ACS Applied Energy Materials最新文献

{"title":"Hierarchical Co-CNT@NG Composite with Enhanced Polysulfide Kinetics in High-Performance Li–S Batteries","authors":"Chao Ma,&nbsp;Ji-Jun Dong,&nbsp;Xue-Yan Wu*,&nbsp;Liang-Yu Wang,&nbsp;Jing-Zhe Wan and Kai-Xue Wang*,&nbsp;","doi":"10.1021/acsaem.5c02085","DOIUrl":"https://doi.org/10.1021/acsaem.5c02085","url":null,"abstract":"<p >Lithium–sulfur (Li–S) batteries are considered promising candidates for next-generation energy storage systems due to their high theoretical energy density. However, their practical application is severely hindered by the polysulfide shuttle effect and the sluggish redox kinetics of lithium polysulfides (LiPSs). To address these challenges, a polypropylene (pp) separator was modified with Co-CNT@NG, a composite prepared by integrating cobalt-embedded carbon nanotubes (Co-CNTs) onto nitrogen-doped expanded graphite (NG). This three-dimensional hierarchical composite enables the simultaneous physical confinement and strong chemical adsorption of LiPSs, effectively suppressing the shuttle effect. The embedded cobalt nanoparticles and doped nitrogen atoms synergistically promote the conversion of LiPS. The conductive 3D framework ensures fast electron transfer and reduces interfacial resistance. As a result, Li–S batteries with the Co-CNT@NG/pp separator deliver superior electrochemical performance, including a high initial discharge capacity of 1346 mAh g^–¹ at 0.1 C, outstanding rate capability with 771 mAh g^–¹ at 6 C, and long-term cycling stability over 500 cycles at 0.5 C with nearly 100% Coulombic efficiency under a high sulfur loading of 8.0 mg cm^–². This work provides an effective strategy for enhancing the kinetic conversion of LiPSs in Li–S batteries through the rational design of a 3D hierarchical catalytic structure.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12878–12886"},"PeriodicalIF":5.5,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007401","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-Voltage Induced Stable Interface Promoting Electrochemical Performance for Halide-Based All-Solid-State Batteries","authors":"Jialong Shi,&nbsp;, ,&nbsp;Yunhao Zhu,&nbsp;, ,&nbsp;Jing Wang,&nbsp;, ,&nbsp;Mansoor Khan,&nbsp;, ,&nbsp;Fanghua Ning*,&nbsp;, ,&nbsp;Xiaoyu Liu,&nbsp;, ,&nbsp;Shigang Lu,&nbsp;, and ,&nbsp;Jin Yi*,&nbsp;","doi":"10.1021/acsaem.5c02238","DOIUrl":"https://doi.org/10.1021/acsaem.5c02238","url":null,"abstract":"<p >Halide-based solid-state electrolytes (SSEs) exhibit favorable ionic conduction with wide electrochemical windows, yet their practical applications are significantly constrained by the interfacial instability between the electrolyte and cathode. In this work, the compatibility and interaction mechanisms between Li₃InCl₆ (LIC) and single-crystal LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cathode material at high voltage have been in-depth investigated. It has been found that spontaneous delithiation can be triggered via direct contact between LIC and NCM811, leading to capacity degradation. However, at a high voltage of 4.7 V, the proposed LIC-based all-solid-state battery presents exceptional cycling stability with 84.7% capacity retention after 200 cycles, outperforming that of 70.8% retention at 4.4 V. The oxidation of LIC at 4.7 V triggers a self-limiting side reaction, leading to the formation of a well-adhered cathode-electrolyte interphase (CEI) through interfacial oxygen scavenging, which suppresses further side reactions and enhances interfacial electrochemical stability. This work provides fundamental insights for designing high-voltage all-solid-state batteries (ASSBs) and advances research on cathode-electrolyte compatibility.