Hao Liu, Zonglin Yi, Qian Sun, Ya-Feng Fan, Lijing Xie, Yan Zhao, Zhenbing Wang, Jiayao Cheng, Fangyuan Su, Cheng-Meng Chen
{"title":"Ionic Exchange Mechanism in Electrical Double Layer Induced by Stable Passivation Film Boosts High Voltage Performance in Supercapacitors","authors":"Hao Liu, Zonglin Yi, Qian Sun, Ya-Feng Fan, Lijing Xie, Yan Zhao, Zhenbing Wang, Jiayao Cheng, Fangyuan Su, Cheng-Meng Chen","doi":"10.1021/acsenergylett.4c02688","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02688","url":null,"abstract":"Constructing a stable passivation film at the negative electrode–electrolyte interface is an effective strategy for optimizing the high voltage stability of propylene carbonate-based electrochemical double-layer capacitors (EDLC). However, the role of passivation film composition in determining high voltage performance is still being established. Herein, the effect of passivation film composition on the energy storage mechanism and high voltage performance is investigate. The modified passivation film inhibits the specific adsorption of anions; thus, the energy storage mechanism is altered to ionic exchange from co-ion desorption. This mechanism inhibits solvents from entering the inner Helmholtz plane, thus effectively reducing solvent decomposition and inhibiting rapid thickening of the passivation film. As expected, the floating stabilization time of EDLC utilizing this electrolyte at 3.3 V increases to 2090 h, which is 4.6 times longer than that for those utilizing commercial electrolyte. This work provides a new perspective for the development of high voltage EDLC.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"3 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782895","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}
Jing Yu, Ivan Pinto-Huguet, Chao Yue Zhang, Yingtang Zhou, Yaolin Xu, Alen Vizintin, Juan-Jesús Velasco-Vélez, Xueqiang Qi, Xiaobo Pan, Gozde Oney, Annabel Olgo, Katharina Märker, Leonardo M. Da Silva, Yufeng Luo, Yan Lu, Chen Huang, Eneli Härk, Joe Fleming, Pascale Chenevier, Andreu Cabot, Yunfei Bai, Marc Botifoll, Ashley P. Black, Qi An, Tazdin Amietszajew, Jordi Arbiol
{"title":"Mechanistic Insights and Technical Challenges in Sulfur-Based Batteries: A Comprehensive In Situ/Operando Monitoring Toolbox","authors":"Jing Yu, Ivan Pinto-Huguet, Chao Yue Zhang, Yingtang Zhou, Yaolin Xu, Alen Vizintin, Juan-Jesús Velasco-Vélez, Xueqiang Qi, Xiaobo Pan, Gozde Oney, Annabel Olgo, Katharina Märker, Leonardo M. Da Silva, Yufeng Luo, Yan Lu, Chen Huang, Eneli Härk, Joe Fleming, Pascale Chenevier, Andreu Cabot, Yunfei Bai, Marc Botifoll, Ashley P. Black, Qi An, Tazdin Amietszajew, Jordi Arbiol","doi":"10.1021/acsenergylett.4c02703","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02703","url":null,"abstract":"Batteries based on sulfur cathodes offer a promising energy storage solution due to their potential for high performance, cost-effectiveness, and sustainability. However, commercial viability is challenged by issues such as polysulfide migration, volume changes, uneven phase nucleation, limited ion transport, and sluggish sulfur redox kinetics. Addressing these challenges requires insights into the structural, morphological, and chemical evolution of phases, the associated volume changes and internal stresses, and ion and polysulfide diffusion within the battery. Such insights can only be obtained through real-time reaction monitoring within the battery’s operational environment, supported by molecular dynamics simulations and advanced artificial intelligence-driven data analysis. This review provides an overview of <i>in situ/operando</i> techniques for real-time tracking of these processes in sulfur-based batteries and explores the integration of simulations with experimental data to provide a holistic understanding of the critical challenges, enabling advancements in their development and commercial adoption.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"82 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142763110","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 : 2024-12-04DOI: 10.1021/acsenergylett.4c0290110.1021/acsenergylett.4c02901
