ACS Applied Energy Materials最新文献

{"title":"Carbon-Supported Cobalt–Nickel Phosphide as a High-Performance Electrocatalyst for the Efficient Overall Water Splitting","authors":"Manju Bhargavi Gumpu*,&nbsp; and ,&nbsp;Ramasamy Karvembu,&nbsp;","doi":"10.1021/acsaem.5c01390","DOIUrl":"https://doi.org/10.1021/acsaem.5c01390","url":null,"abstract":"<p >The need for sustainable energy has driven the development of low-cost electrocatalysts for water splitting, which is a key step in the production of hydrogen. Herein, we report a bifunctional carbon-supported cobalt–nickel phosphide catalyst, which has shown excellent catalytic performance in both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), making it a promising candidate for renewable energy technology. The synthesis involves the controlled heating of cobalt, nickel, and phosphorus precursors in the presence of citric acid in a tubular furnace under a nitrogen atmosphere. The resultant carbon-supported cobalt–nickel phosphide (Co–Ni₅P₄/C) exhibits excellent functionalities as an electrocatalyst toward HER and OER with low overpotentials of 95 and 153 mV at 10 mA cm^–2, respectively, in 1 M KOH alkaline electrolyte. The synergy between cobalt and nickel in the phosphide phase, coupled with the conducting carbon support, enhanced electron transfer kinetics and promoted efficient water splitting. The bifunctional Co–Ni₅P₄/C requires a small voltage of 1.8 V at 50 mA cm^–2 for the overall splitting of water. Carbon-supported cobalt–nickel phosphide holds significant promise for advancing renewable hydrogen production technology, offering a pathway toward sustainable and clean energy solutions.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13264–13277"},"PeriodicalIF":5.5,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104010","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":"Lanthanide-Driven Li+/H+ Exchange for High Proton Conductivity in Li13.9Sr0.1Zn(GeO4+δ)4 Electrolyte for Proton-Conducting Ceramic Fuel Cells","authors":"Xian Pan,&nbsp;, ,&nbsp;Peilin Ding,&nbsp;, ,&nbsp;Xin Zhou,&nbsp;, ,&nbsp;Huiping Yang,&nbsp;, ,&nbsp;Tao Li,&nbsp;, ,&nbsp;Dongxu Cui,&nbsp;, ,&nbsp;Shiliang Wu*,&nbsp;, and ,&nbsp;Rui Xiao,&nbsp;","doi":"10.1021/acsaem.5c01918","DOIUrl":"https://doi.org/10.1021/acsaem.5c01918","url":null,"abstract":"<p >Developing advanced electrolytes is crucial for intermediate-temperature proton-conducting ceramic fuel cells (IT-PCFCs). Li_13.9Sr_0.1Zn(GeO_4+δ)₄ is a lithium conductor exhibiting outstanding Li⁺ conductivity. Its nonframework and interstitial Li⁺ can be reversibly exchanged with H⁺, thereby creating migration pathways for H⁺ transport. This study utilizes a Li⁺/H⁺ ion-exchange strategy to convert the Li⁺ conductor Li_13.9Sr_0.1Zn(GeO_4+δ)₄ into a high-performance H⁺ electrolyte. Lanthanide doping is further employed to enhance the H⁺ conduction capability. Li_13.8La_0.1Sr_0.1Zn(GeO_4+δ)₄ exhibits a proton conductivity of 0.067 S cm^–1 at 600 °C, surpassing most state-of-the-art proton conductors reported in the literature, and enables the electrolyte-supported single cell to achieve a peak power density of 0.42 W cm^–2. Structural and electrochemical characterization reveals that larger lanthanide ions effectively promote lattice expansion and Li⁺/H⁺ exchange, which directly correlates with improved electrochemical performance. The developed Li_13.8La_0.1Sr_0.1Zn(GeO_4+δ)₄ electrolyte offers superior proton conductivity and long-term stability, highlighting its significant potential as a next-generation electrolyte for IT-PCFCs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13549–13560"},"PeriodicalIF":5.5,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104017","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":"Multidimensional Design of Li Hosts for Li–Metal Batteries: Limitations and Future Directions","authors":"Ho Won Kang,&nbsp;, ,&nbsp;Joo An Bang,&nbsp;, ,&nbsp;Seung Woo