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Please wait a minute... For Selected: Download Citations EndNote Ris BibTeX Toggle Thumbnails Select Free-Standing Single-Atom Catalyst-Based Electrodes for CO2 Reduction M. Nur Hossain, Lei Zhang, Roberto Neagu, Xiaolin Li, Enoch Rassachack Electrochemical Energy Reviews    2024, 7 (1): 5-.   DOI: 10.1007/s41918-023-00193-7 Abstract （152）      PDF       Knowledge map    Save Electrochemical CO2 reduction technology could solve the CO2-induced climate warming by electrochemically converting atmospheric CO2 back into fuel, essentially recycling it and building a low carbon emission economy. However, the electrochemical CO2 reduction reaction (CO2RR) poses a significant challenge due to the highly stable and linear CO2 molecules, in addition to a proton-coupled multi-electron transfer process. Thus, highly active catalysts, placed on activity bolstering materials, and permeable electrodes are crucial for CO2RR. Single-atom catalysts (SACs) have recently garnered increasing interest in the electrocatalysis community due to their potentially high mass efficiency and cost benefits (every atom is an active center, resulting in nearly 100% utilization) and adjustable selectivity (higher uniformity of the active sites compared to nanoparticles). However, preserving the accessibility and activity of the SACs inside the electrode poses major materials development and electrode design challenges. A conventional layered structure SAC electrode typically consists of a gas diffusion layer (GDL), a microporous layer (MPL) and a SAC catalyst layer (SACCL), fabricated by using a powder bonding process. However, this process usually encounters issues such as delamination and instability of SACs due to the weak binder-catalyst-support interface. Conversely, the free-standing SAC electrode design has the potential to overcome these issues by eliminating the GDL, MPL, and need of a binder, in contrast to the powder bonding process. This work first reviews the latest developments in experimental and modeling studies of powdered SAC electrode by the traditional powder bonding process. Next, it examines the development towards the free-standing SAC electrode for high-performance electrochemical reduction of CO2. The synthesis-structure-fabrication-performance relationships of SAC-based materials and associated electrodes are analyzed. Furthermore, the article presents future challenges and perspectives for high-performance SAC electrodes for CO2RR. Related Articles | Metrics | Comments（0） Select Electrochemical Carbon Dioxide Reduction in Acidic Media Zhe Yao, Xiaomeng He, Rui Lin Electrochemical Energy Reviews    2024, 7 (1): 8-.   DOI: 10.1007/s41918-024-00210-3 Abstract （143）      PDF       Knowledge map    Save The electrochemical reduction of carbon dioxide (CO2RR) stands as an enticing approach for the production of essential chemicals and feedstocks, storing clean electric energy and mitigating greenhouse gas emissions. Recent years have witnessed remarkable breakthroughs in CO2RR, enhancing its performance and transitioning related research from laboratory settings toward industrial realization. However, the journey of CO2RR development is not devoid of challenges, including issues like mass transfer limitation, salt accumulation, and flooding phenomena. Remarkably, recent studies have unveiled a promising avenue by conducting CO2RR in an acidic environment, effectively circumventing these challenges and presenting novel opportunities. In this review, we embark on a reassessment of H-cells and flow cells, delving into their opportunities, challenges, strengths, and weaknesses. Additionally, we compile recent advancements in CO2RR under acidic conditions, elucidating the performance metrics and strategies embraced by pertinent research. Subsequently, we propose three pivotal concerns in acidic CO2RR: ① balancing the competition between CO2RR and hydrogen evolution reaction (HER), ② enhancing the selectivity, and ③ exploring industrial applications. And finally, we delve into the core factors influencing the performance of CO2RR in acid: local pH, cation effects, and catalyst design. Building upon these strategies, challenges, and insights, prospects are proposed for the future trajectory of CO2RR development. Related Articles | Metrics | Comments（0） Select Ion Exchange Membranes in Electrochemical CO2 Reduction Processes Faezeh Habibzadeh, Peter Mardle, Nana Zhao, Harry D. Riley, Danielle A. Salvatore, Curtis P. Berlinguette, Steven Holdcroft, Zhiqing Shi Electrochemical Energy Reviews    2023, 6 (3): 26-.   