{"title":"Unlocking Ultrafast Diagnosis of Retired Batteries via Interpretable Machine Learning and Optical Fiber Sensors","authors":"Taolue Zhang, Ruifeng Tan, Pinxi Zhu, Tong-Yi Zhang* and Jiaqiang Huang*, ","doi":"10.1021/acsenergylett.4c0305410.1021/acsenergylett.4c03054","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03054https://doi.org/10.1021/acsenergylett.4c03054","url":null,"abstract":"<p >Retired batteries are of great economic and environmental importance, which are indispensable considerations in the life cycle of lithium-ion batteries. However, existing methods for evaluating retired batteries are time- and resource-consuming, hindering efficient screening for later recycling or reuse. Herein, combining optical fiber sensors and interpretable machine learning (ML), we establish a data-driven framework for retired battery datasets with 265 cells of different chemistries (LiFePO<sub>4</sub>/graphite, LiMn<sub>2</sub>O<sub>4</sub>/graphite) and achieve ultrafast state of health diagnosis within 3 min, offering mean absolute errors of 1.17% and 2.78%, respectively. The proposed data-driven framework identifies the salient regions in the time-resolved multivariable data and helps to uncover underlying thermodynamic/kinetic aging mechanisms. We also demonstrate the incorporated thermal information obtained via optical fibers complements voltage signals by improving prediction accuracy and antinoise ability. This work not only showcases the potential of battery sensing in retired battery diagnosis but also unlocks the unexplored synergy between sensing and interpretable ML for diverse battery applications.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"862–871 862–871"},"PeriodicalIF":19.3,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402326","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 : 2025-01-20DOI: 10.1021/acsenergylett.4c0321610.1021/acsenergylett.4c03216
Wenbin Fu, Kaixi Chen, Fujia Wang, Yice Wang, Evan Wilson, Vismay Chandra, Doyoub Kim and Gleb Yushin*,
{"title":"A Conversion Aluminum Fluoride Nanowire Interlayer for Stable Lithium Metal Batteries","authors":"Wenbin Fu, Kaixi Chen, Fujia Wang, Yice Wang, Evan Wilson, Vismay Chandra, Doyoub Kim and Gleb Yushin*, ","doi":"10.1021/acsenergylett.4c0321610.1021/acsenergylett.4c03216","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03216https://doi.org/10.1021/acsenergylett.4c03216","url":null,"abstract":"<p >The use of a lithium metal anode enables batteries with significantly higher energy density, but at the expense of the growth of lithium dendrites that trigger internal short circuits, induce safety risks, and reduce cycle stability. To address this challenge, here, we report the design of an aluminum fluoride nanowire membrane as a conversion interlayer to regulate lithium deposition for significantly more stable and safe lithium metal batteries. The interlayer generates a LiF-rich solid electrolyte interphase and alloy nanoparticles in contact with lithium to offer active sites guiding lithium nucleation, regulating lithium deposition, and increasing Coulombic efficiencies. With such an interlayer, lithium metal full cells show significantly improved stability compared to those with bare Cu, when paired with a LiFePO<sub>4</sub> or LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> cathode. Our results indicate that using an aluminum fluoride interlayer can be a promising strategy in realizing lithium metal batteries with high specific energy density.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"853–861 853–861"},"PeriodicalIF":19.3,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenergylett.4c03216","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402382","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}
{"title":"A Conversion Aluminum Fluoride Nanowire Interlayer for Stable Lithium Metal Batteries","authors":"Wenbin Fu, Kaixi Chen, Fujia Wang, Yice Wang, Evan Wilson, Vismay Chandra, Doyoub Kim, Gleb Yushin","doi":"10.1021/acsenergylett.4c03216","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03216","url":null,"abstract":"The use of a lithium metal anode enables batteries with significantly higher energy density, but at the expense of the growth of lithium dendrites that trigger internal short circuits, induce safety risks, and reduce cycle stability. To address this challenge, here, we report the design of an aluminum fluoride nanowire membrane as a conversion interlayer to regulate lithium deposition for significantly more stable and safe lithium metal batteries. The interlayer generates a LiF-rich solid electrolyte interphase and alloy nanoparticles in contact with lithium to offer active sites guiding lithium nucleation, regulating lithium deposition, and increasing Coulombic efficiencies. With such an interlayer, lithium metal full cells show significantly improved stability compared to those with bare Cu, when paired with a LiFePO<sub>4</sub> or LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> cathode. Our results indicate that using an aluminum fluoride interlayer can be a promising strategy in realizing lithium metal batteries with high specific energy density.