Deda Peng, Ruitao Sun, Jin Han*, Tenglong Zhao, Ruijie Tian, Anran Zhang, Youcai Zhang and Ya You*,
{"title":"A Low-Concentrated Electrolyte with a 3.5 V Electrochemical Stability Window, Made by Restructuring the H-Bond Network, for High-Energy and Long-Life Aqueous Sodium-Ion Batteries","authors":"Deda Peng, Ruitao Sun, Jin Han*, Tenglong Zhao, Ruijie Tian, Anran Zhang, Youcai Zhang and Ya You*, ","doi":"10.1021/acsenergylett.4c0290110.1021/acsenergylett.4c02901","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02901https://doi.org/10.1021/acsenergylett.4c02901","url":null,"abstract":"<p >The narrow electrochemical stability window (ESW) of electrolytes is primarily responsible for the low energy density and poor cycle life of aqueous sodium-ion batteries (ASIBs). Although water-in-salt electrolytes can effectively widen the ESW, their high salt concentration leads to high costs. In this work, we found that weak-polar solvents have more advantages in broadening the ESW than strong-polar solvents. Taking 1,3,6-hexanetricarbonitrile as an example, it evidently enhances the stability of water by weakening the hydrogen bond network. Consequently, it broadens the ESW to 3.5 V at a relatively low concentration and enables Na<sub>2</sub>FeFe(CN)<sub>6</sub>||NaTi<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> full cells with a capacity retention of 70% after 10 000 cycles and an energy density of 71 Wh kg<sup>–1</sup>, based on the active materials’ mass of both electrodes. This work offers new prospects for the development of high-energy and long-life aqueous sodium-ion batteries for large-scale energy storage.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"9 12","pages":"6215–6224 6215–6224"},"PeriodicalIF":19.3,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850426","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 : 2024-12-04DOI: 10.1021/acsenergylett.4c0270310.1021/acsenergylett.4c02703
Jing Yu, Ivan Pinto-Huguet, Chao Yue Zhang, Yingtang Zhou, Yaolin Xu, Alen Vizintin, Juan-Jesús Velasco-Vélez, Xueqiang Qi, Xiaobo Pan, Gozde Oney, Annabel Olgo, Katharina Märker, Leonardo M. Da Silva, Yufeng Luo, Yan Lu, Chen Huang, Eneli Härk, Joe Fleming, Pascale Chenevier, Andreu Cabot*, Yunfei Bai, Marc Botifoll, Ashley P. Black, Qi An, Tazdin Amietszajew and Jordi Arbiol*,
{"title":"Mechanistic Insights and Technical Challenges in Sulfur-Based Batteries: A Comprehensive In Situ/Operando Monitoring Toolbox","authors":"Jing Yu, Ivan Pinto-Huguet, Chao Yue Zhang, Yingtang Zhou, Yaolin Xu, Alen Vizintin, Juan-Jesús Velasco-Vélez, Xueqiang Qi, Xiaobo Pan, Gozde Oney, Annabel Olgo, Katharina Märker, Leonardo M. Da Silva, Yufeng Luo, Yan Lu, Chen Huang, Eneli Härk, Joe Fleming, Pascale Chenevier, Andreu Cabot*, Yunfei Bai, Marc Botifoll, Ashley P. Black, Qi An, Tazdin Amietszajew and Jordi Arbiol*, ","doi":"10.1021/acsenergylett.4c0270310.1021/acsenergylett.4c02703","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02703https://doi.org/10.1021/acsenergylett.4c02703","url":null,"abstract":"<p >Batteries based on sulfur cathodes offer a promising energy storage solution due to their potential for high performance, cost-effectiveness, and sustainability. However, commercial viability is challenged by issues such as polysulfide migration, volume changes, uneven phase nucleation, limited ion transport, and sluggish sulfur redox kinetics. Addressing these challenges requires insights into the structural, morphological, and chemical evolution of phases, the associated volume changes and internal stresses, and ion and polysulfide diffusion within the battery. Such insights can only be obtained through real-time reaction monitoring within the battery’s operational environment, supported by molecular dynamics simulations and advanced artificial intelligence-driven data analysis. This review provides an overview of <i>in situ/operando</i> techniques for real-time tracking of these processes in sulfur-based batteries and explores the integration of simulations with experimental data to provide a holistic understanding of the critical challenges, enabling advancements in their development and commercial adoption.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"9 12","pages":"6178–6214 6178–6214"},"PeriodicalIF":19.3,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenergylett.4c02703","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842339","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}
