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Overcoming the Electrode Challenges of High-Temperature Proton Exchange Membrane Fuel Cells Quentin Meyer, Chujie Yang, Yi Cheng, Chuan Zhao Electrochemical Energy Reviews    2023, 6 (2): 16-.   DOI: 10.1007/s41918-023-00180-y Abstract （847）      PDF       Knowledge map    Save Proton exchange membrane fuel cells (PEMFCs) are becoming a major part of a greener and more sustainable future. However, the costs of high-purity hydrogen and noble metal catalysts alongside the complexity of the PEMFC system severely hamper their commercialization. Operating PEMFCs at high temperatures (HT-PEMFCs, above 120 °C) brings several advantages, such as increased tolerance to contaminants, more affordable catalysts, and operations without liquid water, hence considerably simplifying the system. While recent progresses in proton exchange membranes for HT-PEMFCs have made this technology more viable, the HT-PEMFC viscous acid electrolyte lowers the active site utilization by unevenly diffusing into the catalyst layer while it acutely poisons the catalytic sites. In recent years, the synthesis of platinum group metal (PGM) and PGM-free catalysts with higher acid tolerance and phosphate-promoted oxygen reduction reaction, in conjunction with the design of catalyst layers with improved acid distribution and more triple-phase boundaries, has provided great opportunities for more efficient HT-PEMFCs. The progress in these two interconnected fields is reviewed here, with recommendations for the most promising routes worthy of further investigation. Using these approaches, the performance and durability of HT-PEMFCs will be significantly improved. Related Articles | Metrics | Comments（0）

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Addressing Transport Issues in Non-Aqueous Li–air Batteries to Achieving High Electrochemical Performance Zhuojun Zhang, Xu Xiao, Xingbao Zhu, Peng Tan Electrochemical Energy Reviews    2023, 6 (2): 18-.   DOI: 10.1007/s41918-022-00157-3 Abstract （213）      PDF       Knowledge map    Save Li–air batteries are a promising type of energy storage technology because of the ultra-high theoretical specific energy. Great advances are made in recent years, including the illustration of reaction mechanisms, development of effective catalyst materials, and design of battery structures accelerating species transport. However, the application still suffers from low rate capability, poor round-trip efficiency, and unsatisfactory cycling life. Herein, we mainly focus on the species transport issues of non-aqueous Li–air batteries, including Li+ across the solid surfaces and the electrolyte, O2 solubility and diffusivity, distribution of intermediates and products, and side reactions by other components from the air. Besides, considerable emphasis is paid to expound the approaches for enhancing species transport and accelerating reactions, among which the realization of well-designed electrode structures and flowing electrolytes is of great significance for the rapid migration of O2 and Li+ and mitigating the negative effects by solid insoluble Li2O2. Moreover, optimizing reaction interfaces and operating conditions is an attractive alternative to promote reaction rates. This work aims to identify the mechanism of transport issues and corresponding challenges and perspectives, guiding the structure design and material selection to achieve high-performance Li–air batteries. Related Articles | Metrics | Comments（0）

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Recent Advancements in Photoelectrochemical Water Splitting for Hydrogen Production Yibo Zhao, Zhenjie Niu, Jiwu Zhao, Lan Xue, Xianzhi Fu, Jinlin Long Electrochemical Energy Reviews    2023, 6 (2): 14-.   DOI: 10.1007/s41918-022-00153-7 Abstract （905）      PDF       Knowledge map    Save Sunlight is the most abundant and inexhaustible energy source on earth. However, its low energy density, dispersibility and intermittent nature make its direct utilization with industrial relevance challenging, suggesting that converting sunlight into chemical energy and storing it is a valuable measure to achieve global sustainable development. Carbon–neutral, clean and secondary pollution-free solar-driven water splitting to produce hydrogen is one of the most attractive avenues among all the current options and is expected to realize the transformation from dependence on fossil fuels to zero-pollution hydrogen. Artificial photosynthetic systems (APSs) based on photoelectrochemical (PEC) devices appear to be an ideal avenue to efficiently achieve solar-to-hydrogen conversion. In this review, we comprehensively highlight the recent developments in photocathodes, including architectures, semiconductor photoabsorbers and performance optimization strategies. In particular, frontier research cases of organic semiconductors, dye sensitization and surface grafted molecular catalysts applied to APSs based on frontier (molecular) orbital theory and semiconductor energy band theory are discussed. Moreover, research advances in typical photoelectrodes with the metal–insulator–semiconductor (MIS) architecture based on quantum tunnelling are also introduced. Finally, we discuss the benchmarks and protocols for designing integrated tandem photoelectrodes and PEC systems that conform to the solar spectrum to achieve high-efficiency and cost-effective solar-to-hydrogen conversion at an industrial scale in the near future. Related Articles | Metrics | Comments（0）

