Pub Date : 2026-01-28DOI: 10.1021/acsenergylett.6c00107
Soobin Lee, Young Sun Park, Juwon Yun, Jeongyoub Lee, Subin Moon, Wooyong Jeong, Chang-Seop Jeong, Sumin Kim, Jun Hwan Kim, Donghyun Kim, Wonjun Lee, Hyung-Ho Park, Jeiwan Tan, Jooho Moon
Photoelectrochemical (PEC) water splitting offers a sustainable route for solar-to-hydrogen conversion, yet the limited durability of photoelectrodes due to photocorrosion and catalyst degradation remains a challenge. Herein, we present a novel strategy to design a poly(acrylic acid) (PAAC)-based hydrogel protective layer with tunable physical and mechanical properties achieved by incorporating NaCl and polyethylene glycol (PEG). Na+ reorganizes the hydrogen-bonding network of water, leading to compact chain packing and enlarged pores, while PEG forms hydrogen bonds with PAAC, maintaining network flexibility and elasticity. This cooperative effect yields robust pore architecture, featuring enlarged pores and thickened pore walls with elasticity and fatigue resistance retained. When integrated with Sb2(S,Se)3 photocathodes, the hydrogel enables stable operation for 220 h in an acidic electrolyte (0.1 M H2SO4), facilitating gas bubble release and mitigating device degradation. This study highlights the potential of hydrogel engineering to extend the operating lifetime of PEC systems, advancing durable green hydrogen production.
光电化学（PEC）水分解为太阳能-氢转化提供了一条可持续的途径，但由于光腐蚀和催化剂降解，光电极的耐用性有限仍然是一个挑战。在此，我们提出了一种新的策略，设计了一种基于聚丙烯酸（PAAC）的水凝胶保护层，该保护层通过加入NaCl和聚乙二醇（PEG）来实现物理和机械性能的可调。Na+对水的氢键网络进行重组，导致链式排列紧密，孔隙扩大，而PEG与PAAC形成氢键，保持网络的柔韧性和弹性。这种协同作用产生了坚固的孔隙结构，具有扩大的孔隙和增厚的孔壁，同时保留了弹性和抗疲劳性。当与Sb2(S,Se)3光电阴极集成时，水凝胶可以在酸性电解质（0.1 M H2SO4）中稳定工作220小时，促进气泡释放并减轻器件降解。这项研究强调了水凝胶工程的潜力，可以延长PEC系统的使用寿命，促进持久的绿色制氢。
{"title":"Tailoring a Poly(acrylic acid)-Based Hydrogel Protective Layer for Durable Photoelectrochemical Water Splitting in Acidic Media","authors":"Soobin Lee, Young Sun Park, Juwon Yun, Jeongyoub Lee, Subin Moon, Wooyong Jeong, Chang-Seop Jeong, Sumin Kim, Jun Hwan Kim, Donghyun Kim, Wonjun Lee, Hyung-Ho Park, Jeiwan Tan, Jooho Moon","doi":"10.1021/acsenergylett.6c00107","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c00107","url":null,"abstract":"Photoelectrochemical (PEC) water splitting offers a sustainable route for solar-to-hydrogen conversion, yet the limited durability of photoelectrodes due to photocorrosion and catalyst degradation remains a challenge. Herein, we present a novel strategy to design a poly(acrylic acid) (PAAC)-based hydrogel protective layer with tunable physical and mechanical properties achieved by incorporating NaCl and polyethylene glycol (PEG). Na<sup>+</sup> reorganizes the hydrogen-bonding network of water, leading to compact chain packing and enlarged pores, while PEG forms hydrogen bonds with PAAC, maintaining network flexibility and elasticity. This cooperative effect yields robust pore architecture, featuring enlarged pores and thickened pore walls with elasticity and fatigue resistance retained. When integrated with Sb<sub>2</sub>(S,Se)<sub>3</sub> photocathodes, the hydrogel enables stable operation for 220 h in an acidic electrolyte (0.1 M H<sub>2</sub>SO<sub>4</sub>), facilitating gas bubble release and mitigating device degradation. This study highlights the potential of hydrogel engineering to extend the operating lifetime of PEC systems, advancing durable green hydrogen production.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"3 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072524","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}
LiNi0.5Mn1.5O4 (LNMO) cathode attracts great attention due to its low cost, good air stability, and three-dimensional lithium-diffusion channels. However, the operation voltage of LNMO (∼5 V vs Li+/Li) exceeds the oxidative limitation of most electrolytes, hindering the application of LNMO batteries. Fluorinated carbonate-based electrolytes can partially solve the oxidation challenge, but excessive viscosity and poor solvation ability cause the sluggish transport of Li+. Here we report a moderate solvation electrolyte design using 2,2,2-trifluoroethyl acetate (EA3F) as the main solvent to stabilize LNMO cathodes under fast charging conditions. EA3F not only shows moderate Li+ coordination that can promote fast desolvation, but also facilitates the formation of thin and robust interphases at cathode/anode electrodes. Consequently, the 1.4 Ah graphite||LNMO pouch cells with this electrolyte can achieve 80% capacity retention over 1200 cycles at 1 C and release ∼90% capacity retention at a rate of 4 C (9.4 mA cm–2).
