Pub Date : 2024-07-23DOI: 10.20517/energymater.2024.29
Ming Li, Ruzi Mo, Anting Ding, Kai Zhang, Fan Guo, Chengliang Xiao
The widespread use of lithium-ion batteries (LIBs) in recent years has led to a marked increase in the quantity of spent batteries, resulting in critical global technical challenges in terms of resource scarcity and environmental impact. Therefore, efficient and eco-friendly recycling methods for these batteries are needed. The recycling methods for spent LIBs include hydrometallurgy, pyrometallurgy, solid-phase regeneration, and electrochemical methods. Compared to other recycling methods, electrochemical methods offer high ion selectivity and environmental friendliness. Assembling research on the recycling and reutilization of spent LIBs, with a focus on the various electrochemical techniques that can enhance these processes, is essential. A thorough analysis of the characteristics and evolution of these methods remains crucial to advancing the field of electrochemical technology in battery recycling. This review first discussed the necessity of recycling spent LIBs from multiple perspectives and briefly introduced the main pyrometallurgical and hydrometallurgical recycling technologies, analyzing their advantages and disadvantages. Moreover, we comprehensively summarized the current applications of electrochemical technology in the recycling of spent LIBs, including pretreatment, leaching, element separation, and regeneration. Then, we analyzed the characteristics and advantages of different electrochemical techniques in the LIB recycling process and discussed the obstacles encountered in the application of electrochemical technology and their solutions. Finally, a comparison between electrochemical technology and traditional recycling processes was provided, highlighting the potential advantages of electrochemical technology in reducing recycling costs and minimizing waste emissions.
{"title":"Electrochemical technology to drive spent lithium-ion batteries (LIBs) recycling: recent progress, and prospects","authors":"Ming Li, Ruzi Mo, Anting Ding, Kai Zhang, Fan Guo, Chengliang Xiao","doi":"10.20517/energymater.2024.29","DOIUrl":"https://doi.org/10.20517/energymater.2024.29","url":null,"abstract":"The widespread use of lithium-ion batteries (LIBs) in recent years has led to a marked increase in the quantity of spent batteries, resulting in critical global technical challenges in terms of resource scarcity and environmental impact. Therefore, efficient and eco-friendly recycling methods for these batteries are needed. The recycling methods for spent LIBs include hydrometallurgy, pyrometallurgy, solid-phase regeneration, and electrochemical methods. Compared to other recycling methods, electrochemical methods offer high ion selectivity and environmental friendliness. Assembling research on the recycling and reutilization of spent LIBs, with a focus on the various electrochemical techniques that can enhance these processes, is essential. A thorough analysis of the characteristics and evolution of these methods remains crucial to advancing the field of electrochemical technology in battery recycling. This review first discussed the necessity of recycling spent LIBs from multiple perspectives and briefly introduced the main pyrometallurgical and hydrometallurgical recycling technologies, analyzing their advantages and disadvantages. Moreover, we comprehensively summarized the current applications of electrochemical technology in the recycling of spent LIBs, including pretreatment, leaching, element separation, and regeneration. Then, we analyzed the characteristics and advantages of different electrochemical techniques in the LIB recycling process and discussed the obstacles encountered in the application of electrochemical technology and their solutions. Finally, a comparison between electrochemical technology and traditional recycling processes was provided, highlighting the potential advantages of electrochemical technology in reducing recycling costs and minimizing waste emissions.","PeriodicalId":516209,"journal":{"name":"Energy Materials","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141814060","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The electrochemical reduction of carbon dioxide (CO2RR) offers a promising approach to address the dual challenges of energy scarcity and environmental degradation. This study presents a new, cost-effective, and scalable electrocatalyst: self-supporting carbon paper modified with porous conjugated polyimides. This innovative material facilitates efficient CO2 conversion in aqueous media, eliminating the need for a pyrolysis step. The electrocatalyst’s design utilizes a non-metallic organic polymer with a high density of nitrogen atoms, serving as active sites for catalysis. Its unique mesoporous microsphere structure comprises randomly stacked nanosheets that are generated in situ and aligned along the carbon fibers of carbon paper substrate. This architecture enhances both CO2 adsorption and ensures proper electron transportation, facilitated by the conjugated structure of the polymer. Additionally, the inherent hydrophobicity of conjugated polyimides contributes to its robust catalytic performance in selectively reducing CO2, yielding CO as the primary gaseous product with up to 88.7% Faradaic efficiency and 82.0 mmol g-1 h-1 yield rate. Therefore, the proposed electrocatalyst provides a sustainable solution for electrochemical CO2RR catalyzed by non-metal organic materials, combining high efficiency with the advantages of a simple preparation process and the absence of costly materials or steps. This research contributes to the advancement of CO2RR technologies, potentially leading to more environmentally friendly and energy-efficient solutions.