Shin,&nbsp;, ,&nbsp;Yeong Mu Seo,&nbsp;, ,&nbsp;Jae Young Hwang,&nbsp;, ,&nbsp;Jinyoung Choi,&nbsp;, ,&nbsp;Gwangseok Oh,&nbsp;, ,&nbsp;Jin Hong Lee*,&nbsp;, and ,&nbsp;Byung Gon Kim*,&nbsp;","doi":"10.1021/acsaem.5c01996","DOIUrl":"https://doi.org/10.1021/acsaem.5c01996","url":null,"abstract":"<p >Li–metal batteries (LMBs) have been attracting enormous attention due to their superior performance and high theoretical energy density compared to conventional Li-ion batteries (LIBs). However, due to the uncontrollable Li dendrite growth, safety issues such as internal short circuits arise, which become more pronounced as the cell size increases or the operating conditions become harsh up to practical levels. Additionally, under high Li plating and stripping capacities, severe changes in anode thickness can lead to stability issues, and using a thick Li anode to ensure long-term cycling stability is not suitable for achieving high energy density in LMBs. As one of the strategies to address this problem, multidimensional conductive Li hosts with high surface areas have been investigated, as these structures can store Li inside the host framework, thereby mitigating volume changes during cycling. In this context, this review introduces recent strategies from a material perspective that have been conducted to form the host backbones using metals, carbon, and their hybrids. Then, we address structural design strategies to control the Li growth direction and stabilize the interface, and finally, we suggest host design insights considering energy densities that surpass those of LIBs to maximize the advantages of LMBs with Li hosts from a commercialization perspective. We hope that this review can motivate battery researchers to pave the way for the design of advanced Li hosts for high-performance and safe LMBs in the near future.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13122–13138"},"PeriodicalIF":5.5,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104031","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":"Highly Ordered rGO for Advanced Energy Storage Applications: Scalable and Cost-Effective Production","authors":"Krishnappagari Vijay Kumar,&nbsp;, ,&nbsp;Niranjan Pandit,&nbsp;, ,&nbsp;Rahul Kumar,&nbsp;, ,&nbsp;Patlolla Sai Kiran,&nbsp;, ,&nbsp;Satish Indupuri,&nbsp;, and ,&nbsp;Anup Kumar Keshri*,&nbsp;","doi":"10.1021/acsaem.5c01856","DOIUrl":"https://doi.org/10.1021/acsaem.5c01856","url":null,"abstract":"<p >Reduced graphene oxide (rGO) is emerging as a versatile material with outstanding potential in energy storage, sensors, and electronics due to its excellent conductivity and mechanical properties. For optimal stability and performance, rGO must be highly ordered to ensure efficient electron and ion transport. Despite the emergence of various reduction protocols for graphene oxide, their commercial viability is limited by high costs and low scalability for industrial applications. Here, we present a scalable thermal plasma spraying technique to reduce graphene oxide with a high production rate of 52 g/h at a very low cost of 4.36 USD/g. We achieved highly ordered rGO with a high carbon-to-oxygen ratio (C/O = 11.4), high specific surface area (198 m² g^–1), better electrical conductivity of 3288 S m^–1, thermal stability (600 °C), and low defect density (<i>I</i>_D/<i>I</i>_G = 0.18). The rGO showcased enhanced electrochemical properties, with a specific capacitance of 275 F g^–1 with 96% retention after 10,000 cycles for supercapacitors and a charge capacity of 182 mA h g^–1 for sodium-ion battery applications. This work introduces plasma spray as a cost-effective, scalable method for synthesizing highly ordered rGO, advancing energy storage technologies.