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Interfaces in Sulfide Solid Electrolyte-Based All-Solid-State Lithium Batteries: Characterization, Mechanism and Strategy Zhan Wu, Xiaohan Li, Chao Zheng, Zheng Fan, Wenkui Zhang, Hui Huang, Yongping Gan, Yang Xia, Xinping He, Xinyong Tao, Jun Zhang Electrochemical Energy Reviews    2023, 6 (2): 10-.   DOI: 10.1007/s41918-022-00176-0 Abstract （1021）      PDF       Knowledge map    Save Owing to the advantages of high energy density and environmental friendliness, lithium-ion batteries (LIBs) have been widely used as power sources in electric vehicles, energy storage systems and other devices. Conventional LIBs composed of liquid electrolytes (LEs) have potential safety hazards; thermal runaway easily leads to battery explosion and spontaneous combustion. To realize a large-scale energy storage system with higher safety and higher energy density, replacing LEs with solid-state electrolytes (SSEs) has been pursued. Among the many SSEs, sulfide SSEs are attractive because of their high ionic conductivities, easy processabilities and high thermostabilities. However, interfacial issues (interfacial reactions, chemomechanical failure, lithium dendrite formation, etc.) between sulfide SSEs and electrodes are factors limiting widespread application. In addition, the intrinsic interfacial issues of sulfide SSEs (electrochemical windows, diffusion mechanisms of Li+, etc.) should not be ignored. In this review, the behaviors, properties and mechanisms of interfaces in all-solid-state lithium batteries with a variety of sulfide SSEs are comprehensively summarized. Additionally, recent research progress on advanced characterization methods and designs used to stabilize interfaces is discussed. Finally, outlooks, challenges and possible interface engineering strategies are analyzed and proposed. Related Articles | Metrics | Comments（0）

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High-Energy Room-Temperature Sodium-Sulfur and Sodium-Selenium Batteries for Sustainable Energy Storage Zefu Huang, Pauline Jaumaux, Bing Sun, Xin Guo, Dong Zhou, Devaraj Shanmukaraj, Michel Armand, Teofilo Rojo, Guoxiu Wang Electrochemical Energy Reviews    2023, 6 (3): 21-.   DOI: 10.1007/s41918-023-00182-w Abstract （274）      PDF       Knowledge map    Save Rechargeable room-temperature sodium-sulfur (Na-S) and sodium-selenium (Na-Se) batteries are gaining extensive attention for potential large-scale energy storage applications owing to their low cost and high theoretical energy density. Optimization of electrode materials and investigation of mechanisms are essential to achieve high energy density and long-term cycling stability of Na-S(Se) batteries. Herein, we provide a comprehensive review of the recent progress in Na-S(Se) batteries. We elucidate the Na storage mechanisms and improvement strategies for battery performance. In particular, we discuss the advances in the development of battery components, including high-performance sulfur cathodes, optimized electrolytes, advanced Na metal anodes and modified separators. Combined with current research achievements, this review outlines remaining challenges and clear research directions for the future development of practical high-performance Na-S(Se) batteries. Related Articles | Metrics | Comments（0）