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13894–13901"},"PeriodicalIF":5.5,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104082","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":"Unveiling the Nickel–Manganese Sulfide Electrocatalyst for Enhanced Overall Alkaline Water Splitting","authors":"Harshini Sharan,&nbsp;, ,&nbsp;Angappan Kausalya,&nbsp;, ,&nbsp;Senthilkumar Lakshmipathi,&nbsp;, ,&nbsp;Jayachandran Madhavan,&nbsp;, ,&nbsp;Pavithra Karthikesan,&nbsp;, and ,&nbsp;Alagiri Mani*,&nbsp;","doi":"10.1021/acsaem.5c02072","DOIUrl":"https://doi.org/10.1021/acsaem.5c02072","url":null,"abstract":"<p >Harnessing earth-abundant electrocatalysts for efficient water splitting is a key pursuit in the development of sustainable energy technologies. In this study, plate-like Nickel–manganese sulfide (NMS) was in situ grown on nickel foam, via a simple one-step hydrothermal approach, yielding a binder free electrocatalyst. The synergistic interplay between Ni and Mn in the sulfide matrix, combined with the conductive substrate, endows NMS with an exceptional bifunctional activity for overall water splitting in an alkaline medium. The NMS-based electrolyzer delivers a low cell voltage of 1.69 V at 10 mA/cm² and presents a remarkable stability over 150 h under 1 M KOH electrolyte. Notably, theoretical studies from density functional theory (DFT) strongly reinforce the experimental findings, highlighting NMS as a highly efficient bifunctional electrocatalyst. Thus, the viability of this system is positioned as a promising and scalable alternative to precious metal-based electrocatalysts.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13752–13762"},"PeriodicalIF":5.5,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104054","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":"Controlled Synthesis of Fe3N Sandwiched in Nitrogen-Doped Multilayer Graphene as an Anode Material for Lithium-Ion Batteries","authors":"Ming-Yang Zhao,&nbsp;Feng-Ming Liu,&nbsp;Ming Chen*,&nbsp;Xing Zhang,&nbsp;Xing Qian,&nbsp;Zhong-Yong Yuan,&nbsp;Rong Wan,&nbsp;Chun-Sheng Li and Wen-Xue Yue,&nbsp;","doi":"10.1021/acsaem.5c01871","DOIUrl":"https://doi.org/10.1021/acsaem.5c01871","url":null,"abstract":"<p >Iron nitride, with a high theoretical capacity and excellent electrical conductivity, has emerged as a promising high-rate anode material for lithium-ion batteries (LIBs). However, its commercial viability is still hindered by poor cycling stability resulting from severe volume changes upon cycling. To address this shortcoming, Fe₃N/N-doped multilayer graphene (Fe₃N/N-mG) was prepared by Fe-catalyzed graphitization of phenanthrene and a post-nitridation process. The well-dispersed Fe₃N nanocrystals, with a size of <i>ca</i>. 5–10 nm, were spatially sandwiched in the N-doped multilayer graphene with a controlled thickness of 3.5–10 nm and open pore channels, showing abundant accessible active sites, robust structural stability, and high electron/Li⁺ transportation ability (2.1 S cm^–1, 2.39 × 10^–12 cm² s^–1) when used as anode materials in LIBs. The optimum Fe₃N/N-mG delivered exceptional capacities of 590 mA h g^–1 at 0.1 C and 412 mA h g^–1 at 5 C after 30 cycles, and a capacity retention of 530 mA h g^–1 at 0.1 C after 600 cycles, surpassing the pure Fe₃N, graphene, and many previously reported metal–nitride-based anodes. This work offers an in situ metal catalysis of polycyclic aromatic hydrocarbons and a subsequent post-nitridation strategy for the facile preparation of high-performance metal nitride/graphene electrodes for LIBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12769–12779"},"PeriodicalIF":5.5,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007414","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":"Carbon-Coated MgFeSiO4/Graphene Conductive Network Cathode Enables Ultrahigh-Rate and Long-Cycle-Life Magnesium-Ion Batteries","authors":"Jie Xu,&nbsp;, ,&nbsp;Xirui Lu,&nbsp;, ,&nbsp;Yuqi Hong,&nbsp;, ,&nbsp;Liuyan Xia,&nbsp;, ,&nbsp;Jili Yue*,&nbsp;, ,&nbsp;Shuming Dou,&nbsp;, ,&nbsp;Xuxi Teng,&nbsp;, ,&nbsp;Guangsheng Huang*,&nbsp;, ,&nbsp;Yanan Chen*,&nbsp;, ,&nbsp;Jingfeng