LiNi0.5Mn1.5O4 （LNMO）阴极以其低廉的成本、良好的空气稳定性和三维锂扩散通道而备受关注。然而，LNMO的工作电压（~ 5 V vs Li+/Li）超过了大多数电解质的氧化极限，阻碍了LNMO电池的应用。含氟碳酸盐电解质可以部分解决氧化挑战，但过高的粘度和较差的溶剂化能力导致Li+的运输缓慢。本文报道了一种以2,2,2-三氟乙酸乙酯（EA3F）为主要溶剂的适度溶剂化电解质设计，以稳定快速充电条件下的LNMO阴极。EA3F不仅表现出适度的Li+配位，有利于快速脱溶，而且有利于在阴极/阳极电极形成薄而坚固的界面相。因此，使用这种电解质的1.4 Ah石墨||LNMO袋电池在1c下可以在1200次循环中获得80%的容量保留，并在4c （9.4 mA cm-2）的速率下释放90%的容量保留。
{"title":"Moderate Solvation Structure Design Endows Long Cycling of 5 V-Class Fast-Charging Lithium-Ion Batteries","authors":"Ruilin He, Tong Zhang, Fangzheng Liu, Junhao Li, Jiachun Wu, Xueping Xiao, Xiaoqi Wu, Jun Wang, Yan Li, Fangfang Pan, Yonghong Deng, Guangzhao Zhang","doi":"10.1021/acsenergylett.5c03751","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03751","url":null,"abstract":"LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> (LNMO) cathode attracts great attention due to its low cost, good air stability, and three-dimensional lithium-diffusion channels. However, the operation voltage of LNMO (∼5 V vs Li<sup>+</sup>/Li) exceeds the oxidative limitation of most electrolytes, hindering the application of LNMO batteries. Fluorinated carbonate-based electrolytes can partially solve the oxidation challenge, but excessive viscosity and poor solvation ability cause the sluggish transport of Li<sup>+</sup>. Here we report a moderate solvation electrolyte design using 2,2,2-trifluoroethyl acetate (EA3F) as the main solvent to stabilize LNMO cathodes under fast charging conditions. EA3F not only shows moderate Li<sup>+</sup> coordination that can promote fast desolvation, but also facilitates the formation of thin and robust interphases at cathode/anode electrodes. Consequently, the 1.4 Ah graphite||LNMO pouch cells with this electrolyte can achieve 80% capacity retention over 1200 cycles at 1 C and release ∼90% capacity retention at a rate of 4 C (9.4 mA cm<sup>–2</sup>).","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"41 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146048304","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}
Pub Date : 2026-01-27DOI: 10.1021/acsenergylett.5c03690
Jin Zhang, Peter W. Voorhees
Achieving stable lithium metal anodes requires control over the solid-electrolyte interphase (SEI) and desolvation kinetics. Here, we develop a unified theoretical framework integrating ion transport, desolvation, charge transfer, and SEI breakdown to predict morphological instabilities during electrodeposition. Using linear stability analysis, we identify six dimensionless parameters that govern the onset and evolution of instabilities. We show that SEI transport and desolvation rate effectively modulate apparent reaction kinetics, shifting the system toward a stable, reaction-limited regime. Extending the classical limiting current concept, we demonstrate that a thick, poorly conductive SEI and sluggish desolvation significantly reduce the limiting current. We introduce an apparent Damköhler number to quantify the critical balance: suppressing diffusion-limited instabilities by reaction rate reduction, while maintaining a high limiting current. Our theory enables predictive mapping of electrodeposition morphologies across diverse materials and operating conditions, guiding the rational design of stable lithium metal anodes.