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Li-S Batteries: Challenges, Achievements and Opportunities Hassan Raza, Songyan Bai, Junye Cheng, Soumyadip Majumder, He Zhu, Qi Liu, Guangping Zheng, Xifei Li, Guohua Chen Electrochemical Energy Reviews    2023, 6 (3): 29-.   DOI: 10.1007/s41918-023-00188-4 Abstract （437）      PDF       Knowledge map    Save To realize a low-carbon economy and sustainable energy supply, the development of energy storage devices has aroused intensive attention. Lithium-sulfur (Li-S) batteries are regarded as one of the most promising next-generation battery devices because of their remarkable theoretical energy density, cost-effectiveness, and environmental benignity. However, the practical application of Li-S batteries is hindered by such challenges as low sulfur utilization (< 80%), fast capacity fade, short service life (< 200 redox cycles), and severe self-discharge. The reasons behind the challenges are: (1) low conductivity of the active materials, (2) large volume changes during redox cycling, (3) serious polysulfide shuttling and, (4) lithium-metal anode contamination/corrosion and dendrite formation. Significant achievements have been made to address these problems in the past decade. In this review, the recent advances in material synthesis and technology development are analysed in terms of the electrochemical performance of different Li-S battery components. The critical analysis was conducted based on the merits and shortcomings of the reported work on the issues facing the individual component. A versatile 3D-printing technique is also examined on its practicability for Li-S battery production. The insights on the rational structural design and reasonable parameters for Li-S batteries are highlighted along with the “five 5s” concept from a practical point of view. The remaining challenges are outlined for researchers to devote more efforts on the understanding and commercialization of the devices in terms of the material preparation, cell manufacturing, and characterization. Related Articles | Metrics | Comments（0）

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Structure, Property, and Performance of Catalyst Layers in Proton Exchange Membrane Fuel Cells Jian Zhao, Huiyuan Liu, Xianguo Li Electrochemical Energy Reviews    2023, 6 (2): 13-.   DOI: 10.1007/s41918-022-00175-1 Abstract （849）      PDF       Knowledge map    Save Catalyst layer (CL) is the core component of proton exchange membrane (PEM) fuel cells, which determines the performance, durability, and cost. However, difficulties remain for a thorough understanding of the CLs’ inhomogeneous structure, and its impact on the physicochemical and electrochemical properties, operating performance, and durability. The inhomogeneous structure of the CLs is formed during the manufacturing process, which is sensitive to the associated materials, composition, fabrication methods, procedures, and conditions. The state-of-the-art visualization and characterization techniques are crucial to examine the CL structure. The structure-dependent physicochemical and electrochemical properties are then thoroughly scrutinized in terms of fundamental concepts, theories, and recent progress in advanced experimental techniques. The relation between the CL structure and the associated effective properties is also examined based on experimental and theoretical findings. Recent studies indicated that the CL inhomogeneous structure also strongly affects the performance and degradation of the whole fuel cell, and thus, the interconnection between the fuel cell performance, failure modes, and CL structure is comprehensively reviewed. An analytical model is established to understand the effect of the CL structure on the effective properties, performance, and durability of the PEM fuel cells. Finally, the challenges and prospects of the CL structure-associated studies are highlighted for the development of high-performing PEM fuel cells. Related Articles | Metrics | Comments（0）

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Leap of Li Metal Anodes from Coin Cells to Pouch Cells: Challenges and Progress Qian Wang, Tiantian Lu, Yuanbin Xiao, Jianyang Wu, Lixiang Guan, Lifeng Hou, Huayun Du, Huan Wei, Xiaoda Liu, Chengkai Yang, Yinghui Wei, Henghui Zhou, Yan Yu Electrochemical Energy Reviews    2023, 6 (3): 22-.   DOI: 10.1007/s41918-023-00185-7 Abstract （238）      PDF       Knowledge map    Save Li metal anodes have attracted tremendous attention in the last decade because of their high theoretical capacities and low electrochemical potentials. However, until now, there has only been limited success in improving the interfacial and structural stabilities and in realizing the highly controllable and large-scale fabrication of this emerging material; these limitations have posed great obstacles to further performing fundamental and applied studies in Li metal anodes. In this review, we focus on summarizing the existing challenges of Li metal anodes based on the leap from coin cells to pouch cells and on outlining typical methods for designing Li metal anodes on demand; we controllably engineer their surface protection layers and structure sizes by encapsulating structured Li metal inside a variety of synthetic protection layers. We aim to provide a comprehensive understanding and serve as a strategic guide for designing and fabricating practicable Li metal anodes for use in pouch batteries. Challenges and opportunities regarding this burgeoning field are critically evaluated at the end of this review.Li metal anode has attracted tremendous attention in the last decade because of its high theoretical capacity and low electrochemical potential. However, till now, there is only limited success in improving its interface stability and structure stability, as well as realizing the highly controllable and large-scaled fabrication of this emerging material, posing great obstacles to further promoting its fundamental and applied studies. In this review, we focus on summarizing the existing challenges of Li metal anode based on the leap from coin cells to pouch cells and outlining the typical solutions for designing Li metal anode on-demand through controllably engineering its surface protection layer and structure size, which trend is encapsulating structured Li metal inside a variety of synthetic protection layer. We aim to provide a comprehensive understanding and serve as a strategic guidance for designing and fabricating practicable Li metal anode using in pouch batteries. Challenges and opportunities regarding this burgeoning field are also critically evaluated at the end of this review. Related Articles | Metrics | Comments（0）