Wang,&nbsp;, and ,&nbsp;Fusheng Pan,&nbsp;","doi":"10.1021/acsaem.5c01683","DOIUrl":"https://doi.org/10.1021/acsaem.5c01683","url":null,"abstract":"<p >Rechargeable magnesium ion batteries (RMBs) have garnered intense interest as a promising energy-storage system due to their high safety. However, developing high-performance cathodes with rapid kinetics is a crucial challenge for advanced RMBs. Herein, an <i>in situ</i>-constructed carbon layer and graphene conductive network structure are proposed to modify the MgFeSiO₄ cathode material (denoted as MgFeSiO₄/C@G). As expected, the synthesized MgFeSiO₄/C@G exhibits high magnesium storage capacities (219.6 mAh g^–1 after 250 cycles at 0.5 C), superior high-rate performance (97.5 mAh g^–1 at 50 C), and long-term cycling stability (a specific capacity of 90.88 mAh g^–1 after 5000 cycles at 30 C with ∼85% capacity retention). Remarkably, the outstanding stability, 93.5% capacity retention at 5 C after 1700 cycles at 50 °C, further affirms the high-temperature adaptability and reliability of MgFeSiO₄/C@G. Moreover, the synthesized MgFeSiO₄/C@G has a small volume change (only 0.24%) during magnesium insertion–extraction, which ensures a prolonged cycle life. The stable integration between MgFeSiO₄ and distinctive conductive network architecture shortens the ion diffusion path, promotes electron transfer, enhances Mg²⁺ diffusion kinetics, and achieves excellent structural stability during the cycling.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13367–13376"},"PeriodicalIF":5.5,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104055","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":"Effective Strategy to Develop a Metal-Free Nitrogen-Doped Carbon with Abundant Intrinsic Carbon Defects for Electrochemical CO2 Reduction","authors":"Ryuji Takada*,&nbsp;, ,&nbsp;Kotaro Narimatsu,&nbsp;, ,&nbsp;Koji Miyake*,&nbsp;, ,&nbsp;Yoshiaki Uchida,&nbsp;, and ,&nbsp;Norikazu Nishiyama,&nbsp;","doi":"10.1021/acsaem.5c01071","DOIUrl":"https://doi.org/10.1021/acsaem.5c01071","url":null,"abstract":"<p >For the practical application of carbon dioxide electrochemical reduction reaction (CO₂RR), developing efficient metal-free carbon-based electrocatalysts is extremely important. To date, various heteroatom-doped carbon materials for CO₂ reduction have been synthesized. Even though intrinsic carbon defects are expected to tune the electrocatalytic activity of carbon materials such as heteroatom doping, the role of intrinsic carbon defects has received little attention. Furthermore, it is still challenging to controllably introduce intrinsic carbon defects into a carbon matrix at high density. In this work, a rational strategy to fabricate the high-density intrinsic carbon defects is provided by the sequential processes of the evaporation of atomically dispersed Zn and the removal of pyridinic N species at a pore edge from a single-atom Zn catalyst derived from a carbonized metal–organic framework. From the controlled experimental results, the removal of Zn–N_<i>x</i> can lead to creating the abundant intrinsic carbon defects into the carbon matrix. The optimized defective N-doped carbon materials (DNC-1200-L) exhibited excellent electrocatalytic activity, with a Faradaic efficiency (FE_CO) of 93.0% for CO generation. Notably, DNC-1200-L displayed a high-plateau FE_CO over 90.0% under the potential range from −0.6 to −0.9 V vs RHE. This study offers a simple and effective strategy for developing carbon-based electrocatalysts with high-density intrinsic carbon defects to selectively enhance the CO₂RR into CO.