{"title":"Morphological Stability of Metal Anodes: Roles of Solid Electrolyte Interphases (SEIs) and Desolvation Kinetics","authors":"Jin Zhang, Peter W. Voorhees","doi":"10.1021/acsenergylett.5c03690","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03690","url":null,"abstract":"Achieving stable lithium metal anodes requires control over the solid-electrolyte interphase (SEI) and desolvation kinetics. Here, we develop a unified theoretical framework integrating ion transport, desolvation, charge transfer, and SEI breakdown to predict morphological instabilities during electrodeposition. Using linear stability analysis, we identify six dimensionless parameters that govern the onset and evolution of instabilities. We show that SEI transport and desolvation rate effectively modulate apparent reaction kinetics, shifting the system toward a stable, reaction-limited regime. Extending the classical limiting current concept, we demonstrate that a thick, poorly conductive SEI and sluggish desolvation significantly reduce the limiting current. We introduce an apparent Damköhler number to quantify the critical balance: suppressing diffusion-limited instabilities by reaction rate reduction, while maintaining a high limiting current. Our theory enables predictive mapping of electrodeposition morphologies across diverse materials and operating conditions, guiding the rational design of stable lithium metal anodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"78 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146057134","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}
Pub Date : 2026-01-27DOI: 10.1021/acsenergylett.5c04247
Yizhen Chen, Richard L. Brutchey
Direct recovery of elemental antimony (Sb) and bismuth (Bi) from sulfide ores under mild conditions remains a fundamental challenge. Binary sulfides, such as stibnite (Sb2S3) and bismuthinite (Bi2S3), are abundant mineral sources of critical elements, yet their extremely low solubility precludes conventional electrowinning. Here, we report the first acid-free, room-temperature method for selective electrowinning of Sb and Bi, enabled by a thiol–amine “alkahest” solvent that dissolves otherwise intractable sulfides. This approach enables electrochemical reduction to dense, nanoscale-uniform Sb films from natural ore, maintaining high selectivity against associated sulfides and gangue. The Faradaic efficiency is 80% with an energy consumption of 2.6 kWh/kg for Sb. The same strategy enables Bi electrowinning from bismuthinite and bismite (Bi2O3). These results establish a generalizable pathway for direct recovery of critical elements from sulfide and oxide ores and highlight alkahest solvents as a versatile platform for selective multielectron redox in complex solid–liquid systems.
{"title":"Mild and Selective Alkahest-Enabled Electrochemical Extraction of Critical Elements from Ores","authors":"Yizhen Chen, Richard L. Brutchey","doi":"10.1021/acsenergylett.5c04247","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04247","url":null,"abstract":"Direct recovery of elemental antimony (Sb) and bismuth (Bi) from sulfide ores under mild conditions remains a fundamental challenge. Binary sulfides, such as stibnite (Sb<sub>2</sub>S<sub>3</sub>) and bismuthinite (Bi<sub>2</sub>S<sub>3</sub>), are abundant mineral sources of critical elements, yet their extremely low solubility precludes conventional electrowinning. Here, we report the first acid-free, room-temperature method for selective electrowinning of Sb and Bi, enabled by a thiol–amine “alkahest” solvent that dissolves otherwise intractable sulfides. This approach enables electrochemical reduction to dense, nanoscale-uniform Sb films from natural ore, maintaining high selectivity against associated sulfides and gangue. The Faradaic efficiency is 80% with an energy consumption of 2.6 kWh/kg for Sb. The same strategy enables Bi electrowinning from bismuthinite and bismite (Bi<sub>2</sub>O<sub>3</sub>). These results establish a generalizable pathway for direct recovery of critical elements from sulfide and oxide ores and highlight alkahest solvents as a versatile platform for selective multielectron redox in complex solid–liquid systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"2 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146057136","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}
Pub Date : 2026-01-27DOI: 10.1021/acsenergylett.5c04220
Alexander Juul Nielsen, Feng Wu, Kevin Brennan, Jakob Kibsgaard