Jehad Abed, Ivan Grigioni, Talha Kose, Wajdi Alnoush, Sungjin Park, Annalisa Polo, Byoung-Hoon Lee, David Sinton, Drew Higgins, Edward H. Sargent
{"title":"Zero-Gap Electrolyzers Accelerate Reconstruction of Cu2O-Derived Catalysts under CO2 Reduction","authors":"Jehad Abed, Ivan Grigioni, Talha Kose, Wajdi Alnoush, Sungjin Park, Annalisa Polo, Byoung-Hoon Lee, David Sinton, Drew Higgins, Edward H. Sargent","doi":"10.1021/acsenergylett.4c02634","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02634","url":null,"abstract":"To scale carbon dioxide reduction (CO<sub>2</sub>R), establishing a structure–property–performance relationship of the catalyst under the reaction conditions is a priority. Particularly in membrane electrode assembly (MEA) electrolyzers, knowledge about the valence state and coordination environment of the catalyst is of value yet limited. We developed an MEA electrolyzer that utilizes X-ray absorption spectroscopy to investigate the structural evolution of Cu<sub>2</sub>O-derived catalysts under CO<sub>2</sub>R and compare the same catalysts in a flow cell. Additionally, we study the influence of CO reduction and incorporating Ag on the reconstruction of the catalyst. We find that the strong reduction environment in the MEA and feeding CO leads to reconstruction of Cu<sub>2</sub>O particles, favoring higher coordination and lower oxidation states, which coincides with a shift in the reaction selectivity from C<sub>2+</sub> to hydrogen. Conversely, incorporating small amounts of Ag in the catalyst restricts the reconstruction. These findings advocate for <i>in situ</i> studies in zero-gap electrolyzers.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"79 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142777127","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 : 2024-12-04DOI: 10.1021/acsenergylett.4c0263410.1021/acsenergylett.4c02634
Jehad Abed, Ivan Grigioni, Talha Kose, Wajdi Alnoush, Sungjin Park, Annalisa Polo, Byoung-Hoon Lee, David Sinton, Drew Higgins* and Edward H. Sargent*,
{"title":"Zero-Gap Electrolyzers Accelerate Reconstruction of Cu2O-Derived Catalysts under CO2 Reduction","authors":"Jehad Abed, Ivan Grigioni, Talha Kose, Wajdi Alnoush, Sungjin Park, Annalisa Polo, Byoung-Hoon Lee, David Sinton, Drew Higgins* and Edward H. Sargent*, ","doi":"10.1021/acsenergylett.4c0263410.1021/acsenergylett.4c02634","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02634https://doi.org/10.1021/acsenergylett.4c02634","url":null,"abstract":"<p >To scale carbon dioxide reduction (CO<sub>2</sub>R), establishing a structure–property–performance relationship of the catalyst under the reaction conditions is a priority. Particularly in membrane electrode assembly (MEA) electrolyzers, knowledge about the valence state and coordination environment of the catalyst is of value yet limited. We developed an MEA electrolyzer that utilizes X-ray absorption spectroscopy to investigate the structural evolution of Cu<sub>2</sub>O-derived catalysts under CO<sub>2</sub>R and compare the same catalysts in a flow cell. Additionally, we study the influence of CO reduction and incorporating Ag on the reconstruction of the catalyst. We find that the strong reduction environment in the MEA and feeding CO leads to reconstruction of Cu<sub>2</sub>O particles, favoring higher coordination and lower oxidation states, which coincides with a shift in the reaction selectivity from C<sub>2+</sub> to hydrogen. Conversely, incorporating small amounts of Ag in the catalyst restricts the reconstruction. These findings advocate for <i>in situ</i> studies in zero-gap electrolyzers.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"9 12","pages":"6225–6232 6225–6232"},"PeriodicalIF":19.3,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842668","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 : 2024-12-04DOI: 10.1021/acsenergylett.4c0287410.1021/acsenergylett.4c02874
