement of polysulfides through physical and chemical methods

Sheng-Yi Li, Wen-Peng Wang, Hui Duan, Yu-Guo Guo

2018, 27(6): 1555-1565. DOI: 10.1016/j.jechem.2018.04.014

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With high theoretical energy density and the natural abundance of S, lithium-sulfur (Li-S) batteries are considered to be the promising next generation high-energy rechargeable energy storage devices. However, issues including electronical insulation of S, the lithium polysulfides (LiPSs) dissolution and the short cycle lifespan have prevented Li-S batteries from being practical applied. Feasible settlements of confining LiPSs to reduce the loss of active substances and improve the cycle stability include wrapping sulfur with compact layers, designing matrix with porous or hollow structures, adding adsorbents owning strong interaction with sulfur and inserting polysulfide barriers between cathodes and separators. This review categorizes them into physical and chemical confinements according to the influencing mechanism. With further discussion of their merits and flaws, synergy of the physical and chemical confinement is believed to be the feasible avenue that can guide Li-S batteries to the practical application.

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The application of synchrotron X-ray techniques to the study of rechargeable batteries

Zhengliang Gong, Yong Yang

2018, 27(6): 1566-1583. DOI: 10.1016/j.jechem.2018.03.020

摘要 ( 1024 )

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The increased use of rechargeable batteries in portable electronic devices and the continuous development of novel applications (e.g. transportation and large scale energy storage), have raised a strong demand for high performance batteries with increased energy density, cycle and calendar life, safety and lower costs. This triggers significant efforts to reveal the fundamental mechanism determining battery performance with the use of advanced analytical techniques. However, the inherently complex characteristics of battery systems make the mechanism analysis sophisticated and difficult. Synchrotron radiation is an advanced collimated light source with high intensity and tunable energies. It has particular advantages in electronic structure and geometric structure (both the short-range and long-range structure) analysis of materials on different length and time scales. In the past decades, synchrotron X-ray techniques have been widely used to understand the fundamental mechanism and guide the technological optimization of batteries. In particular, in situ and operando techniques with high spatial and temporal resolution, enable the nondestructive, real time dynamic investigation of the electrochemical reaction, and lead to significant deep insights into the battery operation mechanism.
This review gives a brief introduction of the application of synchrotron X-ray techniques to the investigation of battery systems. The five widely implicated techniques, including X-ray diffraction (XRD), Pair Distribution Function (PDF), Hard and Soft X-ray absorption spectroscopy (XAS) and X-ray photoelectron spectroscopy (XPS) will be reviewed, with the emphasis on their in situ studies of battery systems during cycling.

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Advanced Na metal anodes

Chenglong Zhao, Yaxiang Lu, Jinming Yue, Du Pan, Yuruo Qi, Yong-Sheng Hu, Liquan Chen

2018, 27(6): 1584-1596. DOI: 10.1016/j.jechem.2018.03.004

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Na metal anode, benefiting from its high theoretical capacity and lowest electrochemical potential, is one of the most favorable candidates for future Na-based batteries with high energy density. Dendrite growth, volume change and high reactivity are the formidable challenges in terms of good cycling performance and high Coulombic efficiency as well as an expected safety guarantee of Na metal anode for the practical application. Solid electrolyte interphase (SEI) layer as an indispensable component of a battery, its formation and stability play the critical role in the feasibility of Na metal anode. In this review, we first discuss the current consideration and challenges of Na metal anode, and then summarize several strategies to suppress dendrite growth and improve electrochemical performance, including interface engineering, electrolyte composition, electrode construction, and so on. Finally, the conclusion and future perspective of potential development on Na metal anode are proposed.