DOI: 10.1007/s41918-023-00183-9 Abstract （201）      PDF       Knowledge map    Save The low-temperature electrolysis of CO2 in membrane-based flow reactors is a promising technology for converting captured CO2 into valuable chemicals and fuels. In recent years, substantial improvements in reactor design have significantly improved the economic viability of this technology; thus, the field has experienced a rapid increase in research interest. Among the factors related to reactor design, the ion exchange membrane (IEM) plays a prominent role in the energetic efficiency of CO2 conversion into useful products. Reactors utilizing cation exchange, anion exchange and bipolar membranes have all been developed, each providing unique benefits and challenges that must be overcome before large-scale commercialization is feasible. Therefore, to direct advances in IEM technology specific to electrochemical CO2 reduction reactions (CO2RRs), this review serves to first provide polymer scientists with a general understanding of membrane-based CO2RR reactors and membrane-related shortcomings and to encourage systematic synthetic approaches to develop membranes that meet the specific requirements of CO2RRs. Second, this review provides researchers in the fields of electrocatalysis and CO2RRs with more detailed insight into the often-overlooked membrane roles and requirements; thus, new methodologies for membrane evaluation during CO2RR may be developed. By using CO2-to-CO/HCOO- methodologies as practical baseline systems, a clear conceptualization of the merits and challenges of different systems and reasonable objectives for future research and development are presented. Related Articles | Metrics | Comments（0） Select Catalyst Design for Electrolytic CO2 Reduction Toward Low-Carbon Fuels and Chemicals Yipeng Zang, Pengfei Wei, Hefei Li, Dunfeng Gao, Guoxiong Wang Electrochemical Energy Reviews    2022, 5 (S1): 29-.   DOI: 10.1007/s41918-022-00140-y Abstract （327）      PDF       Knowledge map    Save Electrocatalytic CO2 reduction reaction (CO2RR) is an attractive way to simultaneously convert CO2 into value-added fuels and chemicals as well as to store intermittent electricity derived from renewable energy. However, this process involves multiple proton and electron transfer steps and is kinetically sluggish, thus leading to low conversion efficiency from electrical energy to chemical energy. Therefore, there is an urgent need to develop highly efficient CO2RR catalysts with high activity, selectivity and stability. In this review, we firstly introduce the fundamentals of CO2RR and then discuss the synthesis, characterization, catalytic performance and reaction mechanism of various catalysts based on specific CO2RR products. The structure-performance relationships of some representative catalyst systems are highlighted, benefiting from advanced electrochemical in situ and operando spectroscopic characterizations. At the end, we illustrate existing challenges and emerging research directions, to design new generation of highly efficient catalysts and to advance both fundamental research and practical application of CO2RR to low-carbon fuels and chemicals. Related Articles | Metrics | Comments（0） Select Advances in Graphene-Supported Single-Atom Catalysts for Clean Energy Conversion Yunkun Dai, Fanrong Kong, Xuehan Tai, Yunlong Zhang, Bing Liu, Jiajun Cai, Xiaofei Gong, Yunfei Xia, Pan Guo, Bo Liu, Jian Zhang, Lin Li, Lei Zhao, Xulei Sui, Zhenbo Wang Electrochemical Energy Reviews    2022, 5 (S2): 22-.   DOI: 10.1007/s41918-022-00142-w Abstract （313）      PDF       Knowledge map    Save Recently, heterogeneous single-atom catalysts (SACs) have attracted enormous attention in electrochemical applications owing to their advantages of high metal utilization, well-defined active sites, tunable selectivity, and excellent activity. To avoid the aggregation of atomically dispersed metal sites, an appropriate support has to be adopted to reduce the surface free energy of catalysts. Graphene with a high surface area, outstanding conductivity, and unique electronic properties has generally been utilized as the substrate for SACs. Moreover, the correlations between metal-support interactions and the electrocatalytic performance at the atomic scale can be studied on graphene-supported single-atom catalyst (G-SAC) nanoplatforms. In this review, we start from an overview of the synthetic methods for G-SACs. Subsequently, several advanced and effective characterization techniques are discussed. Then, we present a comprehensive summary of recent progress in G-SACs for a variety of electrochemical applications. Finally, we present challenges for and an outlook on the development of G-SACs with outstanding catalytic activity, stability, and selectivity. Related Articles | Metrics | Comments（0） Select Recent Advances in Non-Precious Metal–Nitrogen–Carbon Single-Site Catalysts for CO2 Electroreduction Reaction to CO Yiqun Chen, Junru Zhang, Lijun Yang, Xizhang Wang, Qiang Wu, Zheng Hu Electrochemical Energy Reviews    2022, 5 (4): 11-.   