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13476–13484"},"PeriodicalIF":5.5,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104025","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":"Interface-Engineered Co@Co3O4@NC Nanoparticles on BiVO4 Photoanodes for Efficient Charge Transfer and Solar Water Oxidation","authors":"Kaixin Zhang,&nbsp;, ,&nbsp;Zimu Li,&nbsp;, ,&nbsp;Yeqiang Wang,&nbsp;, ,&nbsp;Dajun Cui,&nbsp;, ,&nbsp;Jiangxin Wang,&nbsp;, ,&nbsp;Kuanhong Mei,&nbsp;, ,&nbsp;Minmin Liu,&nbsp;, ,&nbsp;Haoyang Dong,&nbsp;, ,&nbsp;Yiman Zhang,&nbsp;, ,&nbsp;Juan Zhang,&nbsp;, ,&nbsp;Weiguo Xu,&nbsp;, and ,&nbsp;Shuo Li*,&nbsp;","doi":"10.1021/acsaem.5c01883","DOIUrl":"https://doi.org/10.1021/acsaem.5c01883","url":null,"abstract":"<p >The employment of Co-based cocatalysts in BiVO₄ (BVO) photoanodes is still suffering from inefficient hole transfer to active sites and sluggish charge kinetic processes. To address this issue, we designed a hierarchical dual-shell Co@Co₃O₄@NC (Co-DS) cocatalyst synthesized via the controlled pyrolysis of CoCo Prussian blue analogs under micro-oxygen conditions. The designed hierarchical structure consists of a graphitic carbon shell that encases the Co₃O₄ interlayer, which is abundant in OER-active sites, coupled with a metallic Co core that enhances hole accumulation and charge transfer across interfaces. The optimized Mo-BVO/Co-DS photoanode achieves a photocurrent density of 4.95 mA/cm² at 1.23 V_RHE, representing a 129% enhancement over pristine BVO (2.16 mA/cm²). This work provides fundamental insights into the design principles of metal-oxide-based cocatalysts for overcoming efficiency limitations in photochemical water oxidation.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13510–13518"},"PeriodicalIF":5.5,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104074","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":"Dissolution-Equilibrium-Driven Synthesis of High-Quality K2Mn[Fe(CN)6] Cathode for High-Energy Potassium-Ion Batteries","authors":"Xunan Wang,&nbsp;, ,&nbsp;Chongwei Gao,&nbsp;, ,&nbsp;Shuhua Zhang,&nbsp;, ,&nbsp;Biao Zhang,&nbsp;, ,&nbsp;Baohua Li,&nbsp;, ,&nbsp;Feiyu Kang,&nbsp;, and ,&nbsp;Dengyun Zhai*,&nbsp;","doi":"10.1021/acsaem.5c02371","DOIUrl":"https://doi.org/10.1021/acsaem.5c02371","url":null,"abstract":"<p >Prussian blue analogues (PBAs), particularly high-energy K₂Mn[Fe(CN)₆] (MnPBA), are considered ideal candidates for cathodes of potassium-ion batteries (PIBs). However, conventional coprecipitation synthesis introduces uncontrollable structural defects, including [Fe(CN)₆]^4– vacancies and lattice water. These defects result from rapid crystal nucleation and growth, which leads to a significant deterioration in electrochemical performance. In this work, we propose a dissolution-equilibrium-driven synthesis strategy that effectively controls crystallization kinetics to synthesize high-quality MnPBA with minimal defects. This work offers a simple and controllable synthesis strategy for high-quality PBAs and emphasizes the importance of minimal defects in the improvement of the electrochemical performance of PBA cathodes.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13191–13197"},"PeriodicalIF":5.5,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104027","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":"Investigation of Structural and Electrochemical Modulation in NaFe0.5Co0.5O2 Cathode Material via Zn Substitution for Fe","authors":"Hoang Van Nguyen,&nbsp;, ,&nbsp;Thi Nhan Tran,&nbsp;, ,&nbsp;Minh Le Nguyen,&nbsp;, ,&nbsp;Quynh Nhu Nguyen,&nbsp;, ,&nbsp;Van Man Tran,&nbsp;, ,&nbsp;Phung M-L. Le*,&nbsp;, ,&nbsp;An-Giang Nguyen,&nbsp;, ,&nbsp;Phi Long Nguyen,&nbsp;, and ,&nbsp;Viet-Bac Thi Phung*,&nbsp;","doi":"10.1021/acsaem.5c01828","DOIUrl":"https://doi.org/10.1021/acsaem.5c01828","url":null,"abstract":"<p >Sodium-ion batteries are gaining attention as viable alternatives to lithium-ion systems, particularly for large-scale energy storage and cost-effective electric mobility. Advancing high-performance electrode materials, especially cathodes, is the key to driving their commercial viability. Among