Dual atom catalysts (DACs) are emerging as a new frontier in electrocatalysis. Building on the success of single atom catalysts (SACs), they are believed to display remarkable activity and selectivity, especially in the electrochemical oxygen reduction and CO2 reduction reactions (ORR and CO2RR). They are, however, difficult to selectively synthesize, and in most studies, there is an overlap with single atom catalysts in terms of both synthesis procedure and electrocatalytic activity. Indisputably determining their prevalence over single atom sites or even clusters and nanoparticles is a daunting task with the characterization methods that are available. In this Perspective, we argue that in many studies, the electrocatalytic activity could be explained simply through the presence of single atom catalysts. Still, some studies stand out as being notably superior to most single atom catalysts, nurturing a hopeful outlook for the field. In electrocatalysis, most studied DACs and SACs are carbon supported. In this Perspective, we go through the state of the field for these catalysts in the two electrochemical reactions ORR and CO2RR. We give an overview of synthesis procedures for carbon supported DACs and the two most used characterization methods, high-angle annular dark-field emission scanning transmission electron microscopy and extended X-ray absorption fine structure (HAADF-STEM and EXAFS). We also highlight common misinterpretations and recommend good practices in future studies.
{"title":"On the Challenge of Verifying Dual Atom Catalyst Presence and Their Superiority over Single Atom Catalysts","authors":"Alexander Juul Nielsen, Feng Wu, Kevin Brennan, Jakob Kibsgaard","doi":"10.1021/acsenergylett.5c04220","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04220","url":null,"abstract":"Dual atom catalysts (DACs) are emerging as a new frontier in electrocatalysis. Building on the success of single atom catalysts (SACs), they are believed to display remarkable activity and selectivity, especially in the electrochemical oxygen reduction and CO<sub>2</sub> reduction reactions (ORR and CO<sub>2</sub>RR). They are, however, difficult to selectively synthesize, and in most studies, there is an overlap with single atom catalysts in terms of both synthesis procedure and electrocatalytic activity. Indisputably determining their prevalence over single atom sites or even clusters and nanoparticles is a daunting task with the characterization methods that are available. In this Perspective, we argue that in many studies, the electrocatalytic activity could be explained simply through the presence of single atom catalysts. Still, some studies stand out as being notably superior to most single atom catalysts, nurturing a hopeful outlook for the field. In electrocatalysis, most studied DACs and SACs are carbon supported. In this Perspective, we go through the state of the field for these catalysts in the two electrochemical reactions ORR and CO<sub>2</sub>RR. We give an overview of synthesis procedures for carbon supported DACs and the two most used characterization methods, high-angle annular dark-field emission scanning transmission electron microscopy and extended X-ray absorption fine structure (HAADF-STEM and EXAFS). We also highlight common misinterpretations and recommend good practices in future studies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"67 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146048401","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}
Semisolid slurry batteries (S3-batteries) can eliminate energy-intensive manufacturing but are hindered by particle sedimentation and rapid capacity fade. Here we report long-lived, abuse-tolerant S3-batteries enabled by a biomimetic ethyl cellulose (EtC) stabilization strategy. EtC forms entangled polymer networks within slurry electrodes, eliminating solid–liquid phase separation and suppressing electrolyte volatilization while maintaining processable rheology. Embedded three-electrode diagnostics in pouch cells identify lithium plating as the primary degradation mechanism. Guided by this diagnosis, we combine N/P capacity ratio fine-tuning with cathode prelithiation to eliminate anode Li plating and compensate for active Li loss, delivering exceptional full-cell stability over 500 cycles and setting a new benchmark for slurry batteries. Prototype pouch-type full cells further demonstrate outstanding mechanical-abuse tolerance while retaining electrochemical function without hazardous failure. Successful adaptation to sodium-ion battery chemistry confirms the versatility of these principles, offering a promising pathway for next-generation, sustainable energy storage technologies.