DOI: 10.1007/s41918-022-00156-4 Abstract （2034）      PDF       Knowledge map    Save The carbon dioxide electroreduction reaction (CO2RR) to fuels and/or chemicals is an efficient prospective strategy to realize global carbon management using intermittent electric energy harvested from renewable sources. Highly efficient inexpensive electrocatalysts are required to achieve high energy and Faradaic efficiencies as well as fast conversion. Metal–nitrogen–carbon (M–N–C) single-site catalysts (SSCs) are highly competitive over precious metal catalysts in the CO2RR to CO due to their high performance, easy regulation and low cost. In the past six years, intensive studies of M–N–C SSCs for CO2RR to CO have been performed, and great progress has been achieved. This review focuses on the important topic of CO2RR to CO with M–N–C SSCs. We first introduce the reaction mechanism of the CO2RR to CO and the regulation of the electronic structure from a theoretical viewpoint. Then, the construction of M–N–C SSCs and the regulation of the electronic structure are demonstrated experimentally. The up-to-date electrocatalytic performance of M–N–C SSCs with different metal centers (Ni, Fe, Co and others) is summarized and compared systematically to highlight structure–performance correlations that were considered from both theoretical and experimental perspectives. Finally, the opportunities, challenges and future outlooks are summarized to deepen and widen research and applications in this promising field. Related Articles | Metrics | Comments（0） Select Copper-Based Catalysts for Electrochemical Carbon Dioxide Reduction to Multicarbon Products Fangfang Chang, Meiling Xiao, Ruifang Miao, Yongpeng Liu, Mengyun Ren, Zhichao Jia, Dandan Han, Yang Yuan, Zhengyu Bai, Lin Yang Electrochemical Energy Reviews    2022, 5 (3): 4-.   DOI: 10.1007/s41918-022-00139-5 Abstract （1808）      PDF       Knowledge map    Save Electrochemical conversion of carbon dioxide into fuel and chemicals with added value represents an appealing approach to reduce the greenhouse effect and realize a carbon-neutral cycle, which has great potential in mitigating global warming and effectively storing renewable energy. The electrochemical CO2 reduction reaction (CO2RR) usually involves multiproton coupling and multielectron transfer in aqueous electrolytes to form multicarbon products (C2+ products), but it competes with the hydrogen evolution reaction (HER), which results in intrinsically sluggish kinetics and a complex reaction mechanism and places higher requirements on the design of catalysts. In this review, the advantages of electrochemical CO2 reduction are briefly introduced, and then, different categories of Cu-based catalysts, including monometallic Cu catalysts, bimetallic catalysts, metal-organic frameworks (MOFs) along with MOF-derived catalysts and other catalysts, are summarized in terms of their synthesis method and conversion of CO2 to C2+ products in aqueous solution. The catalytic mechanisms of these catalysts are subsequently discussed for rational design of more efficient catalysts. In response to the mechanisms, several material strategies to enhance the catalytic behaviors are proposed, including surface facet engineering, interface engineering, utilization of strong metal-support interactions and surface modification. Based on the above strategies, challenges and prospects are proposed for the future development of CO2RR catalysts for industrial applications. Related Articles | Metrics | Comments（0） Select Electrolyzer and Catalysts Design from Carbon Dioxide to Carbon Monoxide Electrochemical Reduction Jingfu He, Yuanli Li, Aoxue Huang, Qinghua Liu, Changli Li Electrochemical Energy Reviews    2021, 4 (4): 680-717.   