电化学还原二氧化碳（CO2RR）为解决能源短缺和环境恶化的双重挑战提供了一种前景广阔的方法。本研究提出了一种新型、经济、可扩展的电催化剂：用多孔共轭聚酰亚胺修饰的自支撑碳纸。这种创新材料有助于在水介质中高效转化二氧化碳，无需热解步骤。这种电催化剂的设计采用了一种非金属有机聚合物，具有高密度的氮原子，可作为催化的活性位点。其独特的介孔微球结构由随机堆叠的纳米片组成，这些纳米片在原位生成，并沿着碳纸基底的碳纤维排列。这种结构既能增强二氧化碳吸附能力，又能在聚合物共轭结构的促进下确保适当的电子传输。此外，共轭聚酰亚胺固有的疏水性也有助于其在选择性还原 CO2 方面发挥强大的催化性能，以高达 88.7% 的法拉第效率和 82.0 mmol g-1 h-1 的产率生成 CO 作为主要气态产物。因此，所提出的电催化剂为非金属有机材料催化的电化学 CO2RR 提供了一种可持续的解决方案，兼具高效率和制备工艺简单、无需昂贵材料或步骤等优点。这项研究有助于推动 CO2RR 技术的发展，有可能带来更环保、更节能的解决方案。
{"title":"Conjugated polyimides modified self-supported carbon electrodes for electrochemical conversion of CO2 to CO","authors":"Daming Feng, Zuo Li, Huifang Guo, Xiaodong Sun, Peng Huang, Ying Sun, Hui Li, Tianyi Ma","doi":"10.20517/energymater.2024.35","DOIUrl":"https://doi.org/10.20517/energymater.2024.35","url":null,"abstract":"The electrochemical reduction of carbon dioxide (CO2RR) offers a promising approach to address the dual challenges of energy scarcity and environmental degradation. This study presents a new, cost-effective, and scalable electrocatalyst: self-supporting carbon paper modified with porous conjugated polyimides. This innovative material facilitates efficient CO2 conversion in aqueous media, eliminating the need for a pyrolysis step. The electrocatalyst’s design utilizes a non-metallic organic polymer with a high density of nitrogen atoms, serving as active sites for catalysis. Its unique mesoporous microsphere structure comprises randomly stacked nanosheets that are generated in situ and aligned along the carbon fibers of carbon paper substrate. This architecture enhances both CO2 adsorption and ensures proper electron transportation, facilitated by the conjugated structure of the polymer. Additionally, the inherent hydrophobicity of conjugated polyimides contributes to its robust catalytic performance in selectively reducing CO2, yielding CO as the primary gaseous product with up to 88.7% Faradaic efficiency and 82.0 mmol g-1 h-1 yield rate. Therefore, the proposed electrocatalyst provides a sustainable solution for electrochemical CO2RR catalyzed by non-metal organic materials, combining high efficiency with the advantages of a simple preparation process and the absence of costly materials or steps. This research contributes to the advancement of CO2RR technologies, potentially leading to more environmentally friendly and energy-efficient solutions.\u0000","PeriodicalId":516209,"journal":{"name":"Energy Materials","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141826228","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-12DOI: 10.20517/energymater.2024.06
A. Rehman, Sanum Saleem, Shahid Ali, S. M. Abbas, Minsu Choi, Wonchang Choi
Sodium-ion batteries (SIBs) are close to commercialization. Although alloying anodes have potential use in next-generation SIB anodes, their limitations of low capacities and colossal volume expansions must be resolved. Traditional approaches involving structural and compositional tunings have not been able to break these lofty barriers. This review is devoted to recent progress in research on alloy-based SIB anodes comprising Sn, Sb, P, Ge, and Si. The current level of understanding, challenges, modifications, optimizations employed up to date, and shortfalls faced by alloying anodes are also described. A detailed future outlook is proposed, focusing on advanced nanomaterial tailoring methods and component modifications in SIB fabrication. Utilizing the latest state-of-the-art characterization techniques, including ex-situ and operando characterization tools, can help us better understand the (de)sodiation mechanism and accompanying capacity fading pathways to pave the way for next-generation SIBs with alloying anode materials.