various strategies, cation doping has shown significant potential to tailor the structural and electronic properties of layered cathode materials, thereby influencing their electrochemical behavior. In this study, the effects of partial Fe³⁺ substitution in NaFe_0.5Co_0.5O₂ were examined by introducing 5% Zn²⁺ (yielding NaFe_0.45Zn_0.05Co_0.5O₂) and by increasing the Co content (NaFe_0.45Co_0.55O₂). The influence of these modifications on the crystal structure, Na⁺ diffusion kinetics, and cycling performance was systematically investigated to clarify the role of doping in tuning electrode properties. Structural analysis revealed that increasing the Co/Fe ratio led to lattice shrinkage along both the <i>a</i>- and <i>c</i>-axes and promoted cation disorder. These changes were associated with reduced capacity fading and a transition from a solid-solution voltage profile to a stepwise voltage profile. For galvanostatic charge–discharge testing, Zn doping in the NaFe_0.45Zn_0.05Co_0.5O₂ cathode enhanced both rate capability and cycling stability, particularly at 1C. This improvement was attributed to a higher Na⁺ diffusion coefficient within the sloping region of the P3 phase. The findings highlight the importance of optimizing redox-active species and structural integrity to improve the layered cathode performance. Zn doping was shown to effectively enhance structural stability and maintain a high capacity while boosting rate performance and long-term cycling durability under high-rate conditions.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13462–13475"},"PeriodicalIF":5.5,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104015","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":"Polythiophene Block Copolymer–Perylene Diimide-Based Electron Donor–Acceptor Double-Cable Polymer and Its Potential as an All-Organic Photocatalyst for Artificial Photosynthesis of H2O2","authors":"Faseeh Akbar,&nbsp;, ,&nbsp;Sana Iqbal,&nbsp;, ,&nbsp;Arwa Sohail,&nbsp;, ,&nbsp;Senem Çitoğlu,&nbsp;, ,&nbsp;Hatice Duran,&nbsp;, and ,&nbsp;Basit Yameen*,&nbsp;","doi":"10.1021/acsaem.5c02208","DOIUrl":"https://doi.org/10.1021/acsaem.5c02208","url":null,"abstract":"<p >Enhancing the light energy harvesting and conversion capabilities of all-organic photoactive materials is of significant scientific interest. Herein, we report the synthesis of a photoactive double-cable polymer (DCP) consisting of a polythiophene (PTh) block copolymer electron donor (D) conjugated to a perylene diimide (PDI) electron acceptor (A). GRIM polymerization and postsynthetic modifications are employed to synthesize the block copolymer [P3HT-<i>b</i>-poly(3-HT-co-PTh/PDI)] consisting of a poly-3-hexylthiophene (P3HT) block and a block comprising of randomly distributed repeat units bearing hexyl and PDI groups. Besides ¹H NMR, ATR-FTIR, UV/visible, and fluorescence spectroscopic characterizations, AFM and XRD analyses are performed to reveal self-assembly and crystallinity behaviors. Compared to P3HT, PDI, and their physical hybrid (P3HT–PDI-PH), the P3HT-<i>b</i>-poly(3-HT-co-PTh/PDI) shows superior D–A electronic communication, higher (photo)electrochemical current, faster electrochemical kinetics, and lower charge transfer resistance. The photocatalytic performance of all photocatalysts in the artificial photosynthesis of H₂O₂ is demonstrated over 10 photocatalytic cycles. Comparing the results from the highest H₂O₂ producing cycles, the photocatalytic performance of P3HT-<i>b</i>-poly(3HT-co-Th/PDI) is ∼2.1, ∼3.2, and ∼1.9 times superior compared to that of P3HT, PDI, and P3HT–PDI-PH, respectively. In summary, this work contributes to the development of organic semiconducting polymer-based photoactive materials for application in light energy harvesting and conversion technologies.