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Engineering, Understanding, and Optimizing Electrolyte/Anode Interfaces for All-Solid-State Sodium Batteries Wenhao Tang, Ruiyu Qi, Jiamin Wu, Yinze Zuo, Yiliang Shi, Ruiping Liu, Wei Yan, Jiujun Zhang Electrochemical Energy Reviews    2024, 7 (3): 23-.   DOI: 10.1007/s41918-024-00228-7 Abstract （437）      PDF       Knowledge map    Save Rechargeable all-solid-state sodium batteries (ASS-SBs), including all-solid-state sodium-ion batteries and all-solid-state sodium-metal batteries, are considered highly advanced electrochemical energy storage technologies. This is owing to their potentially high safety and energy density and the high abundance of sodium resources. However, these materials are limited by the properties of their solid-state electrolytes (SSEs) and various SSE/Na interfacial challenges. In recent years, extensive research has focused on understanding the interfacial behavior and strategies to overcome the challenges in developing ASS-SBs. In this prospective, the sodium-ion conduction mechanisms in different SSEs and the interfacial failure mechanisms of their corresponding batteries are comprehensively reviewed in terms of chemical/electrochemical stability, interfacial contacts, sodium dendrite growth, and thermal stability. Based on mechanistic analysis, representative interfacial engineering strategies for the interface between SSEs and Na anodes are summarized. Advanced techniques, including in situ/ex situ instrumental and electrochemical measurements and analysis for interface characterization, are also introduced. Furthermore, advanced computer-assisted methods, including artificial intelligence and machine learning (which can complement experimental systems), are discussed. The purpose of this review is to outline the solid-state electrolyte and electrolyte/anode interface challenges, and the potential research directions for overcoming these challenges. This would enable target-oriented research for the development of solid-state electrochemical energy storage devices. Related Articles | Metrics | Comments（0）

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Carbon-Based Electrodes for Advanced Zinc-Air Batteries: Oxygen-Catalytic Site Regulation and Nanostructure Design Wenjie Shao, Rui Yan, Mi Zhou, Lang Ma, Christina Roth, Tian Ma, Sujiao Cao, Chong Cheng, Bo Yin, Shuang Li Electrochemical Energy Reviews    2023, 6 (2): 11-.   DOI: 10.1007/s41918-023-00181-x Abstract （863）      PDF       Knowledge map    Save Zn-air batteries are highly attractive for direct chemical-to-electrical energy conversion and for solving the energy crisis and environmental problems. Designing efficient oxygen electrodes has been considered one of the most critical steps in the development of advanced Zn-air batteries because of the sluggish kinetics of the oxygen reduction reaction and the oxygen evolution reaction. In recent years, nanostructured carbon-based electrodes with large surface areas, efficient oxygen-catalytic centers, and hierarchically porous matrices have provided significant opportunities to optimize the performance of the oxygen electrodes in both primary and rechargeable Zn-air batteries. In this review, we provide a comprehensive summary of the reported nanostructured carbon-based electrodes for advanced Zn-air batteries in terms of tailoring the oxygen-catalytic sites and designing carbon supports. The versatile synthetic strategies, characterization methods, and in-depth understanding of the relationships between the oxygen-catalytic sites/nanostructures and the oxygen electrode performance are systematically summarized. Furthermore, we also briefly outline recent progress in engineering flexible and high-power Zn-air batteries. Ultimately, a thorough discussion of current primary challenges and future perspectives on the rational design of nanostructured carbon-based oxygen electrodes is given, thus providing inspiration for the future prosperity of fast-kinetic and efficient Zn-air batteries in a broad range of energy fields. Related Articles | Metrics | Comments（0）