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"30 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142990758","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 : 2025-01-18DOI: 10.1021/acsenergylett.4c0353810.1021/acsenergylett.4c03538
Olivia T. Vulpin, James B. Mitchell, Lihaokun Chen, Jeonghoon Lim, Sayantan Sasmal, Nathan G. Price, Sam R. Jarvis and Shannon W. Boettcher*,
{"title":"Comparing Advanced Bipolar Membranes for High-Current Electrodialysis and Membrane Electrolysis","authors":"Olivia T. Vulpin, James B. Mitchell, Lihaokun Chen, Jeonghoon Lim, Sayantan Sasmal, Nathan G. Price, Sam R. Jarvis and Shannon W. Boettcher*, ","doi":"10.1021/acsenergylett.4c0353810.1021/acsenergylett.4c03538","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03538https://doi.org/10.1021/acsenergylett.4c03538","url":null,"abstract":"<p >Advanced bipolar membranes (BPMs) with low water-dissociation overpotential (η<sub>wd</sub>) may enable new electrochemical technologies for electrolysis, fuel cells, acid–base synthesis, brine remediation, lithium-battery recycling, and cement production. However, these advanced BPMs have only been demonstrated in BPM water electrolysis (BPMWE) configurations where the BPM is under static compression by the porous-transport layers. It is important to study these BPMs in applications like electrodialysis where large degrees of static compression are not possible. We present a BPM electrodialysis (BPMED) platform to measure water-dissociation overpotential (η<sub>wd</sub>) and compare BPMWE and BPMED systems. We show advanced BPMs with half the η<sub>wd</sub> compared to commercial BPMs for BPMED while maintaining ∼90% current efficiency from 0.05–0.5 A cm<sup>–2</sup>. The BPMED η<sub>wd</sub> values are, however, about 0.2 V higher at 0.5 A cm<sup>–2</sup> than those for BPMWE. Regardless, these results show that BPMs developed and optimized in BPMWE applications are well-suited for next-generation high-current-density BPMED technologies.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"845–852 845–852"},"PeriodicalIF":19.3,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402302","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}
Olivia T. Vulpin, James B. Mitchell, Lihaokun Chen, Jeonghoon Lim, Sayantan Sasmal, Nathan G. Price, Sam R. Jarvis, Shannon W. Boettcher
{"title":"Comparing Advanced Bipolar Membranes for High-Current Electrodialysis and Membrane Electrolysis","authors":"Olivia T. Vulpin, James B. Mitchell, Lihaokun Chen, Jeonghoon Lim, Sayantan Sasmal, Nathan G. Price, Sam R. Jarvis, Shannon W. Boettcher","doi":"10.1021/acsenergylett.4c03538","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03538","url":null,"abstract":"Advanced bipolar membranes (BPMs) with low water-dissociation overpotential (η<sub>wd</sub>) may enable new electrochemical technologies for electrolysis, fuel cells, acid–base synthesis, brine remediation, lithium-battery recycling, and cement production. However, these advanced BPMs have only been demonstrated in BPM water electrolysis (BPMWE) configurations where the BPM is under static compression by the porous-transport layers. It is important to study these BPMs in applications like electrodialysis where large degrees of static compression are not possible. We present a BPM electrodialysis (BPMED) platform to measure water-dissociation overpotential (η<sub>wd</sub>) and compare BPMWE and BPMED systems. We show advanced BPMs with half the η<sub>wd</sub> compared to commercial BPMs for BPMED while maintaining ∼90% current efficiency from 0.05–0.5 A cm<sup>–2</sup>. The BPMED η<sub>wd</sub> values are, however, about 0.2 V higher at 0.5 A cm<sup>–2</sup> than those for BPMWE. Regardless, these results show that BPMs developed and optimized in BPMWE applications are well-suited for next-generation high-current-density BPMED technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"30 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989007","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}
