Won Il Kim, Jong Chan Shin, Min Ju Kim, Gun Jang, Minjae Lee, Ho Seok Park
{"title":"Ionic Structured Redox-Mediating Polymeric Sulfurs for Lithium–Sulfur Batteries","authors":"Won Il Kim, Jong Chan Shin, Min Ju Kim, Gun Jang, Minjae Lee, Ho Seok Park","doi":"10.1021/acsenergylett.5c00808","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00808","url":null,"abstract":"Polymeric sulfur demonstrates immense capabilities as a promising active material for lithium–sulfur batteries (LSBs) owing to their ability to capture lithium polysulfides (LiPS) through the formation of covalent bonds. Herein, we demonstrate an ionic structured polymeric sulfur (IP-S) as a redox mediating matrix, which provides structural stability, an ionic conductive pathway, and a uniform distribution of active materials within the electrode. In particular, the cationic structure of IP-S was attributed to the facilitated LiPS conversion kinetics with the high utilization of sulfur. Consequently, the IP-S electrode delivered the high specific capacity of 1398.8 mAh g<sub>sulfur</sub><sup>–1</sup> with a low-capacity fading rate of 0.071% over 400 cycles. Moreover, with a high sulfur loading (6.87 mg<sub>sulfur</sub> cm<sup>–2</sup>), the IP-S electrode achieved a high initial capacity of 7.23 mAh cm<sup>–2</sup>. Therefore, this work provides the rational design of ionic structured polymeric sulfur for high performance LSBs as well as the correlation between the ionic structure and the electrochemical property.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"108 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853253","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Energy Letters Pub Date : 2025-04-21DOI: 10.1021/acsenergylett.5c0080810.1021/acsenergylett.5c00808
Won Il Kim, Jong Chan Shin, Min Ju Kim, Gun Jang, Minjae Lee* and Ho Seok Park*,
{"title":"Ionic Structured Redox-Mediating Polymeric Sulfurs for Lithium–Sulfur Batteries","authors":"Won Il Kim, Jong Chan Shin, Min Ju Kim, Gun Jang, Minjae Lee* and Ho Seok Park*, ","doi":"10.1021/acsenergylett.5c0080810.1021/acsenergylett.5c00808","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00808https://doi.org/10.1021/acsenergylett.5c00808","url":null,"abstract":"<p >Polymeric sulfur demonstrates immense capabilities as a promising active material for lithium–sulfur batteries (LSBs) owing to their ability to capture lithium polysulfides (LiPS) through the formation of covalent bonds. Herein, we demonstrate an ionic structured polymeric sulfur (IP-S) as a redox mediating matrix, which provides structural stability, an ionic conductive pathway, and a uniform distribution of active materials within the electrode. In particular, the cationic structure of IP-S was attributed to the facilitated LiPS conversion kinetics with the high utilization of sulfur. Consequently, the IP-S electrode delivered the high specific capacity of 1398.8 mAh g<sub>sulfur</sub><sup>–1</sup> with a low-capacity fading rate of 0.071% over 400 cycles. Moreover, with a high sulfur loading (6.87 mg<sub>sulfur</sub> cm<sup>–2</sup>), the IP-S electrode achieved a high initial capacity of 7.23 mAh cm<sup>–2</sup>. Therefore, this work provides the rational design of ionic structured polymeric sulfur for high performance LSBs as well as the correlation between the ionic structure and the electrochemical property.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 5","pages":"2410–2418 2410–2418"},"PeriodicalIF":19.3,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921236","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xuesong Zhao, Mengdie Yan, Jialu Bi, Kangren Kong, Liqi Liu, Liya Chen, Yihong Jin, Mengqi Zhou, Chaojiang Niu, Zhaoming Liu, Ruikang Tang, Liguang Wang, Jun Lu, Huilin Pan
