ACS Applied Energy Materials最新文献

{"title":"Unlocking 5 V-Class Lithium-Ion Batteries: Challenges and Perspectives on High-Voltage LNMO Cathodes","authors":"Taemin Kim,&nbsp;, ,&nbsp;Hyunsoo Oh,&nbsp;, ,&nbsp;Seongmin Yang,&nbsp;, and ,&nbsp;Hyeon Jeong Lee*,&nbsp;","doi":"10.1021/acsaem.5c02272","DOIUrl":"https://doi.org/10.1021/acsaem.5c02272","url":null,"abstract":"<p >High-voltage spinel-type lithium nickel manganese oxide (LiNi_0.5Mn_1.5O₄, LNMO) is considered a promising cathode material for lithium-ion batteries due to its high operating voltage (∼4.7 V vs Li/Li⁺) and cobalt-free composition, which enables it to deliver approximately 1.5 times higher energy-to-cost efficiency compared to lithium nickel cobalt manganese oxides (NCM). Although LNMO was among the earliest high-voltage cathode materials studied, it has attracted less commercial attention than layered materials such as NCM and lithium nickel aluminum oxides (NCA). This is primarily attributed to persistent challenges during operation, notably rapid capacity fading induced by structural degradation in both the bulk and interfacial regions under high-voltage and high-temperature conditions. Consequently, a comprehensive understanding of LNMO degradation mechanisms, coupled with the development of targeted design strategies, is essential to overcome these limitations. This review emphasizes the structural characteristics of LNMO, both in the bulk and at the interface, that influence its electrochemical performance. Particular focus is placed on recent advancements in strategies such as doping, coating, and morphology control, which have demonstrated effectiveness in mitigating critical issues, including volume changes, oxygen release, transition metal dissolution, and cation migration. Based on findings from various experimental studies and computational modeling, this review aims to elucidate the origins of performance degradation in LNMO and to propose rational design strategies to improve its cycle life and safety. Overall, this work provides a comprehensive roadmap for advancing LNMO, a historically underutilized spinel cathode with significant potential for next-generation high-voltage Li-ion batteries.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13155–13178"},"PeriodicalIF":5.5,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104115","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Research Progress on Lithium Sulfide Synthesis: A Review","authors":"Wei Weng,&nbsp;, ,&nbsp;Youfen Lan,&nbsp;, ,&nbsp;Ding Tang,&nbsp;, ,&nbsp;Liuyu Fu,&nbsp;, ,&nbsp;Wen Tan*,&nbsp;, and ,&nbsp;Shuiping Zhong*,&nbsp;","doi":"10.1021/acsaem.5c02015","DOIUrl":"https://doi.org/10.1021/acsaem.5c02015","url":null,"abstract":"<p >All-solid-state batteries (ASSBs) are regarded as the core direction of the next generation of energy storage technology, with their commercialization time schedule being specifically listed out officially. However, the promising future of ASSBs is highly dependent on the high-efficiency synthesis of lithium sulfide (Li₂S), which is a critical raw material for fabricating solid electrolytes. In fact, Li₂S is also a competitive cathode material for lithium–sulfur batteries due to its high theoretical specific capacity (1167 mAh/g). Unlike previous reports that focus on a single reaction path or experimental details, this review systematically summarizes Li₂S synthesis strategies from a new dimension of reaction medium (liquid phase, solid–solid, gas–solid) and constructs a six-dimensional radar evaluation system based on economic, technical, and environmental impacts. The contents can hopefully provide a comprehensive understanding of synthesizing critical Li₂S raw materials for energy storage, especially for ASSBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13139–13154"},"PeriodicalIF":5.5,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104135","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mitigating Open-Circuit-Voltage Loss in CsPbI2Br Perovskite Solar Cells Based on CsAc/SnO2 Hybrid Electron Transport