{"title":"Uniform Sub-5 nm Crystalline Nickel-Based Heterojunctions for Overall Water Splitting Electrocatalysis","authors":"Yuanyuan Wang, Rui Yin, Lei Yuan, Xingmei Guo, Xiangjun Zheng, Qianqian Fan, Zhongyao Duan, Yuanjun Liu, Junhao Zhang, Shenglin Xiong","doi":"10.1021/acsenergylett.4c03097","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03097","url":null,"abstract":"Exploring a general method for constructing uniform heterostructures with sub-5 nm crystallites and dense interfaces is crucial yet challenging for advancing water electrocatalysis. Herein, a bottom-up cocrystallization strategy, involving in situ transformation of amorphous Ni–P through gas–solid reactions, is proposed to synthesize a series of nickel-based heterojunctions on carbon cloth (CC). Thereinto, interface-wealthy NiS<sub>2</sub>-Ni<sub>2</sub>P/CC with densely packed 3–4 nm crystallites demonstrates superb catalytic performance for both hydrogen and oxygen evolution. The electrolyzer merely requires cell voltages of 1.79 and 1.89 V to propel overall water splitting currents of 200 and 400 mA cm<sup>–2</sup>, respectively, outperforming the vast majority of reported nickel-based heterojunctions. Theoretical calculations reveal that charge redistribution and electronic structure modulation optimize the hydrogen and oxygen evolution pathways at the NiS<sub>2</sub> and Ni<sub>2</sub>P sides of the interfaces, respectively. Moreover, uniform hybridization with densely distributed heterointerfaces offers abundant active sites for electrocatalysis, pioneering an extendable approach for constructing advanced heterojunction catalysts for green hydrogen production.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"27 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989008","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}
{"title":"Uniform Sub-5 nm Crystalline Nickel-Based Heterojunctions for Overall Water Splitting Electrocatalysis","authors":"Yuanyuan Wang, Rui Yin, Lei Yuan, Xingmei Guo*, Xiangjun Zheng, Qianqian Fan, Zhongyao Duan, Yuanjun Liu, Junhao Zhang* and Shenglin Xiong*, ","doi":"10.1021/acsenergylett.4c0309710.1021/acsenergylett.4c03097","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03097https://doi.org/10.1021/acsenergylett.4c03097","url":null,"abstract":"<p >Exploring a general method for constructing uniform heterostructures with sub-5 nm crystallites and dense interfaces is crucial yet challenging for advancing water electrocatalysis. Herein, a bottom-up cocrystallization strategy, involving in situ transformation of amorphous Ni–P through gas–solid reactions, is proposed to synthesize a series of nickel-based heterojunctions on carbon cloth (CC). Thereinto, interface-wealthy NiS<sub>2</sub>-Ni<sub>2</sub>P/CC with densely packed 3–4 nm crystallites demonstrates superb catalytic performance for both hydrogen and oxygen evolution. The electrolyzer merely requires cell voltages of 1.79 and 1.89 V to propel overall water splitting currents of 200 and 400 mA cm<sup>–2</sup>, respectively, outperforming the vast majority of reported nickel-based heterojunctions. Theoretical calculations reveal that charge redistribution and electronic structure modulation optimize the hydrogen and oxygen evolution pathways at the NiS<sub>2</sub> and Ni<sub>2</sub>P sides of the interfaces, respectively. Moreover, uniform hybridization with densely distributed heterointerfaces offers abundant active sites for electrocatalysis, pioneering an extendable approach for constructing advanced heterojunction catalysts for green hydrogen production.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"837–844 837–844"},"PeriodicalIF":19.3,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402300","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 : 2025-01-16DOI: 10.1021/acsenergylett.4c0352510.1021/acsenergylett.4c03525
Jaeyong Lee, Zach J. Hoffman, Saheli Chakraborty, Vivaan Patel and Nitash P. Balsara*,