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13231–13238"},"PeriodicalIF":5.5,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104052","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":"In-Depth Understanding of Cycling Degradation Mechanisms in Lithium Metal Batteries","authors":"Xiong Xiao,&nbsp;Zicen Deng,&nbsp;Yan Liu,&nbsp;Zhenwei Zhu,&nbsp;Xiukang Yang* and Hao Zhang*,&nbsp;","doi":"10.1021/acsaem.5c01344","DOIUrl":"https://doi.org/10.1021/acsaem.5c01344","url":null,"abstract":"<p >Lithium metal batteries (LMBs) are widely recognized for their substantial advantages in energy density, but their cycle life and safety still face the challenges of lithium dendrites and the generation of dead lithium, which limit their practical applications. LMBs experience dramatic volume changes during charge and discharge cycles, thereby requiring external pressure to ensure normal operation. Additionally, the charge and discharge conditions equally influence their self-generated pressure. To better understand the degradation mechanisms of LMBs, we analyzed the intricate correlation between external pressure, charge–discharge rates, and cycle life of LMBs based on recent literature. Using a 420 Wh/kg (9.8 Ah) LMB pouch cell, we conducted long-term cycling tests under various charge–discharge rates. After 710 cycles at 0.2C-3C rates, the capacity retention remained as high as 91%. Furthermore, through in situ high-resolution pressure sensing, we measured the expansion force of the lithium metal pouch cell under slow charge/fast discharge and fast charge/slow discharge conditions. Applying appropriate external pressure in combination with slow charge/fast discharge can effectively mitigate battery volume changes and enhance cycle life.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12452–12459"},"PeriodicalIF":5.5,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007381","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":"Co(1–x–y)FexZny-Glycerolate Microspheres as Electrocatalysts for the Oxygen Evolution Reaction","authors":"Mesaque C. França,&nbsp;Irlan S. Lima,&nbsp;Alireza Ghorbani,&nbsp;Reza Shahbazian-Yassar,&nbsp;Iranaldo S. da Silva,&nbsp;Auro A. Tanaka,&nbsp;Lúcio Angnes*,&nbsp;Josué M. Gonçalves* and Pedro de Lima-Neto*,&nbsp;","doi":"10.1021/acsaem.5c01604","DOIUrl":"https://doi.org/10.1021/acsaem.5c01604","url":null,"abstract":"<p >Coordination compounds based on transition metals have attracted significant attention for electrocatalyst applications due to their tunable composition and excellent properties as electrode materials. Herein, the design of ternary CoFeZn-glycerolate (CoFeZn-Gly) as an efficient electrocatalyst for oxygen evolution reaction (OER) in an alkaline medium is reported. The combination of Co, Fe, and Zn in the generated microspheres, approaching equimolar conditions, was noted to tend to generate aggregated spheres with an average size of ∼306 nm. The optimized CoFeZn-Gly OER electrocatalyst showed an overpotential of 335 mV (at a current density of 10 mA cm^–2) and a Tafel slope of 37.2 mV dec^–1, having the glassy carbon electrode (GCE) as a substrate. Further, the ternary electrocatalyst delivered good stability with a potential retention of 99.22% after 24 h of chronopotentiometry collected at 10 mA cm^–2, in a 1.0 M KOH electrolyte.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12618–12626"},"PeriodicalIF":5.5,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsaem.5c01604","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007394","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":"Large-Area Flexible Organic Charge-Transfer Cocrystal Membranes for Photothermal and Photothermoelectric Conversion with Excellent Durability","authors":"Guan Wang,&nbsp;Yongyi Zhang,&nbsp;Tao Jin,&nbsp;Lei Yao,&nbsp;Jiacheng Zhang,&nbsp;Jing Zhang* and Peng Sheng*,&nbsp;","doi":"10.1021/acsaem.5c02140","DOIUrl":"https://doi.org/10.1021/acsaem.5c02140","url":null,"abstract":"<p >Organic photothermal materials with superior capabilities in green and sustainable energy conversion have attracted significant attention due to their simple processability, flexibility, and good biocompatibility. Nevertheless, their practical applications are limited by complex synthesis and