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Advanced Catalyst Design Strategies and In-Situ Characterization Techniques for Enhancing Electrocatalytic Activity and Stability of Oxygen Evolution Reaction Cejun Hu, Yanfang Hu, Bowen Zhang, Hongwei Zhang, Xiaojun Bao, Jiujun Zhang, Pei Yuan Electrochemical Energy Reviews    2024, 7 (3): 19-.   DOI: 10.1007/s41918-024-00219-8 Abstract （453）      PDF       Knowledge map    Save Water electrolysis for hydrogen production holds great promise as an energy conversion technology. The electrolysis process contains two necessary electrocatalytic reactions, one is the hydrogen evolution reaction (HER) at the cathode, and the other is the oxygen evolution reaction (OER) at the anode. In general, the kinetics of OER is much slower than that of HER, dominating the overall of performance electrolysis. As identified, the slow kinetics of catalytic OER is mainly resulted from multiple electron transfer steps, and the catalysts often undergo compositional, structural, and electronic changes during operation, leading to complicated dynamic reaction mechanisms which have not been fully understood. Obviously, this challenge presents formidable obstacles to the development of highly efficient OER electrocatalysts. To address the issue, it is crucial to unravel the origins of intrinsic OER activity and stability and elucidate the catalytic mechanisms across diverse catalyst materials. In this context, in-situ/operando characterization techniques would play a pivotal role in understanding the catalytic reaction mechanisms by enabling real-time monitoring of catalyst structures under operational conditions. These techniques can facilitate the identification of active sites for OER and provide essential insights into the types and quantities of key reaction intermediates. This comprehensive review explores various catalyst design and synthesis strategies aimed at enhancing the intrinsic OER activity and stability of catalysts and examines the application of advanced in-situ/operando techniques for probing catalyst mechanisms during the OER process. Furthermore, the imperative need for developing innovative in-situ/operando techniques, theoretical artificial intelligence and machine learning and conducting theoretical research to better understand catalyst structural evolution under conditions closely resembling practical OER working states is also deeply discussed. Those efforts should be able to lay the foundation for the improved fabrication of practical OER catalysts. Related Articles | Metrics | Comments（0）

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Recent Progress in and Perspectives on Emerging Halide Superionic Conductors for All-Solid-State Batteries Kaiyong Tuo, Chunwen Sun, Shuqin Liu Electrochemical Energy Reviews    2023, 6 (2): 17-.   DOI: 10.1007/s41918-023-00179-5 Abstract （364）      PDF       Knowledge map    Save Rechargeable all-solid-state batteries (ASSBs) are considered to be the next generation of devices for electrochemical energy storage. The development of solid-state electrolytes (SSEs) is one of the most crucial subjects in the field of energy storage chemistry. The newly emerging halide SSEs have recently been intensively studied for application in ASSBs due to their favorable combination of high ionic conductivity, exceptional chemical and electrochemical stability, and superior mechanical deformability. In this review, a critical overview of the development, synthesis, chemical stability and remaining challenges of halide SSEs is given. The design strategies for optimizing the ionic conductivity of halide SSEs, such as element substitution and crystal structure design, are summarized in detail. Moreover, the associated chemical stability issues in terms of solvent compatibility, humid air stability and corresponding degradation mechanisms are discussed. In particular, advanced in situ/operando characterization techniques applied to halide-based ASSBs are highlighted. In addition, a comprehensive understanding of the interface issues, cost issues, and scalable processing challenges faced by halide-based ASSBs for practical application is provided. Finally, future perspectives on how to design high-performance electrode/electrolyte materials are given, which are instructive for guiding the development of halide-based ASSBs for energy conversion and storage. Related Articles | Metrics | Comments（0）