{"title":"Long-Lived and Mechanical-Abuse-Tolerant Semisolid Slurry Batteries","authors":"Hongli Chen, Wei You, Yong Wang, Yilin Chen, Yu-Shi He, Xianxia Yuan, Zi-Feng Ma, Linsen Li","doi":"10.1021/acsenergylett.5c03717","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03717","url":null,"abstract":"Semisolid slurry batteries (S<sup>3</sup>-batteries) can eliminate energy-intensive manufacturing but are hindered by particle sedimentation and rapid capacity fade. Here we report long-lived, abuse-tolerant S<sup>3</sup>-batteries enabled by a biomimetic ethyl cellulose (EtC) stabilization strategy. EtC forms entangled polymer networks within slurry electrodes, eliminating solid–liquid phase separation and suppressing electrolyte volatilization while maintaining processable rheology. Embedded three-electrode diagnostics in pouch cells identify lithium plating as the primary degradation mechanism. Guided by this diagnosis, we combine N/P capacity ratio fine-tuning with cathode prelithiation to eliminate anode Li plating and compensate for active Li loss, delivering exceptional full-cell stability over 500 cycles and setting a new benchmark for slurry batteries. Prototype pouch-type full cells further demonstrate outstanding mechanical-abuse tolerance while retaining electrochemical function without hazardous failure. Successful adaptation to sodium-ion battery chemistry confirms the versatility of these principles, offering a promising pathway for next-generation, sustainable energy storage technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"180 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072646","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}
Pub Date : 2026-01-27DOI: 10.1021/acsenergylett.5c02980
Zhuohan Li, Benjamin X. Lam, Shilong Wang, Gerbrand Ceder
Understanding the moisture stability of oxide Li-ion conductors is important for their practical applications in solid-state batteries. Unlike sulfide or halide conductors, oxide conductors generally better resist degradation when in contact with water but can still undergo topotactic Li+/H+ exchange (LHX). Here, we combine density functional theory (DFT) calculations with a machine-learning interatomic potential model to investigate the thermodynamic driving force of the LHX reaction for two representative oxide Li-ion conductor families: garnets and NASICONs. Li-stuffed garnets exhibit a strong driving force for proton exchange due to their high Li chemical potential. In contrast, NASICONs demonstrate a higher resistance against proton exchange due to the lower Li chemical potential and the lower O–H bond covalency for polyanion-bonded oxygens. Our findings reveal a critical trade-off: Li stuffing enhances conductivity but increases moisture susceptibility. This study underscores the importance of designing Li-ion conductors that possess both high conductivity and high stability in practical environments.
{"title":"Li+/H+ Exchange in Solid-State Oxide Li-Ion Conductors","authors":"Zhuohan Li, Benjamin X. Lam, Shilong Wang, Gerbrand Ceder","doi":"10.1021/acsenergylett.5c02980","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c02980","url":null,"abstract":"Understanding the moisture stability of oxide Li-ion conductors is important for their practical applications in solid-state batteries. Unlike sulfide or halide conductors, oxide conductors generally better resist degradation when in contact with water but can still undergo topotactic Li<sup>+</sup>/H<sup>+</sup> exchange (LHX). Here, we combine density functional theory (DFT) calculations with a machine-learning interatomic potential model to investigate the thermodynamic driving force of the LHX reaction for two representative oxide Li-ion conductor families: garnets and NASICONs. Li-stuffed garnets exhibit a strong driving force for proton exchange due to their high Li chemical potential. In contrast, NASICONs demonstrate a higher resistance against proton exchange due to the lower Li chemical potential and the lower O–H bond covalency for polyanion-bonded oxygens. Our findings reveal a critical trade-off: Li stuffing enhances conductivity but increases moisture susceptibility. This study underscores the importance of designing Li-ion conductors that possess both high conductivity and high stability in practical environments.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 1 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146057133","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}
Pub Date : 2026-01-27DOI: 10.1021/acsenergylett.5c03992
Ling Che, Kun Zhang, Zhaowen Hu, Guangyao Liu, Shu Chen, Zihao Li, Chao Shen, Yiran Ying, Keyu Xie
Lithium plating and poor low-temperature performance of graphite anodes stem from sluggish Li+ desolvation and transport across the solid electrolyte interphase (SEI). Here, we construct a LiF-LiCl-LiBr hybrid (LiFCB)-rich SEI, which simultaneously suppresses electron tunneling and facilitates Li+ migration. We further introduce two quantitative descriptors: SSEI (related to Li+/solvent adsorption for desolvation) and WSEI (linked to the electron work function and Li+ transfer barrier for charge/ion transfer). These descriptors enable a predictive framework for evaluating the coupled charge/ion transfer and ion desolvation–peeling capabilities of SEIs. Consequently, a 5 Ah LiFePO4||graphite pouch cell with the heterohalogenated SEI delivers nearly 100% capacity retention at −20 °C relative to room temperature and 75.6% retention even at −40 °C. Furthermore, the cell sustains 95.6% capacity over 350 cycles at −20 °C without observable Li plating. This work establishes a mechanistic link between SEI composition and interfacial kinetics for developing high-performance and durable low-temperature LIBs.