difficulties in forming large-area films. Here, we report a photothermal charge-transfer cocrystal composed of benzo[<i>c</i>]carbazole (BCZ) and tetracyanoquinodimethane (TCNQ), self-assembled via a simple solution-evaporation method. This cocrystal achieves a high photothermal conversion efficiency (PCE) of ∼71% under 808 nm irradiation. Furthermore, large-area BCZ-TCNQ membranes can be conformally coated onto various substrates using a bar-coating technique, serving as flexible heat sources with excellent durability. By integrating the organic cocrystal with thermoelectric devices under 1 sun irradiation, the photothermoelectric system produces an excellent output voltage of 0.22 V and a power density of 5.5 W m^–2. This work demonstrates the potential of organic cocrystals for outdoor power generation through solar-thermal-electric energy conversion.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12952–12959"},"PeriodicalIF":5.5,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007387","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":"Operation of MXene-Derived Zinc-Preintercalated Bilayered Vanadium Oxide Cathode in Aqueous Zn-Ion Batteries","authors":"Timofey Averianov,&nbsp;Kyle Matthews,&nbsp;Xinle Zhang,&nbsp;Huyen T. K. Nguyen,&nbsp;Yuan Zhang,&nbsp;Yury Gogotsi and Ekaterina Pomerantseva*,&nbsp;","doi":"10.1021/acsaem.5c01721","DOIUrl":"https://doi.org/10.1021/acsaem.5c01721","url":null,"abstract":"<p >Layered hydrated vanadium oxides, particularly those with bilayered structures, show remarkable electrochemical performance as cathodes for aqueous Zn-ion batteries (AZIBs). However, their wide-scale adoption is hindered by limited understanding of their charge storage mechanisms in different Zn-containing electrolytes. Here, we demonstrate the first synthesis of a MXene-derived Zn-preintercalated bilayered vanadium oxide (MD-ZVO) with a nanoflower-like morphology comprised of two-dimensional (2D) nanosheets, achieved via a two-step dissolution–recrystallization process. The strategic Zn²⁺ preintercalation establishes well-defined ion diffusion pathways, while the nanoflower-like assembly of 2D nanosheets enhances structural integrity, together contributing to improved electrochemical performance over other layered vanadium oxides. A systematic evaluation of four electrolytes (2 M ZnSO₄, 2.6 M Zn(OTf)₂, 2 M ZnCl₂, and 30 m ZnCl₂) showed that MD-ZVO electrodes delivered high reversible capacities (450 and 315 mAh g^–1 at 0.1 A g^–1), excellent rate capability (223 mAh g^–1 for both electrolytes at 1.0 A g^–1), and good electrochemical stability (84% and 48% over 1000 cycles at 1.0 A g^–1) in saturated 2.6 M Zn(OTf)₂ and highly concentrated 30 m ZnCl₂, respectively. The material’s superior electrochemical stability in concentrated electrolytes is attributed to suppressed vanadium oxide dissolution during cycling. <i>In situ</i> and <i>ex situ</i> XRD analyses of MD-ZVO electrodes reveal larger contribution of Zn²⁺-associated species for charge storage in cells containing 2.6 M Zn(OTf)₂ and proton dominant charge transfer in cells containing 30 m ZnCl₂. Additionally, the combination of <i>in situ</i> and <i>ex situ</i> characterization demonstrates the reversible formation of Zn_<i>x</i>OTf_<i>y</i>(OH)_{2<i>x</i>–<i>y</i>}·<i>n</i>H₂O in cells using 2.6 M Zn(OTf)₂ and Zn₅(OH)₈Cl₂·H₂O in cells using 30 m ZnCl₂ on the MD-ZVO electrode surface over extended cycling. This work highlights the superior performance of nanoflower MD-ZVO for cathodes in aqueous Zn-ion batteries, which benefits from the proper selection of highly concentrated electrolytes that enable better utilization of the cathode material.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12695–12711"},"PeriodicalIF":5.5,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsaem.5c01721","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007412","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}