{"title":"Recent advances in alloying anode materials for sodium-ion batteries: material design and prospects","authors":"A. Rehman, Sanum Saleem, Shahid Ali, S. M. Abbas, Minsu Choi, Wonchang Choi","doi":"10.20517/energymater.2024.06","DOIUrl":"https://doi.org/10.20517/energymater.2024.06","url":null,"abstract":"Sodium-ion batteries (SIBs) are close to commercialization. Although alloying anodes have potential use in next-generation SIB anodes, their limitations of low capacities and colossal volume expansions must be resolved. Traditional approaches involving structural and compositional tunings have not been able to break these lofty barriers. This review is devoted to recent progress in research on alloy-based SIB anodes comprising Sn, Sb, P, Ge, and Si. The current level of understanding, challenges, modifications, optimizations employed up to date, and shortfalls faced by alloying anodes are also described. A detailed future outlook is proposed, focusing on advanced nanomaterial tailoring methods and component modifications in SIB fabrication. Utilizing the latest state-of-the-art characterization techniques, including ex-situ and operando characterization tools, can help us better understand the (de)sodiation mechanism and accompanying capacity fading pathways to pave the way for next-generation SIBs with alloying anode materials.","PeriodicalId":516209,"journal":{"name":"Energy Materials","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141654685","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-08DOI: 10.20517/energymater.2024.41
Cheng’ao Liu, Yanping Cui, Yao Zhou
Single-atom catalysts (SACs) have emerged as a focal point in energy catalytic conversion due to their remarkable atomic efficiency and catalytic performance. The challenge lies in efficiently anchoring active sites on a specific substrate to prevent agglomeration, maximizing their effectiveness. Substrate characteristics play a pivotal role in shaping the catalytic performance of SACs, influencing the dispersion and stability of single atoms. In recent years, amorphous materials have gained attention as substrates due to their unique surface structure and abundance of unsaturated coordination sites, offering an ideal platform for capturing and anchoring single atoms effectively, thus enhancing catalytic activity. To clarify the interaction between single atoms and amorphous substrates, this review outlines amorphization methods, the mechanism of single-atom anchoring and the characterization methods of amorphous SACs. Subsequently, it summarizes the physical properties and electrocatalytic mechanisms of amorphous materials. Then, interactions between single atoms and amorphous substrates are categorized and summarized. Finally, the paper consolidates the research progress of amorphous SACs and outlines future development prospects. By exploring the synergistic relationship between single atoms and amorphous substrates, this review aims to deepen the understanding of their interaction mechanisms, thereby propelling advancements in SACs for energy catalytic conversion.
{"title":"The recent progress of single-atom catalysts on amorphous substrates for electrocatalysis","authors":"Cheng’ao Liu, Yanping Cui, Yao Zhou","doi":"10.20517/energymater.2024.41","DOIUrl":"https://doi.org/10.20517/energymater.2024.41","url":null,"abstract":"Single-atom catalysts (SACs) have emerged as a focal point in energy catalytic conversion due to their remarkable atomic efficiency and catalytic performance. The challenge lies in efficiently anchoring active sites on a specific substrate to prevent agglomeration, maximizing their effectiveness. Substrate characteristics play a pivotal role in shaping the catalytic performance of SACs, influencing the dispersion and stability of single atoms. In recent years, amorphous materials have gained attention as substrates due to their unique surface structure and abundance of unsaturated coordination sites, offering an ideal platform for capturing and anchoring single atoms effectively, thus enhancing catalytic activity. To clarify the interaction between single atoms and amorphous substrates, this review outlines amorphization methods, the mechanism of single-atom anchoring and the characterization methods of amorphous SACs. Subsequently, it summarizes the physical properties and electrocatalytic mechanisms of amorphous materials. Then, interactions between single atoms and amorphous substrates are categorized and summarized. Finally, the paper consolidates the research progress of amorphous SACs and outlines future development prospects. By exploring the