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Designing Organic Material Electrodes for Lithium-Ion Batteries: Progress, Challenges, and Perspectives Qiyu Wang, Thomas O'Carroll, Fengchun Shi, Yafei Huang, Guorong Chen, Xiaoxuan Yang, Alena Nevar, Natallia Dudko, Nikolai Tarasenko, Jingying Xie, Liyi Shi, Gang Wu, Dengsong Zhang Electrochemical Energy Reviews    2024, 7 (2): 15-.   DOI: 10.1007/s41918-024-00218-9 Abstract （223）      PDF       Knowledge map    Save Organic material electrodes are regarded as promising candidates for next-generation rechargeable batteries due to their environmentally friendliness, low price, structure diversity, and flexible molecular structure design. However, limited reversible capacity, high solubility in the liquid organic electrolyte, low intrinsic ionic/electronic conductivity, and low output voltage are the main problems they face. A lot of research work has been carried out to explore comprehensive solutions to the above problems through molecular structure design, the introduction of specific functional groups and specific molecular frameworks, from small molecules to polymer molecules, metal-organic frameworks (MOFs), covalent organic frameworks (COFs) and heterocyclic molecules; from simple organic materials to organic composites; from single functional groups to multi-functional groups; etc. The inevitable relationship between various molecular structure design and enhanced electrochemical properties has been illustrated in detail. This work also specifically discusses several approaches for the current application of organic compounds in batteries, including interfacial protective layer of inorganic metal oxide cathode, anode (metal lithium or silicon) and solid-state electrolyte, and host materials of sulfur cathode and redox media in lithium-sulfur batteries. This overview provides insight into a deep understanding of the molecular structure of organic electrode materials (OEMs) and electrochemical properties, broadens people’s research ideas, and inspires researchers to explore the advanced application of electroactive organic compounds in rechargeable batteries. Related Articles | Metrics | Comments（0）

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Electrospun Flexible Nanofibres for Batteries: Design and Application P. Robert Ilango, A. Dennyson Savariraj, Hongjiao Huang, Linlin Li, Guangzhi Hu, Huaisheng Wang, Xiaodong Hou, Byung Chul Kim, Seeram Ramakrishna, Shengjie Peng Electrochemical Energy Reviews    2023, 6 (4): 31-.   DOI: 10.1007/s41918-022-00148-4 Abstract （248）      PDF       Knowledge map    Save Flexible and free-standing electrospun nanofibres have been used as electrode materials in electrochemical energy storage systems due to their versatile properties, such as mechanical stability, superb electrical conductivity, and high functionality. In energy storage systems such as metal-ion, metal-air, and metal-sulphur batteries, electrospun nanofibres are vital for constructing flexible electrodes and substantially enhancing their electrochemical properties. The need for flexible batteries has increased with increasing demand for new products such as wearable and flexible devices, including smartwatches and flexible displays. Conventional batteries have several semirigid to rigid components that limit their expansion in the flexible device market. The creation of flexible and wearable batteries with greater mechanical flexibility, higher energy, and substantial power density is critical in meeting the demand for these new electronic items. The implementation of carbon and carbon-derived composites into flexible electrodes is required to realize this goal. It is essential to understand recent advances and the comprehensive foundation behind the synthesis and assembly of various flexible electrospun nanofibres. The design of nanofibres, including those comprising carbon, N-doped carbon, hierarchical, porous carbon, and metal/metal oxide carbon composites, will be explored. We will highlight the merits of electrospun carbon flexible electrodes by describing porosity, surface area, binder-free and free-standing electrode construction, cycling stability, and performance rate. Significant scientific progress has been achieved and logistical challenges have been met in promoting secondary battery usage; therefore, this review of flexible electrode materials will advance this easily used and sought-after technology. The challenges and prospects involved in the timely development of carbon nanofibre composite flexible electrodes and batteries will be addressed. Related Articles | Metrics | Comments（0）