DOI: 10.1007/s41918-021-00100-y Abstract （849）      PDF       Knowledge map    Save Electrochemical CO2 reduction reaction (CO2RR) has attracted considerable attention in the recent decade for its critical role in the storage of renewable energy and fulfilling of the carbon cycle, and catalysts with varying morphology and modification strategies have been studied to improve the CO2RR activity and selectivity. However, most of the achievements are focused on preliminary reduction products such as CO and HCOOH. Development and research on electrochemical CO reduction reaction (CORR) are considered to be more promising to achieve multicarbon products and a better platform to understand the mechanism of C-C formation. In this review, we introduce the current achievements of CO2RR and emphasize the potential of CORR. We provide a summary of how electrolysis environment, electrode substrates, and cell design affect the performance of CORR catalysts in order to offer a guideline of standard operating conditions for CORR research. The composition-structure-activity relationships for CORR catalysts studied in H-cells and gas-phase flow cells are separately analyzed to give a comprehensive understanding of the development of catalyst design. Finally, the reaction mechanism, latest progress, major challenges and potential opportunities of CORR are also analyzed to provide a critical overview for further performance improvement of CORR.This work reviews the recent progress and potential of carbon monoxide reduction (CORR) research. A comprehensive summary of how electrolysis environment, electrode substrate, and cell design affect the performance of CORR catalysts is performed and the composition-structure-activity relationships for CORR catalysts are analyzed. Related Articles | Metrics | Comments（0） Select Silicon/Carbon Composite Anode Materials for Lithium-Ion Batteries Fei Dou, Liyi Shi, Guorong Chen, Dengsong Zhang Electrochemical Energy Reviews    2019, 2 (1): 149-198.   DOI: 10.1007/s41918-018-00028-w Abstract （1028）      PDF       Knowledge map    Save Silicon (Si) is a representative anode material for next-generation lithium-ion batteries due to properties such as a high theoretical capacity, suitable working voltage, and high natural abundance. However, due to inherently large volume expansions (~400%) during insertion/deinsertion processes as well as poor electrical conductivity and unstable solid electrolyte interfaces (SEI) flms, Si-based anodes possess serious stability problems, greatly hindering practical application. To resolve these issues, the modifcation of Si anodes with carbon (C) is a promising method which has been demonstrated to enhance electrical conductivity and material plasticity. In this review, recent researches into Si/C anodes are grouped into categories based on the structural dimension of Si materials, including nanoparticles, nanowires and nanotubes, nanosheets, and porous Si-based materials, and the structural and electrochemical performance of various Si/C composites based on carbon materials with varying structures will be discussed. In addition, the progress and limitations of the design of existing Si/C composite anodes are summarized, and future research perspectives in this feld are presented. Full-text：https://link.springer.com/article/10.1007/s41918-018-00028-w Related Articles | Metrics | Comments（0） Select Carbon-Encapsulated Electrocatalysts for the Hydrogen Evolution Reaction Jiajia Lu, Shibin Yin, Pei Kang Shen Electrochemical Energy Reviews    2019, 2 (1): 105-127.   DOI: 10.1007/s41918-018-0025-9 Abstract （726）      PDF       Knowledge map    Save Water electrolysis is a promising approach for large-scale and sustainable hydrogen production; however, its kinetics is slow and requires precious metal electrocatalysts to efciently operate. Therefore, great eforts are being undertaken to design and prepare low-cost and highly efcient electrocatalysts to boost the hydrogen evolution reaction (HER). This is because traditional transition-metal electrocatalysts and corresponding hybrids with nonmetal atoms rely mainly on the interaction of metal-H bonds for the HER, which inevitably sufers from corrosion in extreme acidic and alkaline solutions. And as a result of all this efort, novel nanostructured electrocatalysts, such as carbon-encapsulated precious metals and non-precious metals including single metals or their alloys, transition-metal carbides, phosphides, oxides, sulfdes, and selenides have all been recently reported to exhibit good catalytic activities and stabilities for hydrogen evolution. Here, the catalytic activity is thought to originate from the electron penetration efect of the inner metals to the surface carbon, which can alter the Gibbs free energy of hydrogen adsorption on the surface of materials. In this review, recent progresses of carbon-encapsulated materials for the HER are summarized, with a focus on the unique efects of carbon shells. In addition, perspectives on the future development of carbon-coated electrocatalysts for the HER are provided. Full-text：https://link.springer.com/article/10.1007/s41918-018-0025-9 Related Articles | Metrics | Comments（0）