Sabin Neupane, Deng-Bing Li*, Manoj Kumar Jamarkattel, Abasi Abudulimu, Chun-Sheng Jiang, Sandip S. Bista, Alisha Adhikari, Sanjeeb Budhathoki, Hamim Sharif, Kiran Lamichhane, Tyler Brau, Adam B. Phillips, Ambalanath Shan, Randall J. Ellingson, Michael J. Heben and Yanfa Yan*,
{"title":"Evaporated CdSe for Efficient Polycrystalline CdSeTe Thin-Film Solar Cells","authors":"Sabin Neupane, Deng-Bing Li*, Manoj Kumar Jamarkattel, Abasi Abudulimu, Chun-Sheng Jiang, Sandip S. Bista, Alisha Adhikari, Sanjeeb Budhathoki, Hamim Sharif, Kiran Lamichhane, Tyler Brau, Adam B. Phillips, Ambalanath Shan, Randall J. Ellingson, Michael J. Heben and Yanfa Yan*, ","doi":"10.1021/acsenergylett.4c0287410.1021/acsenergylett.4c02874","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02874https://doi.org/10.1021/acsenergylett.4c02874","url":null,"abstract":"<p >Recent progress has shown that alloying cadmium telluride (CdTe) with cadmium selenide (CdSe) to create a CdSe<sub><i>x</i></sub>Te<sub>1–<i>x</i></sub> (CdSeTe) gradient region can significantly boost the performance of polycrystalline CdSeTe thin-film solar cells. However, improper CdSeTe alloying might introduce problematic band alignment and deleterious voids at the front interface, limiting the benefit maximization of this technique. Here, we show that the CdSe layers deposited by thermal evaporation result in CdSeTe cells with a higher performance than the sputtered CdSe. This is because evaporated CdSe can avoid the formation of voids at the front interface, producing improved front junction quality with suppressed front junction nonradiative recombination. The champion cell using evaporated CdSe demonstrated a power conversion efficiency (PCE) of 19.7%, much higher than 18.1% in the cell using sputtered CdSe.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"9 12","pages":"6233–6237 6233–6237"},"PeriodicalIF":19.3,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842669","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}
Deda Peng, Ruitao Sun, Jin Han, Tenglong Zhao, Ruijie Tian, Anran Zhang, Youcai Zhang, Ya You
{"title":"A Low-Concentrated Electrolyte with a 3.5 V Electrochemical Stability Window, Made by Restructuring the H-Bond Network, for High-Energy and Long-Life Aqueous Sodium-Ion Batteries","authors":"Deda Peng, Ruitao Sun, Jin Han, Tenglong Zhao, Ruijie Tian, Anran Zhang, Youcai Zhang, Ya You","doi":"10.1021/acsenergylett.4c02901","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02901","url":null,"abstract":"The narrow electrochemical stability window (ESW) of electrolytes is primarily responsible for the low energy density and poor cycle life of aqueous sodium-ion batteries (ASIBs). Although water-in-salt electrolytes can effectively widen the ESW, their high salt concentration leads to high costs. In this work, we found that weak-polar solvents have more advantages in broadening the ESW than strong-polar solvents. Taking 1,3,6-hexanetricarbonitrile as an example, it evidently enhances the stability of water by weakening the hydrogen bond network. Consequently, it broadens the ESW to 3.5 V at a relatively low concentration and enables Na<sub>2</sub>FeFe(CN)<sub>6</sub>||NaTi<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> full cells with a capacity retention of 70% after 10 000 cycles and an energy density of 71 Wh kg<sup>–1</sup>, based on the active materials’ mass of both electrodes. This work offers new prospects for the development of high-energy and long-life aqueous sodium-ion batteries for large-scale energy storage.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"208 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142763344","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}