{"title":"Unveiling Electrode–Electrolyte Interface Dynamics for Aqueous Zn Batteries","authors":"Xuesong Zhao, Mengdie Yan, Jialu Bi, Kangren Kong, Liqi Liu, Liya Chen, Yihong Jin, Mengqi Zhou, Chaojiang Niu, Zhaoming Liu, Ruikang Tang, Liguang Wang, Jun Lu, Huilin Pan","doi":"10.1021/acsenergylett.5c00445","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00445","url":null,"abstract":"Aqueous Zn batteries are a promising solution for energy storage due to their safety and cost-effectiveness. However, conventional Zn anodes face challenges such as slow interfacial kinetics and structural collapse at high rates and Zn utilization. Here, we design an integrated Zn anode with an embedded heterophase boundary framework (HPF-Zn) that could regulate the chemical environment and charge transport kinetics for uniform, fast Zn deposition. Well-designed in situ Raman spectra clearly visualize the dynamic interface evolution under various conditions, confirming rapid Zn<sup>2+</sup> replenishment at the interface for HPF-Zn anode. Consequently, the HPF-Zn anode achieves 60× the cycle life of conventional Zn anodes with nearly 100% Zn utilization. Zn||V<sub>2</sub>O<sub>5</sub> full cells exhibit excellent cycling stability, retaining 80% capacity over 5500 cycles (N/P = 5.6) and 2500 cycles (N/P = 3.2). Moreover, Ah-level pouch cells demonstrate superior durability. This work advances our understanding of dynamic interfaces and highlights a strategy for stabilizing electrode–electrolyte interfaces via heterophase boundary design.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"30 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Energy Letters Pub Date : 2025-04-20DOI: 10.1021/acsenergylett.5c0044510.1021/acsenergylett.5c00445
Xuesong Zhao, Mengdie Yan, Jialu Bi, Kangren Kong, Liqi Liu, Liya Chen, Yihong Jin, Mengqi Zhou, Chaojiang Niu, Zhaoming Liu, Ruikang Tang, Liguang Wang*, Jun Lu* and Huilin Pan*,
{"title":"Unveiling Electrode–Electrolyte Interface Dynamics for Aqueous Zn Batteries","authors":"Xuesong Zhao, Mengdie Yan, Jialu Bi, Kangren Kong, Liqi Liu, Liya Chen, Yihong Jin, Mengqi Zhou, Chaojiang Niu, Zhaoming Liu, Ruikang Tang, Liguang Wang*, Jun Lu* and Huilin Pan*, ","doi":"10.1021/acsenergylett.5c0044510.1021/acsenergylett.5c00445","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00445https://doi.org/10.1021/acsenergylett.5c00445","url":null,"abstract":"<p >Aqueous Zn batteries are a promising solution for energy storage due to their safety and cost-effectiveness. However, conventional Zn anodes face challenges such as slow interfacial kinetics and structural collapse at high rates and Zn utilization. Here, we design an integrated Zn anode with an embedded heterophase boundary framework (HPF-Zn) that could regulate the chemical environment and charge transport kinetics for uniform, fast Zn deposition. Well-designed in situ Raman spectra clearly visualize the dynamic interface evolution under various conditions, confirming rapid Zn<sup>2+</sup> replenishment at the interface for HPF-Zn anode. Consequently, the HPF-Zn anode achieves 60× the cycle life of conventional Zn anodes with nearly 100% Zn utilization. Zn||V<sub>2</sub>O<sub>5</sub> full cells exhibit excellent cycling stability, retaining 80% capacity over 5500 cycles (N/P = 5.6) and 2500 cycles (N/P = 3.2). Moreover, Ah-level pouch cells demonstrate superior durability. This work advances our understanding of dynamic interfaces and highlights a strategy for stabilizing electrode–electrolyte interfaces via heterophase boundary design.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 5","pages":"2400–2409 2400–2409"},"PeriodicalIF":19.3,"publicationDate":"2025-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921466","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Brian Seger, Georg Kastlunger, Alexander Bagger, Soren B. Scott
{"title":"A Perspective on the Reaction Mechanisms of CO2 Electrolysis","authors":"Brian Seger, Georg Kastlunger, Alexander Bagger, Soren B. Scott","doi":"10.1021/acsenergylett.4c03599","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03599","url":null,"abstract":"In this work, we analyze the current state of mechanistic understanding in CO<sub>2</sub> electrolysis and give our best analysis of what we believe is the most dominant mechanism for the predominant products in CO<sub>2</sub> electrolysis. We draw on both computational and experimental literature to develop conclusions for C1 and C2 products. From this, we develop a set of self-consistent mechanistic rules. As the volume of literature on the mechanism toward C3 products is substantially smaller than on C1 and C2 products, these rules help us in evaluating mechanistic pathways toward C3 products. While these mechanistic pathways are speculative, it does give us a point of reference that can be modified in the future based on further developments in the field.