{"title":"Toward Optimization of Polymer Electrolytes by Electrochemical Characterization: Poly(pentyl malonate) versus Poly(ethylene oxide)","authors":"Jaeyong Lee, Zach J. Hoffman, Saheli Chakraborty, Vivaan Patel and Nitash P. Balsara*, ","doi":"10.1021/acsenergylett.4c0352510.1021/acsenergylett.4c03525","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03525https://doi.org/10.1021/acsenergylett.4c03525","url":null,"abstract":"<p >Ion transport in two polymer electrolytes, poly(ethylene oxide) (PEO) and poly(pentyl malonate) (PPM), mixed with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) is studied in the vicinity of the limiting current. The experimental measurements are in quantitative agreement with theoretical predictions based on the concentrated solution theory. The properties of two electrolytes are compared using a new plot wherein the length-normalized limiting current, <i>i</i><sub>lim</sub><i>L</i>, is plotted as a function of the length-normalized potential drop, Φ<sub>lim</sub>/<i>L</i>, in symmetric cells with electrolyte thickness, <i>L</i>. We propose that electrolyte design should aim to obtain the largest values of <i>i</i><sub>lim</sub><i>L</i> and the smallest values of Φ<sub>lim</sub>/<i>L</i>. Using this criterion, PPM/LiTFSI is a better polymer electrolyte than PEO/LiTFSI. We hope that PPM/LiTFSI will serve as a benchmark for developing next-generation polymer electrolytes.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"831–836 831–836"},"PeriodicalIF":19.3,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402194","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}
Jaeyong Lee, Zach J. Hoffman, Saheli Chakraborty, Vivaan Patel, Nitash P. Balsara
{"title":"Toward Optimization of Polymer Electrolytes by Electrochemical Characterization: Poly(pentyl malonate) versus Poly(ethylene oxide)","authors":"Jaeyong Lee, Zach J. Hoffman, Saheli Chakraborty, Vivaan Patel, Nitash P. Balsara","doi":"10.1021/acsenergylett.4c03525","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03525","url":null,"abstract":"Ion transport in two polymer electrolytes, poly(ethylene oxide) (PEO) and poly(pentyl malonate) (PPM), mixed with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) is studied in the vicinity of the limiting current. The experimental measurements are in quantitative agreement with theoretical predictions based on the concentrated solution theory. The properties of two electrolytes are compared using a new plot wherein the length-normalized limiting current, <i>i</i><sub>lim</sub><i>L</i>, is plotted as a function of the length-normalized potential drop, Φ<sub>lim</sub>/<i>L</i>, in symmetric cells with electrolyte thickness, <i>L</i>. We propose that electrolyte design should aim to obtain the largest values of <i>i</i><sub>lim</sub><i>L</i> and the smallest values of Φ<sub>lim</sub>/<i>L</i>. Using this criterion, PPM/LiTFSI is a better polymer electrolyte than PEO/LiTFSI. We hope that PPM/LiTFSI will serve as a benchmark for developing next-generation polymer electrolytes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"127 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142986222","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}
Tae-Ung Wi, Zachary H Levell, Shaoyun Hao, Ahmad Elgazzar, Peng Zhu, Yuge Feng, Feng-Yang Chen, Wei Ping Lam, Mohsen Shakouri, Yuanyue Liu, Haotian Wang
{"title":"Selective and Stable Ethanol Synthesis via Electrochemical CO2 Reduction in a Solid Electrolyte Reactor","authors":"Tae-Ung Wi, Zachary H Levell, Shaoyun Hao, Ahmad Elgazzar, Peng Zhu, Yuge Feng, Feng-Yang Chen, Wei Ping Lam, Mohsen Shakouri, Yuanyue Liu, Haotian Wang","doi":"10.1021/acsenergylett.4c03091","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03091","url":null,"abstract":"Electrochemical CO<sub>2</sub> reduction to ethanol faces challenges such as low selectivity, a product mixture with liquid electrolyte, and poor catalyst/reactor stability. Here, we developed a grain-rich zinc-doped Cu<sub>2</sub>O precatalyst that presented a high ethanol Faradaic efficiency of over 40% under a current density of 350 mA·cm<sup>–2</sup>. Our density functional theory (DFT) simulation suggested that Zn atoms inside the structure have a greater carbophilicity than the Cu atoms to help facilitate *CHCHO formation, a key reaction intermediate toward ethanol instead of other C<sub>2</sub> products. A high Faradaic efficiency ratio between ethanol and ethylene (FE<sub>EtOH</sub>/FE<sub>C2H4</sub>) reached 2.34 in the zinc-doped Cu<sub>2</sub>O precatalyst, representing an over 4-fold improvement compared to bare Cu<sub>2</sub>O precatalyst. By integrating this Cu-based catalyst into a porous solid electrolyte (PSE) reactor with a salt-managing design, we achieved stable ethanol production for over 180 h under a current density of 250 mA·cm<sup>–2</sup> while maintaining ethanol selectivity at ∼30%.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"106 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981170","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}