Layer","authors":"Sai Yang,&nbsp;, ,&nbsp;Yiran Lu,&nbsp;, ,&nbsp;Xiaolong Wang,&nbsp;, ,&nbsp;Jiahao Tian,&nbsp;, ,&nbsp;Hongcai Yu,&nbsp;, ,&nbsp;Chongan Chen,&nbsp;, ,&nbsp;Haoxuan Guo,&nbsp;, ,&nbsp;Yun Lin,&nbsp;, ,&nbsp;Shulin Chen,&nbsp;, ,&nbsp;Yongbo Yuan,&nbsp;, ,&nbsp;Junhui Ran*,&nbsp;, and ,&nbsp;Bin Yang,&nbsp;","doi":"10.1021/acsaem.5c01975","DOIUrl":"https://doi.org/10.1021/acsaem.5c01975","url":null,"abstract":"<p >Significant open-circuit-voltage (<i>V</i>_OC) loss is present in all-inorganic perovskite solar cells (e.g., based on CsPbI₂Br), owing to energy level mismatch between the perovskite layer and charge transport layer. Here, cesium acetate (CsAc) was mixed with tin oxide (SnO₂) to form a hybrid electron transport layer that can reduce the energy level mismatch with the CsPbI₂Br perovskite layer. Ultraviolet photoelectron spectroscopy characterization suggested that the conduction band of the electron transport layer was elevated from −4.51 eV for the SnO₂-only material to −3.64 eV for the CsAc/SnO₂ hybrid form. This change due to the introduction of CsAc in the SnO₂ layer to tune its conduction band is most likely attributed to the formation of a Cs⁺–Ac^– dipole layer near the top surface of the CsAc/SnO₂ hybrid electron transport layer. Additionally, the Cs⁺ ions in the top surface of the hybrid CsAc/SnO₂ electron transport layer play a positive role in facilitating the growth of a follow-up CsPbI₂Br perovskite layer with finer grains and a denser morphology. Compared to the SnO₂-only electron transport layer-based device, CsPbI₂Br solar cells based on CsAc/SnO₂ exhibited a significantly improved photovoltaic performance. The <i>V</i>_OC was increased from 1.11 V for the SnO₂-only device to 1.28 V for the CsAc/SnO₂ device, while the power conversion efficiency increased from 10.9% to 14.67%. This work presents a practicable approach through modifying the SnO₂ layer with CsAc to significantly reduce the <i>V</i>_OC loss by 0.17 V, which paves an important road to develop high-<i>V</i>_OC CsPbI₂Br perovskite solar cells.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13645–13652"},"PeriodicalIF":5.5,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104113","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Iron Single Atoms-Anchored Hollow Porous Carbon Spheres of Brain Fold-like Surfaces Composited with Manganese Dioxide Nanowires as an Advanced Sulfur Host for Lithium–Sulfur Batteries","authors":"Guan-Ru Li,&nbsp;, ,&nbsp;Chih-Chieh Cheng,&nbsp;, ,&nbsp;Yu-Chieh Ting,&nbsp;, ,&nbsp;Tzu-Hsiang Lin,&nbsp;, ,&nbsp;Chiung-Wen Chang,&nbsp;, ,&nbsp;Fan-Yu Yen,&nbsp;, ,&nbsp;Shao-I. Chang,&nbsp;, ,&nbsp;Kai-An Lee,&nbsp;, and ,&nbsp;Shih-Yuan Lu*,&nbsp;","doi":"10.1021/acsaem.5c02205","DOIUrl":"https://doi.org/10.1021/acsaem.5c02205","url":null,"abstract":"<p >Design of sulfur hosts for effective suppression of shuttling of lithium polysulfides (LiPS) is critical to achieving high-performance lithium–sulfur batteries (LSBs). Here, iron single atoms (SA(Fe))-decorated hollow porous carbon spheres (HPCS) composited with α-MnO₂ nanowires are fabricated as a high-performance sulfur host for LSBs. This composite sulfur host takes advantage of Fe SAs to accelerate conversion reactions of LiPS, α-MnO₂ nanowires to adsorb LiPS, and HPCS to boost charge transport and to confine LiPS, enabling high performance of LSBs. The HPCS@SA(Fe)/α-MnO₂-based LSB exhibits a high initial specific capacity of 1095 mAh g^–1 at 0.1C and maintains a decent specific capacity of 343 mAh g^–1 at 2C. A high capacity retention rate of 81.3% after a 300 cycle operation at 1C is achieved, corresponding to a low average capacity decay rate of 0.062% per cycle. Construction of composite sulfur hosts, synergizing unique shuttling suppression functionalities of multiple constituent components, proves to be a promising strategy for development of advanced LSBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13818–13830"},"PeriodicalIF":5.5,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsaem.5c02205","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104134","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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":"Combined