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"3 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846531","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jong-Ho Choi, Tanya Agarwal, Heemin Park, Jiyoon Jung, Ain Uddin, Su Min Ahn, Jeffrey Michael Klein, Albert S. Lee, Michelle Lehmann, Cy Fujimoto, Eun Joo Park, Tomonori Saito, Rod L. Borup, Yu Seung Kim
{"title":"Performance-Limiting Factors of Hydrocarbon Ionomeric Binders for Fuel Cells and Electrolyzers","authors":"Jong-Ho Choi, Tanya Agarwal, Heemin Park, Jiyoon Jung, Ain Uddin, Su Min Ahn, Jeffrey Michael Klein, Albert S. Lee, Michelle Lehmann, Cy Fujimoto, Eun Joo Park, Tomonori Saito, Rod L. Borup, Yu Seung Kim","doi":"10.1021/acsenergylett.5c00487","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00487","url":null,"abstract":"The move toward nonfluorinated hydrocarbon ionomers for fuel cells and electrolyzers is driven by potential restrictions on polyfluoroalkyl substances such as Nafion. This study examines the key limitations of hydrocarbon ionomers through half- and single-cell experiments with model hydrocarbon ionomers. Half-cell tests reveal three major performance barriers: undesirable adsorption, electrochemical oxidation, and low gas permeability. Competitive sulfate adsorption helps counteract ionomer adsorption and oxidation. These findings align with single-cell performance data, which further reveal additional oxygen mass transport limitations likely caused by localized electrode flooding. Together, these findings offer valuable insights to guide the development of high-performance, fluorine-free hydrocarbon ionomers for next-generation fuel cells and electrolyzers.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"17 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846532","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Energy Letters Pub Date : 2025-04-18DOI: 10.1021/acsenergylett.4c0359910.1021/acsenergylett.4c03599
Brian Seger*, Georg Kastlunger, Alexander Bagger and Soren B. Scott,
{"title":"A Perspective on the Reaction Mechanisms of CO2 Electrolysis","authors":"Brian Seger*, Georg Kastlunger, Alexander Bagger and Soren B. Scott, ","doi":"10.1021/acsenergylett.4c0359910.1021/acsenergylett.4c03599","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03599https://doi.org/10.1021/acsenergylett.4c03599","url":null,"abstract":"<p >In this work, we analyze the current state of mechanistic understanding in CO<sub>2</sub> electrolysis and give our best analysis of what we believe is the most dominant mechanism for the predominant products in CO<sub>2</sub> electrolysis. We draw on both computational and experimental literature to develop conclusions for C1 and C2 products. From this, we develop a set of self-consistent mechanistic rules. As the volume of literature on the mechanism toward C3 products is substantially smaller than on C1 and C2 products, these rules help us in evaluating mechanistic pathways toward C3 products. While these mechanistic pathways are speculative, it does give us a point of reference that can be modified in the future based on further developments in the field.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 5","pages":"2212–2227 2212–2227"},"PeriodicalIF":19.3,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921391","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Energy Letters Pub Date : 2025-04-18DOI: 10.1021/acsenergylett.5c0048710.1021/acsenergylett.5c00487
Jong-Ho Choi, Tanya Agarwal, Heemin Park, Jiyoon Jung, Ain Uddin, Su Min Ahn, Jeffrey Michael Klein, Albert S. Lee, Michelle Lehmann, Cy Fujimoto, Eun Joo Park, Tomonori Saito, Rod L. Borup and Yu Seung Kim*,