{"title":"Heterohalogenated Hybrid SEI Reconstructs Graphite Anode Interfacial Kinetics at Low Temperatures","authors":"Ling Che, Kun Zhang, Zhaowen Hu, Guangyao Liu, Shu Chen, Zihao Li, Chao Shen, Yiran Ying, Keyu Xie","doi":"10.1021/acsenergylett.5c03992","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03992","url":null,"abstract":"Lithium plating and poor low-temperature performance of graphite anodes stem from sluggish Li<sup>+</sup> desolvation and transport across the solid electrolyte interphase (SEI). Here, we construct a LiF-LiCl-LiBr hybrid (LiFCB)-rich SEI, which simultaneously suppresses electron tunneling and facilitates Li<sup>+</sup> migration. We further introduce two quantitative descriptors: S<sub>SEI</sub> (related to Li<sup>+</sup>/solvent adsorption for desolvation) and W<sub>SEI</sub> (linked to the electron work function and Li<sup>+</sup> transfer barrier for charge/ion transfer). These descriptors enable a predictive framework for evaluating the coupled charge/ion transfer and ion desolvation–peeling capabilities of SEIs. Consequently, a 5 Ah LiFePO<sub>4</sub>||graphite pouch cell with the heterohalogenated SEI delivers nearly 100% capacity retention at −20 °C relative to room temperature and 75.6% retention even at −40 °C. Furthermore, the cell sustains 95.6% capacity over 350 cycles at −20 °C without observable Li plating. This work establishes a mechanistic link between SEI composition and interfacial kinetics for developing high-performance and durable low-temperature LIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"30 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146057135","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}
Pub Date : 2026-01-26DOI: 10.1021/acsenergylett.5c03901
Na Shi,Hao Tian,Guangyue Yang,Panyu Wang,Yu Lei,Wei Li,Jingfu Jiang,Xiaoqing Jiang,Zhongjin Shen,Marina Freitag,Xin Guo,Shuping Pang
The incorporation of self-polymerizable additives is an effective strategy to improve both efficiency and stability of perovskite solar cells (PSCs), yet the structure-performance relationship remains unclear. Here, two self-polymerizable additives, 2,2,3,3,3-pentafluoropropyl acrylate (PFPA) and n-propyl acrylate (NPA), are systematically investigated. Both additives undergo in situ thermal polymerization during perovskite annealing. The fluorinated PFPA exhibits strong interactions with undercoordinated Pb2+, enabling effective crystallization regulation and defect passivation. Polymerized PFPA preferentially accumulates at the perovskite top surface, forming a hydrophobic dipole layer that enhances charge extraction and interfacial stability. As a result, PSCs with polymerized PFPA achieve a champion power conversion efficiency (PCE) of 26.01% and retain 90.0% of the initial efficiency after 840 h at 85 °C in nitrogen and 95.1% after 1000 h under maximum power point tracking conditions. Furthermore, minimodules with an active area of 14 cm2 deliver a PCE of 21.66%.