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Progress and prospect for NASICON-type Na₃V₂(PO₄)₃ for electrochemical energy storage

Qiong Zheng, Hongming Yi, Xianfeng Li, Huamin Zhang

2018, 27(6): 1597-1617. DOI: 10.1016/j.jechem.2018.05.001

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Sodium-ion batteries (SIBs) have attracted increasing attention in the past decades, because of high overall abundance of precursors, their even geographical distribution, and low cost. Na₃V₂(PO₄)₃ (NVP), a typical sodium super ion conductor (NASICON)-based electrode material, exhibits pronounced structural stability, exceptionally high ion conductivity, rendering it a most promising electrode for sodium storage. However, the comparatively low electronic conductivity makes the theoretical capacity of NVP cannot be fully accessible even at comparatively low rates, presenting a major drawback for further practical applications, especially when high rate capability is especially important. Thus, many endeavors have been conformed to increase the surface and intrinsic electrical conductivity of NVP by coating the active materials with a conductive carbon layer, downsizing the NVP particles, combining the NVP particle with various carbon materials and ion doping strategy. In this review, to get a better understanding on the sodium storage in NVP, we firstly present 4 distinct crystal structures in the temperature range of -30℃~225℃ namely α-NVP, β-NVP, β'-NVP and γ-NVP. Moreover, we give an overview of recent approaches to enhance the surface electrical conductivity and intrinsic electrical conductivity of NVP. Finally, some potential applications of NVP such as in all-climate environment and PHEV, EV fields have been prospected.

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Recent development of methanol electrooxidation catalysts for direct methanol fuel cell

Liyuan Gong, Zhiyuan Yang, Kui Li, Wei Xing, Changpeng Liu, Junjie Ge

2018, 27(6): 1618-1628. DOI: 10.1016/j.jechem.2018.01.029

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Direct methanol fuel cells (DMFCs) are very promising power source for stationary and portable miniature electric appliances due to its high efficiency and low emissions of pollutants. As the key material, catalysts for both cathode and anode face several problems which hinder the commercialization of DMFCs. In this review, we mainly focus on anode catalysts of DMFCs. The process and mechanism of methanol electrooxidation on Pt and Pt-based catalysts in acidic medium have been introduced. The influences of size effect and morphology on electrocatalytic activity are discussed though whether there is a size effect in MOR catalyst is under debate. Besides, the non Pt catalysts are also listed to emphasize though Pt is still deemed as the indispensable element in anode catalyst of DMFCs in acidic medium. Different catalyst systems are compared to illustrate the level of research at present. Some debates need to be verified with experimental evidences.

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Selective electrocatalytic conversion of methane to fuels and chemicals

Shunji Xie, Shengqi Lin, Qinghong Zhang, Zhongqun Tian, Ye Wang

2018, 27(6): 1629-1636. DOI: 10.1016/j.jechem.2018.03.015

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The increase in natural gas reserves makes methane a significant hydrocarbon feedstock. However, the direct catalytic conversion of methane into liquid fuels and useful chemicals remains a great challenge, and many studies have been devoted to this field in the past decades. Electrocatalysis is considered as an important alternative approach for the direct conversion of methane into value-added chemicals, although many other innovative methods have been developed. This review highlights recent advances in electrocatalytic conversion of methane to ethylene and methanol, two important chemicals. The electrocatalytic systems efficient for methane conversions are summarized with an emphasis on catalysts and electrolytes. The effects of reaction conditions such as the temperature and the acid-base property of the reaction medium are also discussed.

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Porous core-shell CoMn₂O₄ microspheres as anode of lithium ion battery with excellent performances and their conversion reaction mechanism investigated by XAFS

Hang Su, Yue-Feng Xu, Shou-Yu Shen, Jian-Qiang Wang, Jun-Tao Li, Ling Huang, Shi-Gang Sun