{"title":"Performance-Limiting Factors of Hydrocarbon Ionomeric Binders for Fuel Cells and Electrolyzers","authors":"Jong-Ho Choi, Tanya Agarwal, Heemin Park, Jiyoon Jung, Ain Uddin, Su Min Ahn, Jeffrey Michael Klein, Albert S. Lee, Michelle Lehmann, Cy Fujimoto, Eun Joo Park, Tomonori Saito, Rod L. Borup and Yu Seung Kim*, ","doi":"10.1021/acsenergylett.5c0048710.1021/acsenergylett.5c00487","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00487https://doi.org/10.1021/acsenergylett.5c00487","url":null,"abstract":"<p >The move toward nonfluorinated hydrocarbon ionomers for fuel cells and electrolyzers is driven by potential restrictions on polyfluoroalkyl substances such as Nafion. This study examines the key limitations of hydrocarbon ionomers through half- and single-cell experiments with model hydrocarbon ionomers. Half-cell tests reveal three major performance barriers: undesirable adsorption, electrochemical oxidation, and low gas permeability. Competitive sulfate adsorption helps counteract ionomer adsorption and oxidation. These findings align with single-cell performance data, which further reveal additional oxygen mass transport limitations likely caused by localized electrode flooding. Together, these findings offer valuable insights to guide the development of high-performance, fluorine-free hydrocarbon ionomers for next-generation fuel cells and electrolyzers.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 5","pages":"2392–2399 2392–2399"},"PeriodicalIF":19.3,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921462","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Energy Letters Pub Date : 2025-04-17DOI: 10.1021/acsenergylett.5c0077510.1021/acsenergylett.5c00775
Yuxin Zhao*,
{"title":"Urban Energy Reconfiguration: China’s Hydrogen-Blended Gas Networks as a Catalyst for Global Carbon-Neutral Cities","authors":"Yuxin Zhao*, ","doi":"10.1021/acsenergylett.5c0077510.1021/acsenergylett.5c00775","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00775https://doi.org/10.1021/acsenergylett.5c00775","url":null,"abstract":"","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 5","pages":"2372–2376 2372–2376"},"PeriodicalIF":19.3,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921453","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Energy Letters Pub Date : 2025-04-17DOI: 10.1021/acsenergylett.5c0051710.1021/acsenergylett.5c00517
Jiwei Wang, and , Hongli Zhu*,
{"title":"Sulfide-Based Anode-Free Solid-State Batteries: Key Challenges and Emerging Solutions","authors":"Jiwei Wang, and , Hongli Zhu*, ","doi":"10.1021/acsenergylett.5c0051710.1021/acsenergylett.5c00517","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00517https://doi.org/10.1021/acsenergylett.5c00517","url":null,"abstract":"<p >Sulfide-based anode-free solid-state batteries (AFSSBs) have emerged as a transformative technology for next-generation energy storage, offering compelling advantages in energy density, safety, and manufacturing scalability. However, these batteries face significant challenges, particularly rapid capacity degradation that currently limits their practical implementation. This comprehensive review critically examines three fundamental issues affecting AFSSBs: nonuniform lithium nucleation on bare current collectors, unstable interfaces between plated lithium and sulfide electrolytes, and formation of interfacial voids during cycling. We systematically evaluate recent strategic advances in addressing these challenges, including metal seed coatings, conversion reaction-based compounds, and carbon-based interlayers. The review also analyzes the crucial role of advanced characterization techniques, from cryo-FIB-SEM to operando methods, in understanding failure mechanisms and validating improvement strategies. Finally, we present a forward-looking perspective on research directions necessary for commercialization. This work provides a thorough framework for understanding and advancing sulfide-based AFSSBs toward practical applications in next-generation energy storage systems.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 5","pages":"2377–2391 2377–2391"},"PeriodicalIF":19.3,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenergylett.5c00517","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921454","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}