Experimental and Computational Analysis of Lithium Diffusion in Isostructural Pair VNb9O25 and VTa9O25","authors":"Manish Kumar,&nbsp;, ,&nbsp;Md Abdullah Al Muhit,&nbsp;, ,&nbsp;CJ Sturgill,&nbsp;, ,&nbsp;Nima Karimitari,&nbsp;, ,&nbsp;John T. Barber,&nbsp;, ,&nbsp;Hunter Tisdale,&nbsp;, ,&nbsp;Morgan Stefik*,&nbsp;, ,&nbsp;Hans-Conrad zur Loye*,&nbsp;, and ,&nbsp;Christopher Sutton*,&nbsp;","doi":"10.1021/acsaem.5c01738","DOIUrl":"https://doi.org/10.1021/acsaem.5c01738","url":null,"abstract":"<p >The increasing demand for fast charging batteries has motivated the search for materials with improved transport characteristics. Wadsley–Roth crystal structures are an attractive class of materials for batteries because fast lithium diffusion is facilitated by the ReO₃-like block structure, with electron transport enabled by edge-sharing along the shear planes. However, a clear understanding of structure–property relationships remains limited, making it challenging to develop improved materials within this class of promising compounds. Here, the first lithiation of VTa₉O₂₅ is reported, enabling a direct isostructural comparison with the better-known VNb₉O₂₅. These materials have similar atomic radii and unit cell volumes yet exhibit different voltage windows, C-rate-dependent capacities, and transport metrics. Time-dependent overpotential analysis revealed ionic diffusion as the primary bottleneck to high-rate performance in both cases. However, the corresponding lithium diffusivity for VNb₉O₂₅ was an order of magnitude faster than that for VTa₉O₂₅. These experimental trends aligned well with density functional theory calculations combined with molecular dynamics that show a factor of 7 faster diffusion in VNb₉O₂₅ compared to VTa₉O₂₅. Nudged elastic band calculations of the probable hopping pathways indicate that VNb₉O₂₅ consistently exhibits a lower activation barrier for lithium diffusion than VTa₉O₂₅, which can be attributed to the larger net charge transfer during Li hopping in VNb₉O₂₅. DFT calculations indicate that the structures show only a small overall volume change of about 6% across lithiation, with little structural difference between VNb₉O₂₅ and VTa₉O₂₅. In contrast, the electronic structures differ, with VNb₉O₂₅ undergoing an insulator–to–metal transition at a state of charge lower than that of VTa₉O₂₅. Overall, the results indicate that the choice of cation (Nb or Ta) influences the electronic and transport properties during lithiation.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13407–13420"},"PeriodicalIF":5.5,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104130","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tungsten Carbide Nano Sponge: A Dual-Application Material for Lithium-Ion Batteries and Supercapacitors","authors":"Jeyakiruba Palraj,&nbsp; and ,&nbsp;Helen Annal Therese*,&nbsp;","doi":"10.1021/acsaem.5c01421","DOIUrl":"https://doi.org/10.1021/acsaem.5c01421","url":null,"abstract":"<p >Tungsten carbide (WC) has emerged as a promising material for advanced lithium-ion batteries (LIBs) and supercapacitor technologies owing to its remarkable intrinsic properties. This study reports the synthesis of porous tungsten carbide (WC) via a simple and efficient solid-state route to obtain a phase-pure WC nanosponge (WC-NS) with a unique nanostructured morphology that enhances electrochemical performance, making it a promising electrode material for LIBs and supercapacitors. The WC-NS was characterized using X-ray diffraction, high-resolution scanning electron microscopy (HRSEM), high-resolution transmission electron microscopy (HRTEM), and X-ray photoelectron spectroscopy (XPS) to elucidate its structural and compositional attributes. As an LIB anode, it delivered an initial specific capacity of 454 mA h/g at 1000 mA/g, retaining 244 mA h/g after 200 cycles with 99.9% Coulombic efficiency. In supercapacitor applications, WC-NS demonstrated