synergistic relationship between single atoms and amorphous substrates, this review aims to deepen the understanding of their interaction mechanisms, thereby propelling advancements in SACs for energy catalytic conversion.","PeriodicalId":516209,"journal":{"name":"Energy Materials","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141668593","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Potassium-ion batteries (PIBs) represent a promising battery technology for energy storage applications. Nevertheless, the progress of PIBs is still hindered by the lack of electrode materials that allow rapid and repeatable accommodation of the large K+ ions. Herein, a composite anode material containing interlayered-expanded MoS2 (55.6% larger) nanoroses in carbon nanonets (MoS2/C@CNs) is designed with the assistance of biomass bagasse, of which the dual carbon sources convert into interlayer and skeleton carbon, respectively. The unique structure facilitates electron/ion transport in the entire electrode and offers excellent structural stability, leading to much improved electrochemical performance compared to simple MoS2/C composite and pure MoS2. Furthermore, the role of electrolyte salts (potassium hexafluorophosphate and potassium bis(fluorosulfonyl)imide) and the electrolyte concentration on the interfacial properties in PIBs have been explored. The results indicate that the low-concentration potassium bis(fluorosulfonyl)imide electrolyte helps to produce optimized organic-inorganic solid electrolyte interface films, contributing to a capacity retention of 90% after 1,000 cycles at 2 A g-1.
{"title":"Interlayer expansion and conductive networking of MoS2 nanoroses mediated by bio-derived carbon for enhanced potassium-ion storage","authors":"Shuo Zhang, Zonggui Yin, Lili Wang, Mengyao Shu, Xin Liang, Sheng Liang, Lei Hu, Chonghai Deng, Kunhong Hu, Xiaobo Zhu","doi":"10.20517/energymater.2024.25","DOIUrl":"https://doi.org/10.20517/energymater.2024.25","url":null,"abstract":"Potassium-ion batteries (PIBs) represent a promising battery technology for energy storage applications. Nevertheless, the progress of PIBs is still hindered by the lack of electrode materials that allow rapid and repeatable accommodation of the large K+ ions. Herein, a composite anode material containing interlayered-expanded MoS2 (55.6% larger) nanoroses in carbon nanonets (MoS2/C@CNs) is designed with the assistance of biomass bagasse, of which the dual carbon sources convert into interlayer and skeleton carbon, respectively. The unique structure facilitates electron/ion transport in the entire electrode and offers excellent structural stability, leading to much improved electrochemical performance compared to simple MoS2/C composite and pure MoS2. Furthermore, the role of electrolyte salts (potassium hexafluorophosphate and potassium bis(fluorosulfonyl)imide) and the electrolyte concentration on the interfacial properties in PIBs have been explored. The results indicate that the low-concentration potassium bis(fluorosulfonyl)imide electrolyte helps to produce optimized organic-inorganic solid electrolyte interface films, contributing to a capacity retention of 90% after 1,000 cycles at 2 A g-1.","PeriodicalId":516209,"journal":{"name":"Energy Materials","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141685412","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-11DOI: 10.20517/energymater.2023.144
Borui Yang, Ting Li, Yu Pan, Liu Yang, Kun Li, Jiahao Chen, Zhongfu Yan, Anjun Hu, Jianping Long
The emergence of lithium metal batteries (LMBs) as a promising technology in energy storage devices is attributed to their high energy density. However, the inherent flammability and leakage of the internal liquid organic electrolyte pose serious safety risks when exposed to heat. In response to this challenge, gel polymer electrolytes (GPEs) have been developed to mitigate leakage and enhance nonflammability by incorporating flame-retardant groups, thereby improving the safety of LMBs. This review commences with a brief analysis of the thermal runaway mechanism specific to LMBs, emphasizing its distinctions from that of lithium-ion batteries. Following this, the various methods employed to assess the safety of LMBs are discussed, including flammability, thermal stability, and abuse assessment. The following section categorizes recent research on safe GPEs according to different flame retardancy levels providing a concise overview of each category. Finally, the review explores current advancements in developing safety-oriented GPEs and considers potential future research directions.