2018, 27(6): 1637-1643. DOI: 10.1016/j.jechem.2018.04.009

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Porous core-shell CoMn₂O₄ microspheres of ca. 3-5μm in diameter were synthesized and served as anode of lithium ion battery. Results demonstrate that the as-synthesized CoMn₂O₄ materials exhibit excellent electrochemical properties. The CoMn₂O₄ anode can deliver a large capacity of 1070 mAh g^-1 in the first discharge, a reversible capacity of 500 mAh g^-1 after 100 cycles with a coulombic efficiency of 98.5% at a charge-discharge current density of 200 mA g^-1, and a specific capacity of 385 mAh g^-1 at a much higher charge-discharge current density of 1600 mA g^-1. Synchrotron X-ray absorption fine structure (XAFS) techniques were applied to investigate the conversion reaction mechanism of the CoMn₂O₄ anode. The X-ray absorption near edge structure (XANES) spectra revealed that, in the first discharge-charge cycle, Co and Mn in CoMn₂O₄ were reduced to metallic Co and Mn when the electrode was discharged to 0.01 V, while they were oxidized respectively to CoO and MnO when the electrode was charged to 3.0 V. Experiments of both XANES and extended X-ray absorption fine structure (EXAFS) revealed that neither valence evolution nor phase transition of the porous core-shell CoMn₂O₄ microspheres could happen in the discharge plateau from 0.8 to 0.6 V, which demonstrates the formation of solid electrolyte interface (SEI) on the anode.

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Core-shell structured 1,4-benzoquinone@TiO₂ cathode for lithium batteries

Aikai Yang, Xingchao Wang, Yong Lu, Licheng Miao, Wei Xie, Jun Chen

2018, 27(6): 1644-1650. DOI: 10.1016/j.jechem.2018.06.003

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Organic carbonyl compounds are considered as promising candidates for lithium batteries due to their high capacity and environmental friendliness. However, they suffer from serious dissolution in the electrolyte, leading to fast capacity decay. Here we report core-shell structured 1,4-benzoquinone@titanium dioxide (BQ@TiO₂) composite as cathode for lithium batteries. The composite cathode can deliver a high discharge capacity of 441.2 mA h/g at 50 mA/g and a high capacity retention of 80.7% after 100 cycles. The good cycling performance of BQ@TiO₂ composite can be attributed to the suppressed dissolution of BQ, which results from the physical confinement effect of TiO₂ shell and the strong interactions between BQ and TiO₂. Moreover, the combination of ex situ infrared spectra and density functional theory calculations reveals that the active redox sites of BQ are carbonyl groups. This work provides an alternative way to mitigate the dissolution of small carbonyl compounds and thus enhance their cycling stability.

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All boron-based 2D material as anode material in Li-ion batteries

Ning Jiang, Biao Li, Fanghua Ning, Dingguo Xia

2018, 27(6): 1651-1654. DOI: 10.1016/j.jechem.2018.01.026

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To design the high-energy-density Li-ion batteries, the anode materials with high specific capacity have attracted much attention. In this work, we adopt the first principles calculations to investigate the possibility of a new two dimensional boron material, named B_G, as anode material for Li-ion batteries. The calculated results show that the maximum theoretical specific capacity of B_G is 1653 mAh g^-1 (LiB_1.5). Additionally, the energy barriers of Li ion and Li vacancy diffusion are 330 meV and 110 meV, respectively, which imply fast charge and discharge ability for B_G as an anode material. The theoretical findings reported in this work suggest that B_G is a potential candidate as anode material of high-energy-density Li-ion batteries.

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In situ X-ray diffraction and thermal analysis of LiNi_0.8Co_0.15Al_0.05O₂ synthesized via co-precipitation method

Na Zhang, Xiaoyu Zhang, Erbo Shi, Shiyong Zhao, Kezhu Jiang, Di Wang, Pengfei Wang, Shaohua Guo, Ping He, Haoshen Zhou

2018, 27(6): 1655-1660. DOI: 10.1016/j.jechem.2018.06.007

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LiNi_0.8Co_0.15Al_0.05O₂ (NCA) material is successfully synthesized with a modified co-precipitation method, in which NH₃·H₂O and EDTA are used as two chelating agents. The obtained LiNi_0.8Co_0.15Al_0.05O₂ material has well-defined layered structure and uniform element distribution, which reveals an enhanced electrochemical performance with a capacity retention of 97.9% after 100 cycles at 0.2 C, and reduced thermal runaway from the isothermal calorimetry test. In situ X-ray diffraction (XRD) was employed to capture the structural changes during the charge-discharge process. The reversible evolutions of lattice parameters (a, b, c, and V) further verify the structural stability.