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Si-Based Anodes: Advances and Challenges in Li-Ion Batteries for Enhanced Stability Hongshun Zhao, Jianbin Li, Qian Zhao, Xiaobing Huang, Shuyong Jia, Jianmin Ma, Yurong Ren Electrochemical Energy Reviews    2024, 7 (2): 11-.   DOI: 10.1007/s41918-024-00214-z Abstract （207）      PDF       Knowledge map    Save Owing to their advantages, such as a high energy density, low operating potential, high abundance, and low cost, rechargeable silicon (Si) anode lithium-ion batteries (LIBs) have attracted considerable interest. Significant advancements in Si-based LIBs have been made over the past decade. Nevertheless, because the cycle instability is a crucial factor in the half/full-battery design and significantly affects the consumption of active components and the weight of the assembled battery, it has become a concern in recent years. This paper presents a thorough analysis of the recent developments in the enhancement methods for the stability of LIBs. Comprehensive in situ and operando characterizations are performed to thoroughly evaluate the electrochemical reactions, structural evolution, and degradation processes. Approaches for enhancing the cycle stability of Si anodes are systematically divided from a design perspective into several categories, such as the structural regulation, interfacial design, binder architecture, and electrolyte additives. The advantages and disadvantages of several methods are emphasized and thoroughly evaluated, offering insightful information for the logical design and advancement of cutting-edge solutions to address the deteriorating low-cycle stability of silicon-based LIBs. Finally, the conclusions and potential future research perspectives for promoting the cycling instability of silicon-based LIBs are presented. Related Articles | Metrics | Comments（0）

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Towards High Value-Added Recycling of Spent Lithium-Ion Batteries for Catalysis Application Ruyu Shi, Boran Wang, Di Tang, Xijun Wei, Guangmin Zhou Electrochemical Energy Reviews    2024, 7 (3): 28-.   DOI: 10.1007/s41918-024-00220-1 Abstract （172）      PDF       Knowledge map    Save With the proposal of the global carbon neutrality target, lithium-ion batteries (LIBs) are bound to set off the next wave of applications in portable electronic devices, electric vehicles, and energy-storage grids due to their unique merits. However, the growing LIB market poses a severe challenge for waste management during LIB recycling after end-of-life, which could cause serious environmental pollution and resource waste without proper treatment. Pyrometallurgical, hydrometallurgical, and direct recycling of spent LIBs have been developed, guided by the “waste to wealth” principle, and were applied to LIB remanufacturing. However, some spent LIB materials with low values or great direct regeneration difficulties may not be suitable for the above options, necessitating expanded application ranges of spent LIBs. Considering their unique compositions, using waste electrode materials directly or as precursors to prepare advanced catalysts has been proposed as another promising disposal technology for end-of-life LIBs. For example, transition metal elements in the cathode, like Ni, Co, Mn, and Fe, have been identified as catalytic active centers, and graphite anodes can serve as the catalyst loading matrix. This scheme has been adopted in various catalysis applications, and preliminary progress has been made. Therefore, this review summarizes and discusses the application of spent LIB recycling materials in catalysis and classified it into three aspects: environmental remediation, substance conversion, and battery-related catalysis. Moreover, the existing challenges and possible foci of future research on spent LIB recycling are also discussed. This review is anticipated to mark the start of close attention to the high-value-added applications of spent LIB products, enhancing economic efficiency and sustainable development. Related Articles | Metrics | Comments（0）

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Pathways of the Electrochemical Nitrogen Reduction Reaction: From Ammonia Synthesis to Metal-N2 Batteries Sebastian Cyril Jesudass, Subramani Surendran, Joon Young Kim, Tae-Yong An, Gnanaprakasam Janani, Tae-Hoon Kim, Jung Kyu Kim, Uk Sim Electrochemical Energy Reviews    2023, 6 (3): 27-.   DOI: 10.1007/s41918-023-00186-6 Abstract （269）      PDF       Knowledge map    Save Ammonia is considered as an alternative fuel resource for a sustainable green future. The production of ammonia involves the electrochemical nitrogen reduction reaction (NRR), which has gained considerable attention due to its eco-friendly resources and nonharmful byproducts. Even with the manifold works on NRR, the technique has not reached the industrial scale because of the impediments of NRR electrocatalysts, and in addition, state-of-the-art electrocatalysts have not yet been discovered. In this review, first, the mechanism of the NRR, key metrics, and operational procedures for NRR electrochemistry are presented. Then, the electrocatalyst designs for efficient NRR are briefly introduced, followed by a discussion on the influence of the electrolytes that enhance NRR performance. The counterion effects of electrolytes on NRR performance and strategies for suppressing the HER by electrolyte additives are also discussed. Later, the NRR mechanisms are upgraded, and a comprehensive review of metal-N2 batteries is provided. This review summarizes the effective methods for performing the NRR and strategies to suppress the HER on various electrocatalysts by tuning electrolytes and their additives. The review concludes by discussing the prospects of metal-N2 batteries. Related Articles | Metrics | Comments（0）