outstanding electrochemical performance, achieving 334 F/g at 1 A/g and 102 F/g at 8 A/g, while maintaining 98% retention over 5000 cycles with 100% Coulombic efficiency. A symmetric WC-NS supercapacitor exhibited a capacitance of 300 F/g at 0.8 A/g, 98% retention over 20,000 cycles, a maximum power density of 3600 W/kg, and an energy density of 30 Wh/kg. The comprehensive post-mortem analyses of WC confirm its stable nanoporous structure without any noticeable degradation even after prolonged cycling in both LIBs and supercapacitor. These results demonstrate the exceptional versatility and promise of WC as a next-generation multifunctional material for cutting-edge energy storage applications.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13288–13305"},"PeriodicalIF":5.5,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104110","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Interplay of Polymorphism in FeS2 Thin Films by Phosphorus Doping","authors":"Dipta Suryya Mahanta,&nbsp;, ,&nbsp;Rudra Narayan Chakraborty,&nbsp;, ,&nbsp;Sethuraman Divagar,&nbsp;, ,&nbsp;Rajalingam Thangavel,&nbsp;, and ,&nbsp;Kasilingam Senthilkumar*,&nbsp;","doi":"10.1021/acsaem.5c01890","DOIUrl":"https://doi.org/10.1021/acsaem.5c01890","url":null,"abstract":"<p >Achieving <i>p</i>-type pyrite FeS₂ is essential for its effective use in thin film photovoltaics. Phosphorus (P) is emerging as a prominent anionic dopant in pyrite to induce <i>p</i>-type electrical conductivity. This study investigates the impact of P doping on the structural and electrical characteristics of pyrite thin films. Films are fabricated using DC magnetron sputtering, initially yielding sulfur (S)-poor FeS_2–<i>x</i> phase. Annealing in S atmosphere yields phase-pure pyrite, while coannealing with higher P introduces mixed pyrite-marcasite phase <i>p</i>-type conductivity. An Increasing of band gap from 1.08 to 1.43 eV is also observed, with high hole mobility of 150.62 cm² V^–1 s^–1. P integration in FeS₂ is confirmed by X-ray photoelectron spectroscopy (XPS) via P–S and Fe–P binding energies. The mixed pyrite-marcasite phase is confirmed by Raman results. This mixed phase <i>p</i>-type FeS₂ can help increase the photovoltaic performance. However, it also shows excessive doping causing nonuniformity and contact behavior.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13519–13528"},"PeriodicalIF":5.5,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104142","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-Dielectric Ultrathin BaTiO3 Anode via Electrophoretic Deposition: A Platform for Pseudocapacitive Li Storage and Interface Stabilization","authors":"Ji-Yeon Lee,&nbsp;, ,&nbsp;Jiwon Shin,&nbsp;, ,&nbsp;Minsu Heo,&nbsp;, ,&nbsp;Chanyoung Yoo,&nbsp;, ,&nbsp;Mincheol Chang,&nbsp;, ,&nbsp;Jedo Kim,&nbsp;, ,&nbsp;Hyun-Sik Kim*,&nbsp;, and ,&nbsp;Byoung-Nam Park*,&nbsp;","doi":"10.1021/acsaem.5c01550","DOIUrl":"https://doi.org/10.1021/acsaem.5c01550","url":null,"abstract":"<p >We report the development of an ultrathin barium titanate (BaTiO₃, BTO) anode fabricated via alternating current electrophoretic deposition (AC-EPD), enabling an interface-sensitive platform for Li-ion batteries (LIBs). The additive-free design without conductive agents or binders allows direct probing of the intrinsic electrochemical behavior of BTO. Owing to its high dielectric constant, BTO generates a uniform internal electric field at the electrode–electrolyte interface, effectively suppressing localized field fluctuations and minimizing parasitic side reactions. This interface-stabilizing effect is especially advantageous for lithium metal systems, where controlling interfacial reactivity is critical for long-term performance. Beyond its role as a stable interfacial layer, BTO exhibits significant pseudocapacitive charge storage with a <i>b</i> value of 0.83 and high Li ion diffusivity (1.3 × 10^–8 cm² s^–1), indicating its dual function as a Li ion storage medium and a Li ion-permeable passivation layer. The ultrathin BTO anode demonstrates excellent high-rate capability