{"title":"Design strategy towards flame-retardant gel polymer electrolytes for safe lithium metal batteries","authors":"Borui Yang, Ting Li, Yu Pan, Liu Yang, Kun Li, Jiahao Chen, Zhongfu Yan, Anjun Hu, Jianping Long","doi":"10.20517/energymater.2023.144","DOIUrl":"https://doi.org/10.20517/energymater.2023.144","url":null,"abstract":"The emergence of lithium metal batteries (LMBs) as a promising technology in energy storage devices is attributed to their high energy density. However, the inherent flammability and leakage of the internal liquid organic electrolyte pose serious safety risks when exposed to heat. In response to this challenge, gel polymer electrolytes (GPEs) have been developed to mitigate leakage and enhance nonflammability by incorporating flame-retardant groups, thereby improving the safety of LMBs. This review commences with a brief analysis of the thermal runaway mechanism specific to LMBs, emphasizing its distinctions from that of lithium-ion batteries. Following this, the various methods employed to assess the safety of LMBs are discussed, including flammability, thermal stability, and abuse assessment. The following section categorizes recent research on safe GPEs according to different flame retardancy levels providing a concise overview of each category. Finally, the review explores current advancements in developing safety-oriented GPEs and considers potential future research directions.","PeriodicalId":516209,"journal":{"name":"Energy Materials","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141355407","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-07DOI: 10.20517/energymater.2024.26
Saivineeth Penukula, Favian Tippin, Muzhi Li, K. Khawaja, Feng Yan, Nicholas Rolston
Ion migration is one of the prime reasons for the rapid degradation of metal halide perovskite solar cells (PSCs), and we report on a method for quantifying mobile ion concentration (No) using a transient dark current measurement. We perform both ex-situ and in-situ measurements on PSCs and study the evolution of No in films and devices under a range of temperatures. We also study the effect of device architecture, top electrode chemistry, and metal halide perovskite composition and dimensionality on No. Two-dimensional perovskites are shown to reduce the ion concentration along with inert C electrodes that do not react with halides by ~99% while also improving mechanical reliability by ~250%. We believe this work can provide design guidelines for the development of stable PSCs through the lens of minimizing mobile ions and their evolution over time under operational conditions.
离子迁移是金属卤化物包光体太阳能电池（PSCs）快速降解的主要原因之一，我们报告了一种利用瞬态暗电流测量来量化移动离子浓度（No）的方法。我们对 PSC 进行了原位和原位测量，并研究了一系列温度条件下薄膜和器件中 No 的演变情况。我们还研究了器件结构、顶部电极化学以及金属卤化物包晶成分和尺寸对 No 的影响。研究表明，二维包晶与不与卤化物发生反应的惰性 C 电极一起可将离子浓度降低约 99%，同时还可将机械可靠性提高约 250%。我们相信，这项工作可以为开发稳定的 PSC 提供设计指南，即从最大限度地减少移动离子及其在运行条件下随时间演变的角度出发。
{"title":"Use of carbon electrodes to reduce mobile ion concentration and improve reliability of metal halide perovskite photovoltaics","authors":"Saivineeth Penukula, Favian Tippin, Muzhi Li, K. Khawaja, Feng Yan, Nicholas Rolston","doi":"10.20517/energymater.2024.26","DOIUrl":"https://doi.org/10.20517/energymater.2024.26","url":null,"abstract":"Ion migration is one of the prime reasons for the rapid degradation of metal halide perovskite solar cells (PSCs), and we report on a method for quantifying mobile ion concentration (No) using a transient dark current measurement. We perform both ex-situ and in-situ measurements on PSCs and study the evolution of No in films and devices under a range of temperatures. We also study the effect of device architecture, top electrode chemistry, and metal halide perovskite composition and dimensionality on No. Two-dimensional perovskites are shown to reduce the ion concentration along with inert C electrodes that do not react with halides by ~99% while also improving mechanical reliability by ~250%. We believe this work can provide design guidelines for the development of stable PSCs through the lens of minimizing mobile ions and their evolution over time under operational conditions.","PeriodicalId":516209,"journal":{"name":"Energy Materials","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141375358","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-06DOI: 10.20517/energymater.2023.109
Yitian Ma, Linqing Chang, Dawei Yi, Meng Liu, Peichun Wang, Shuliang Luo, Zhiyun Zhang, Yan Yuan, Hai Lu
One crucial problem hindering the commercial application of lithium-sulfur batteries with high theoretical specific energy is the ceaseless shuttle of soluble lithium polysulfides (LiPSs) between cathodes and anodes, which usually leads to rapid capacity fade and serious self-discharge issues. Herein, a unique bilayer coating strategy designed to modify the polypropylene separator was developed in this study, which consisted of a bottom zeolite (SSZ-13) layer serving as a LiPS movement barrier and a top ZnS layer used for accelerating redox processes of LiPSs. Benefiting from the synergetic effect, the bilayer-modified separator offers absolute block capability to LiPS diffusion, moreover, significant catalysis effect on sulfur species conversion, as well as outstanding lithium-ion (Li+) conductivity, excellent electrolyte wettability, and desirable mechanical properties. Consequently, the assembled lithium-sulfur cell with the SSZ-13/ZnS@polypropylene separator demonstrates excellent cycle stability and rate capability, showcasing a capacity decay rate of only 0.052% per cycle at 1 C over 500 cycles.