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High-Entropy Strategy for Electrochemical Energy Storage Materials Feixiang Ding, Yaxiang Lu, Liquan Chen, Yong-Sheng Hu Electrochemical Energy Reviews    2024, 7 (2): 16-.   DOI: 10.1007/s41918-024-00216-x Abstract （170）      PDF       Knowledge map    Save Electrochemical energy storage technologies have a profound influence on daily life, and their development heavily relies on innovations in materials science. Recently, high-entropy materials have attracted increasing research interest worldwide. In this perspective, we start with the early development of high-entropy materials and the calculation of the configurational entropy. Then, we summarize the recent progress in material design and application using the high-entropy strategy, especially highlighting rechargeable battery materials. Finally, we discuss the potential directions for the future development of high-entropy energy materials. Related Articles | Metrics | Comments（0）

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Building Better Full Manganese-Based Cathode Materials for Next-Generation Lithium-Ion Batteries Jin Song, Hangchao Wang, Yuxuan Zuo, Kun Zhang, Tonghuan Yang, Yali Yang, Chuan Gao, Tao Chen, Guang Feng, Zewen Jiang, Wukun Xiao, Tie Luo, Dingguo Xia Electrochemical Energy Reviews    2023, 6 (3): 20-.   DOI: 10.1007/s41918-023-00184-8 Abstract （241）      PDF       Knowledge map    Save Lithium-manganese-oxides have been exploited as promising cathode materials for many years due to their environmental friendliness, resource abundance and low biotoxicity. Nevertheless, inevitable problems, such as Jahn-Teller distortion, manganese dissolution and phase transition, still frustrate researchers; thus, progress in full manganese-based cathode materials (FMCMs) has been relatively slow and limited in recent decades. Recently, with the fast growth of vehicle electrification and large-scale energy-storage grids, there has been an urgent demand to develop novel FMCMs again; actually, new waves of research based on FMCMs are being created. Herein, we systematically review the history of FMCMs, correctly describe their structures, evaluate the advantages and challenges, and discuss the resolution strategies and latest developments. Additionally, beyond FMCMs, a profound discussion of current controversial issues, such as oxygen redox reaction, voltage decay and voltage hysteresis in Li2MnO3-based cathode materials, is also presented. This review summarizes the effectively optimized approaches and offers a few new possible enhancement methods from the perspective of the electronic-coordination-crystal structure for building better FMCMs for next-generation lithium-ion batteries. Related Articles | Metrics | Comments（0）

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Safety Issues and Improvement Measures of Ni-Rich Layered Oxide Cathode Materials for Li-Ion Batteries Baichuan Cui, Zhenxue Xiao, Shaolun Cui, Sheng Liu, Xueping Gao, Guoran Li Electrochemical Energy Reviews    2024, 7 (3): 27-.   DOI: 10.1007/s41918-024-00211-2 Abstract （114）      PDF       Knowledge map    Save Ni-rich layered oxide cathode materials hold great promise for enhancing the energy density of lithium-ion batteries (LIBs) due to their impressive specific capacity. However, the chemical and structural stability issues associated with the materials containing a high Ni content have emerged as a primary safety concern, particularly in the context of traction batteries for electric vehicles. Typically, when these materials are in a highly charged state, their metastable layered structure and highly oxidized transition metal ions can trigger detrimental phase transitions. This leads to the generation of oxygen gas and the degradation of the material’s microstructure, including the formation of cracks, which can promote the interactions between Ni-rich materials and electrolytes, further generating flammable gases. Consequently, various strategies have been devised at the material level to mitigate potential safety hazards. This review begins by providing an in-depth exploration of the sources of instability in Ni-rich layered oxides, drawing from their crystal and electronic structures, and subsequently outlines the safety issues that arise as a result. Subsequently, it delves into recent advancements and approaches aiming at modifying Ni-rich cathode materials and electrolytes to enhance safety. The primary objective of this review is to offer a concise and comprehensive understanding of why Ni-rich cathode materials are susceptible to safety incidents and to present potential methods for improving the safety of Ni-rich cathode materials in high-density LIBs. Related Articles | Metrics | Comments（0）