Sabin Neupane, Deng-Bing Li, Manoj Kumar Jamarkattel, Abasi Abudulimu, Chun-Sheng Jiang, Sandip S. Bista, Alisha Adhikari, Sanjeeb Budhathoki, Hamim Sharif, Kiran Lamichhane, Tyler Brau, Adam B. Phillips, Ambalanath Shan, Randall J. Ellingson, Michael J. Heben, Yanfa Yan
{"title":"Evaporated CdSe for Efficient Polycrystalline CdSeTe Thin-Film Solar Cells","authors":"Sabin Neupane, Deng-Bing Li, Manoj Kumar Jamarkattel, Abasi Abudulimu, Chun-Sheng Jiang, Sandip S. Bista, Alisha Adhikari, Sanjeeb Budhathoki, Hamim Sharif, Kiran Lamichhane, Tyler Brau, Adam B. Phillips, Ambalanath Shan, Randall J. Ellingson, Michael J. Heben, Yanfa Yan","doi":"10.1021/acsenergylett.4c02874","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02874","url":null,"abstract":"Recent progress has shown that alloying cadmium telluride (CdTe) with cadmium selenide (CdSe) to create a CdSe<sub><i>x</i></sub>Te<sub>1–<i>x</i></sub> (CdSeTe) gradient region can significantly boost the performance of polycrystalline CdSeTe thin-film solar cells. However, improper CdSeTe alloying might introduce problematic band alignment and deleterious voids at the front interface, limiting the benefit maximization of this technique. Here, we show that the CdSe layers deposited by thermal evaporation result in CdSeTe cells with a higher performance than the sputtered CdSe. This is because evaporated CdSe can avoid the formation of voids at the front interface, producing improved front junction quality with suppressed front junction nonradiative recombination. The champion cell using evaporated CdSe demonstrated a power conversion efficiency (PCE) of 19.7%, much higher than 18.1% in the cell using sputtered CdSe.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"17 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142777129","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 : 2024-12-03DOI: 10.1021/acsenergylett.4c0199910.1021/acsenergylett.4c01999
Peiyuan Ma, Cindy Xue, Ke-Hsin Wang, Priyadarshini Mirmira, Minh Canh Vu, Oscar Rivera and Chibueze V. Amanchukwu*,
{"title":"Molecular Structure Optimization of Fluorinated Ether Electrolyte for All Temperature Fast Charging Lithium-Ion Battery","authors":"Peiyuan Ma, Cindy Xue, Ke-Hsin Wang, Priyadarshini Mirmira, Minh Canh Vu, Oscar Rivera and Chibueze V. Amanchukwu*, ","doi":"10.1021/acsenergylett.4c0199910.1021/acsenergylett.4c01999","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01999https://doi.org/10.1021/acsenergylett.4c01999","url":null,"abstract":"<p >New electrolytes are needed to replace commercial carbonate electrolytes to enable a wider working temperature range, higher energy density, and faster charging of lithium-ion batteries (LIBs). Fluorinated diluents and solvents have shown promise in LIB electrolyte design, but most of them are considered per- and polyfluoroalkyl substances (PFAS) with significant environmental and health concerns. In this work, we design a family of non-PFAS, partially fluorinated ether solvents for LIB electrolytes. Through rational molecular design, an optimized rate capability is achieved by low viscosity, weak lithium-ion solvation, and high ion diffusivity. The optimized electrolytes enable a longer cycle life and better rate capability (up to 6 C) than previously reported fluorinated ethers or commercial carbonate electrolyte in graphite/LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (Gr/NMC811) full cells. In addition, they also show an extended working temperature window with stable long-term cycling from 60 to −40 °C. This work shows a promising path to next generation batteries capable of extreme conditions without introducing PFAS concerns.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"9 12","pages":"6144–6152 6144–6152"},"PeriodicalIF":19.3,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842075","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}
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