at a current density of 1 A g^–1. These results establish BTO as a multifunctional material capable of enhancing both energy storage and interfacial stability in next-generation LIBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13278–13287"},"PeriodicalIF":5.5,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104109","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enabling High-Performance Li-Rich Single-Crystalline Cathode via Mo-Doping","authors":"Li Xie,&nbsp;, ,&nbsp;Lei Wu,&nbsp;, ,&nbsp;Hao Ding,&nbsp;, ,&nbsp;Ruijuan Wang,&nbsp;, ,&nbsp;Shuang Cao,&nbsp;, ,&nbsp;Yunfeng Lu,&nbsp;, ,&nbsp;Li Yang*,&nbsp;, ,&nbsp;Hong Liu*,&nbsp;, and ,&nbsp;Xianyou Wang*,&nbsp;","doi":"10.1021/acsaem.5c01387","DOIUrl":"https://doi.org/10.1021/acsaem.5c01387","url":null,"abstract":"<p >Although Li-rich layered oxides (LLOs) can achieve high capacity (&gt;300 mAh g^–¹) and thereby enhance energy density of Li-ion battery cathodes, they encounter persistent challenges, including low initial Coulombic efficiency (ICE), poor cycling performance, and bad rate capability. In the present study, the layered–spinel heterostructure is constructed on the surface of single-crystalline LLO materials by Mo doping with a facile sol–gel method. The Li-rich layered–spinel heterostructure can provide 3D Li-ion channels and restrain the growth of the SEI film and oxygen release. Additionally, the larger ionic radius of Mo⁶⁺ also can contribute to enhancing the discharge specific capacity and improving Li⁺ diffusion kinetics. Benefiting from these collaborative contributions of solid oxygen framework and unique layered–spinel heterostructure, the as-prepared material shows good electrochemical properties, including a high ICE of 93.44%, an outstanding initial discharge specific capacity of 302.01 mAh g^–1, an excellent capacity retention of 92.55% after 100 cycles under 1 C, and a remarkable rate capability.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13253–13263"},"PeriodicalIF":5.5,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104111","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Modulation of Zn2+ Solvation Structure and Deposition Behavior to Achieve High-Performance Zn Anodes","authors":"Ge Xue,&nbsp;, ,&nbsp;Haifeng Bian,&nbsp;, ,&nbsp;Biao Wang,&nbsp;, ,&nbsp;Qing Zhou,&nbsp;, ,&nbsp;Shunshun Jia,&nbsp;, ,&nbsp;Yujie Ma,&nbsp;, ,&nbsp;Jian Gu,&nbsp;, and ,&nbsp;Xiangkang Meng*,&nbsp;","doi":"10.1021/acsaem.5c01994","DOIUrl":"https://doi.org/10.1021/acsaem.5c01994","url":null,"abstract":"<p >Aqueous zinc-ion batteries (AZIBs) have gained wide attention as a promising next-generation energy storage solution, owing to their inherent safety, eco-friendliness, and exceptional volumetric capacity (5855 mAh cm^–3). However, the severe dendrite formation and side reactions of the Zn anode have impeded the development of AZIBs. Herein, a low-cost, easy-to-handle, and efficient small-molecule electrolyte additive, 1-Methoxy-2-propanol (PM), is employed to address these issues. The multifunctional additive can inhibit side reactions by disrupting the electrolyte’s hydrogen-bonding network and adjusting the solvated structure of Zn²⁺. Additionally, it can induce the preferential orientation deposition of Zn(002) on the surface of the Zn anode. It is worth mentioning that the PM-modified electrolyte enables the Zn||Zn symmetric cell to achieve an ultralong cycling stability of 2400 h (1 mA cm^–2, 1 mAh cm^–2) and 3000 h (5 mA cm^–2, 1 mAh cm^–2), while the Zn||Cu asymmetric cell maintains a high average Coulombic efficiency of 99.49% over 650 cycles (5 mA cm^–2, 1 mAh cm^–2). In addition, compared to the ZnSO₄ electrolyte, the full cell using the PM modified electrolyte exhibits higher capacity retention. This study provides a strategic approach to designing multifunctional electrolyte additives for high-performance AZIBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13653–13662"},"PeriodicalIF":5.5,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104112","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}