{"title":"Multifunctional Fluorinated Self-Polymerizable Additive Improves the Performance of Perovskite Photovoltaics","authors":"Na Shi,Hao Tian,Guangyue Yang,Panyu Wang,Yu Lei,Wei Li,Jingfu Jiang,Xiaoqing Jiang,Zhongjin Shen,Marina Freitag,Xin Guo,Shuping Pang","doi":"10.1021/acsenergylett.5c03901","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03901","url":null,"abstract":"The incorporation of self-polymerizable additives is an effective strategy to improve both efficiency and stability of perovskite solar cells (PSCs), yet the structure-performance relationship remains unclear. Here, two self-polymerizable additives, 2,2,3,3,3-pentafluoropropyl acrylate (PFPA) and n-propyl acrylate (NPA), are systematically investigated. Both additives undergo in situ thermal polymerization during perovskite annealing. The fluorinated PFPA exhibits strong interactions with undercoordinated Pb2+, enabling effective crystallization regulation and defect passivation. Polymerized PFPA preferentially accumulates at the perovskite top surface, forming a hydrophobic dipole layer that enhances charge extraction and interfacial stability. As a result, PSCs with polymerized PFPA achieve a champion power conversion efficiency (PCE) of 26.01% and retain 90.0% of the initial efficiency after 840 h at 85 °C in nitrogen and 95.1% after 1000 h under maximum power point tracking conditions. Furthermore, minimodules with an active area of 14 cm2 deliver a PCE of 21.66%.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"51 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044951","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}
Pub Date : 2026-01-26DOI: 10.1021/acsenergylett.5c03901
Na Shi,Hao Tian,Guangyue Yang,Panyu Wang,Yu Lei,Wei Li,Jingfu Jiang,Xiaoqing Jiang,Zhongjin Shen,Marina Freitag,Xin Guo,Shuping Pang
The incorporation of self-polymerizable additives is an effective strategy to improve both efficiency and stability of perovskite solar cells (PSCs), yet the structure-performance relationship remains unclear. Here, two self-polymerizable additives, 2,2,3,3,3-pentafluoropropyl acrylate (PFPA) and n-propyl acrylate (NPA), are systematically investigated. Both additives undergo in situ thermal polymerization during perovskite annealing. The fluorinated PFPA exhibits strong interactions with undercoordinated Pb2+, enabling effective crystallization regulation and defect passivation. Polymerized PFPA preferentially accumulates at the perovskite top surface, forming a hydrophobic dipole layer that enhances charge extraction and interfacial stability. As a result, PSCs with polymerized PFPA achieve a champion power conversion efficiency (PCE) of 26.01% and retain 90.0% of the initial efficiency after 840 h at 85 °C in nitrogen and 95.1% after 1000 h under maximum power point tracking conditions. Furthermore, minimodules with an active area of 14 cm2 deliver a PCE of 21.66%.
{"title":"Multifunctional Fluorinated Self-Polymerizable Additive Improves the Performance of Perovskite Photovoltaics","authors":"Na Shi,Hao Tian,Guangyue Yang,Panyu Wang,Yu Lei,Wei Li,Jingfu Jiang,Xiaoqing Jiang,Zhongjin Shen,Marina Freitag,Xin Guo,Shuping Pang","doi":"10.1021/acsenergylett.5c03901","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03901","url":null,"abstract":"The incorporation of self-polymerizable additives is an effective strategy to improve both efficiency and stability of perovskite solar cells (PSCs), yet the structure-performance relationship remains unclear. Here, two self-polymerizable additives, 2,2,3,3,3-pentafluoropropyl acrylate (PFPA) and n-propyl acrylate (NPA), are systematically investigated. Both additives undergo in situ thermal polymerization during perovskite annealing. The fluorinated PFPA exhibits strong interactions with undercoordinated Pb2+, enabling effective crystallization regulation and defect passivation. Polymerized PFPA preferentially accumulates at the perovskite top surface, forming a hydrophobic dipole layer that enhances charge extraction and interfacial stability. As a result, PSCs with polymerized PFPA achieve a champion power conversion efficiency (PCE) of 26.01% and retain 90.0% of the initial efficiency after 840 h at 85 °C in nitrogen and 95.1% after 1000 h under maximum power point tracking conditions. Furthermore, minimodules with an active area of 14 cm2 deliver a PCE of 21.66%.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"68 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044950","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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