{"title":"Synergetic effect of block and catalysis on polysulfides by functionalized bilayer modification on the separator for lithium-sulfur batteries","authors":"Yitian Ma, Linqing Chang, Dawei Yi, Meng Liu, Peichun Wang, Shuliang Luo, Zhiyun Zhang, Yan Yuan, Hai Lu","doi":"10.20517/energymater.2023.109","DOIUrl":"https://doi.org/10.20517/energymater.2023.109","url":null,"abstract":"One crucial problem hindering the commercial application of lithium-sulfur batteries with high theoretical specific energy is the ceaseless shuttle of soluble lithium polysulfides (LiPSs) between cathodes and anodes, which usually leads to rapid capacity fade and serious self-discharge issues. Herein, a unique bilayer coating strategy designed to modify the polypropylene separator was developed in this study, which consisted of a bottom zeolite (SSZ-13) layer serving as a LiPS movement barrier and a top ZnS layer used for accelerating redox processes of LiPSs. Benefiting from the synergetic effect, the bilayer-modified separator offers absolute block capability to LiPS diffusion, moreover, significant catalysis effect on sulfur species conversion, as well as outstanding lithium-ion (Li+) conductivity, excellent electrolyte wettability, and desirable mechanical properties. Consequently, the assembled lithium-sulfur cell with the SSZ-13/ZnS@polypropylene separator demonstrates excellent cycle stability and rate capability, showcasing a capacity decay rate of only 0.052% per cycle at 1 C over 500 cycles.","PeriodicalId":516209,"journal":{"name":"Energy Materials","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141378237","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-03-22DOI: 10.20517/energymater.2023.89
Leiping Liao, Huanhuan Duan, Guohua Chen, Yuanfu Deng
The inevitable shuttling of lithium polysulfides (LiPSs) and poor redox kinetics restrict real-world applications of lithium-sulfur (Li-S) batteries, although they have been paid plentiful attention. Herein, a thin and multifunctional heterostructure (ZIF-L/MXene), consisting of leaf-like zeolitic imidazolate framework sheets (ZIF-L) and two-dimensional layered Ti3C2Tx MXene nanosheets, is developed for modification of polyolefin-based separators. A good combination of the merits of the ZIF-L and MXene can hinder the restacking of MXene nanosheets and achieve a large specific surface area, thus exposing plentiful active sites for adsorption and catalytic reaction of LiPSs. Taking these obviously synergistic effects, the ZIF-L/MXene heterostructure modified separators not only alleviate the shuttling of LiPSs but also promote their kinetics conversion. Furthermore, with an improved electrolyte affinity, the ZIF-L/MXene modified separators can accelerate the transport of Li+. Thus, the modified separator endows a Li-S cell with an admirable discharge capacity of 1371.7 mAh g-1 at 0.2 C and favorable cycling stability, with a slow capacity decay ratio of 0.075% per cycle during 500 cycles. Even under a sulfur loading of ~ 4.1 mg cm-2, the Li-S battery can achieve an excellent capacity of 990.6 mAh g-1 at 0.1 C and maintain an excellent cycling performance. The novel ZIF-L/MXene heterostructure modified separator in this work can provide an alternative strategy for designing thin and light separators for high-performance Li-S batteries, via the enhancement of redox kinetics and reduction of shuttling of the LiPSs.