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Hierarchically porous nitrogen-doped carbon as cathode for lithium-sulfur batteries

Rui Wu, Siguo Chen, Jianghai Deng, Xun Huang, Yujie Song, Ruiyi Gan, Xiaoju Wan, Zidong Wei

2018, 27(6): 1661-1667. DOI: 10.1016/j.jechem.2018.02.010

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Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellent conductivity, stable physicochemical properties, easy processability, controllable porosity and low price. Herein, we reported a novel well-designed hierarchically porous nitrogen-doped carbon (HPNC) via a combination of salt template (ZnCl₂) and hard template (SiO₂) as sulfur host for lithium-sulfur batteries. The low-melting ZnCl₂ is boiled off and leaves behind micropores and small size mesopores during pyrolysis process, while the silica spheres are removed by acid leaching to generate interconnected 3D network of macropores. The HPNC-S electrode exhibits an initial specific capacity of 1355 mAh g^-1 at 0.1 C (1 C=1675 mAh g^-1), a high-rate capability of 623 mAh g^-1 at 2 C, and a small decay of 0.13% per cycle over 300 cycles at 0.2 C. This excellent rate capability and remarkable long-term cyclability of the HPNC-S electrode are attributed to its hierarchical porous structures for confining the soluble lithium polysulfide as well as the nitrogen doping for high absorbability of lithium polysulfide.

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Correlating Fe source with Fe-N-C active site construction: Guidance for rational design of high-performance ORR catalyst

Liqin Gao, Meiling Xiao, Zhao Jin, Changpeng Liu, Jianbing Zhu, Junjie Ge, Wei Xing

2018, 27(6): 1668-1673. DOI: 10.1016/j.jechem.2018.06.008

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Pyrolyzed Fe-N_X/C materials derived from Fe-doped ZIF-8 are recently emerged as promising alternatives to noble metal platinum-based catalysts towards oxygen reduction reaction (ORR) and elucidating the dependacne of Fe source on the active site structure and final ORR performance is highly desirbale for further development of these materials. Here, we designed and synthesized a series of Fe-N-C catalysts using ZIF-8 and various iron salts (Fe(acac)₃, FeCl₃, Fe(NO₃)₃) as precusors. We found that the iron precursors, mainly the molecular size, hydrolysis extent, do play a major role in determining the final morphology of Fe, namely forming the Fe-Nx coordination or Fe₃C nanoparticles, as well as the site density, therefore, significantly affecting the ORR activity. Among the three iron sources, Fe(acac)₃ is most advantageous to the preferential formation of single-atom Fe-Nx active sites and the derived catalyst demonstrated best ORR performance.

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Highly reversible lead-carbon battery anode with lead grafting on the carbon surface

Jian Yin, Nan Lin, Wenli Zhang, Zheqi Lin, Ziqing Zhang, Yue Wang, Jun Shi, Jinpeng Bao, Haibo Lin

2018, 27(6): 1674-1683. DOI: 10.1016/j.jechem.2018.03.002

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A novel C/Pb composite has been successfully prepared by electroless plating to reduce the hydrogen evolution and achieve the high reversibility of the anode of lead-carbon battery (LCB). The deposited lead on the surface of C/Pb composite was found to be uniform and adherent to carbon surface. Because lead has been stuck on the surface of C/Pb composite, the embedded structure suppresses the hydrogen evolution of lead-carbon anode and strengthens the connection between carbon additive and sponge lead. Compared with the blank anode, the lead-carbon anode with C/Pb composite displays excellent charge-discharge reversibility, which is attributed to the good connection between carbon additives and lead that has been stuck on the surface of C/Pb composite during the preparation process. The addition of C/Pb composite maintains a solid anode structure with high specific surface area and power volume, and thereby, it plays a significant role in the highly reversible lead-carbon anode.

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