{"title":"Active sites-rich zeolitic imidazolate framework/MXene heterostructure modified separator with improved Li+ transport for high-performance Li-S batteries","authors":"Leiping Liao, Huanhuan Duan, Guohua Chen, Yuanfu Deng","doi":"10.20517/energymater.2023.89","DOIUrl":"https://doi.org/10.20517/energymater.2023.89","url":null,"abstract":"The inevitable shuttling of lithium polysulfides (LiPSs) and poor redox kinetics restrict real-world applications of lithium-sulfur (Li-S) batteries, although they have been paid plentiful attention. Herein, a thin and multifunctional heterostructure (ZIF-L/MXene), consisting of leaf-like zeolitic imidazolate framework sheets (ZIF-L) and two-dimensional layered Ti3C2Tx MXene nanosheets, is developed for modification of polyolefin-based separators. A good combination of the merits of the ZIF-L and MXene can hinder the restacking of MXene nanosheets and achieve a large specific surface area, thus exposing plentiful active sites for adsorption and catalytic reaction of LiPSs. Taking these obviously synergistic effects, the ZIF-L/MXene heterostructure modified separators not only alleviate the shuttling of LiPSs but also promote their kinetics conversion. Furthermore, with an improved electrolyte affinity, the ZIF-L/MXene modified separators can accelerate the transport of Li+. Thus, the modified separator endows a Li-S cell with an admirable discharge capacity of 1371.7 mAh g-1 at 0.2 C and favorable cycling stability, with a slow capacity decay ratio of 0.075% per cycle during 500 cycles. Even under a sulfur loading of ~ 4.1 mg cm-2, the Li-S battery can achieve an excellent capacity of 990.6 mAh g-1 at 0.1 C and maintain an excellent cycling performance. The novel ZIF-L/MXene heterostructure modified separator in this work can provide an alternative strategy for designing thin and light separators for high-performance Li-S batteries, via the enhancement of redox kinetics and reduction of shuttling of the LiPSs.","PeriodicalId":516209,"journal":{"name":"Energy Materials","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140220273","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-03-20DOI: 10.20517/energymater.2023.92
Jules Moutet, Tarek H. El-Assaad, Ramandeep Kaur, David D. Mills, T. Gianetti
In recent years, non-aqueous fully organic Redox Flow Batteries (RFBs) have displayed potential in broadening the electrochemical window and enhancing energy density in RFBs by relying on redox-active organic molecules to provide improved sustainability in comparison to metal-based charge carriers. Of particular interest, systems that rely on a single bipolar redox molecule (BRM) for their operation, known as symmetrical organic RFBs, have gained momentum as the utilization of a BRM eliminates membrane crossover issues, thus extending the lifespan of electrical energy storage systems while reducing their cost. In this manuscript, we will present our contribution to this field through the design of tunable bipolar molecules within the helicene carbocation class. This particular type of BRM is synthetically very affordable and has proven to be highly modifiable and robust. Through the examination of 11 examples, we will demonstrate how an approach based on readily available electrochemical tools can be efficiently employed to generate and assess a library of compounds for future full flow RFB applications.
{"title":"Designing the next generation of symmetrical organic redox flow batteries using helical carbocations","authors":"Jules Moutet, Tarek H. El-Assaad, Ramandeep Kaur, David D. Mills, T. Gianetti","doi":"10.20517/energymater.2023.92","DOIUrl":"https://doi.org/10.20517/energymater.2023.92","url":null,"abstract":"In recent years, non-aqueous fully organic Redox Flow Batteries (RFBs) have displayed potential in broadening the electrochemical window and enhancing energy density in RFBs by relying on redox-active organic molecules to provide improved sustainability in comparison to metal-based charge carriers. Of particular interest, systems that rely on a single bipolar redox molecule (BRM) for their operation, known as symmetrical organic RFBs, have gained momentum as the utilization of a BRM eliminates membrane crossover issues, thus extending the lifespan of electrical energy storage systems while reducing their cost. In this manuscript, we will present our contribution to this field through the design of tunable bipolar molecules within the helicene carbocation class. This particular type of BRM is synthetically very affordable and has proven to be highly modifiable and robust. Through the examination of 11 examples, we will demonstrate how an approach based on readily available electrochemical tools can be efficiently employed to generate and assess a library of compounds for future full flow RFB applications.","PeriodicalId":516209,"journal":{"name":"Energy Materials","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140226403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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