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13861–13876"},"PeriodicalIF":5.5,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104147","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":"Enhancing Lithium-Ion-Battery Reliability through Weakly Solvating Molecule-Modified Carbonate Electrolytes","authors":"Piqiang Tan*,&nbsp;, ,&nbsp;Zhiyong Chen,&nbsp;, ,&nbsp;Xiang Liu,&nbsp;, ,&nbsp;Chaojie Yao,&nbsp;, and ,&nbsp;Ke Lu,&nbsp;","doi":"10.1021/acsaem.5c02362","DOIUrl":"https://doi.org/10.1021/acsaem.5c02362","url":null,"abstract":"<p >Ester-based electrolytes, characterized by their high dielectric constant and low viscosity, have become the dominant commercial choice for lithium-ion batteries (LIBs). However, conventional solvents such as ethylene carbonate (EC) and dimethyl carbonate (DMC) exhibit strong coordination with Li⁺ ions, leading to high desolvation energy barriers that limit the battery performance. In this study, we propose a modified electrolyte system based on commercial ester electrolytes by introducing weakly solvated solvents 1,2-dimethoxyethane (DME) or methyl acetate (MA). Through combined first-principles calculations and molecular dynamics simulations, we elucidate the atomic-scale mechanisms underlying the superior performance of DME and MA as solvent molecules. Experimental results demonstrate that the incorporation of DME significantly enhances the cycling stability, with Li–LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cells maintaining 80% capacity retention after 156 cycles at 4.3 V. This work provides fundamental insights for optimizing commercial LIB electrolytes and paves the way for developing next-generation electrolyte systems.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13198–13206"},"PeriodicalIF":5.5,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104090","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":"Atomic Layer Deposition of Nanoscale MoO3–x@ZnO Heterostructures for Kinetically Regulating Lithium Storage Behaviors","authors":"Xin Ji,&nbsp;, ,&nbsp;Jiyi Li,&nbsp;, ,&nbsp;Daxian Cao*,&nbsp;, ,&nbsp;Hangcheng Yang,&nbsp;, ,&nbsp;Chaohui Yuan,&nbsp;, ,&nbsp;Bin Zhao,&nbsp;, ,&nbsp;Dandan Ma,&nbsp;, ,&nbsp;Zhihui Li,&nbsp;, ,&nbsp;Jianwen Shi,&nbsp;, ,&nbsp;Yu Chen,&nbsp;, ,&nbsp;Yonghong Cheng,&nbsp;, ,&nbsp;Xiaogang Han,&nbsp;, ,&nbsp;Wenlei Liu*,&nbsp;, ,&nbsp;Hongkang Wang*,&nbsp;, and ,&nbsp;Xuan Lu*,&nbsp;","doi":"10.1021/acsaem.5c02186","DOIUrl":"https://doi.org/10.1021/acsaem.5c02186","url":null,"abstract":"<p >Metal oxides are considered among the most promising anode materials for next-generation lithium-ion batteries (LIBs) owing to their high theoretical capacities. Nevertheless, their practical application is hindered by intrinsic drawbacks, such as limited active sites, low electrical conductivity, and drastic volume variation during cycling. Rational construction of heterostructures offers a powerful strategy to overcome these limitations, but precise control at the nanoscale and a fundamental understanding of how heterostructures influence lithium storage behavior remain elusive. Herein, we report the atomic layer deposition (ALD)-enabled synthesis of two distinct MoO_3-<i>x</i>@ZnO heterostructures with controllable oxygen vacancies and tunable ZnO crystallinity. The underlying mechanism between the lithium storage behavior and the varied structures has been well revealed. A transition from amorphous ZnO (MoO_3-<i>x</i>@a-ZnO) to crystalline ZnO with a preferred (100) orientation (MoO_3-<i>x</i>@c-ZnO) leads to a shift in the dominant lithium storage mechanism─from pseudocapacitive behavior to diffusion-controlled processes. As a result, MoO_3-<i>x</i>@a-ZnO delivers a high specific capacity of 1016 mA h/g but suffers from rapid capacity fading, whereas MoO_3-<i>x</i>@c-ZnO exhibits delayed activation and gradually reaches 1035 mA h/g after prolonged cycling. This study provides critical insights into the structure–property relationships of oxide-based heterostructures and offers valuable guidance for the rational design of advanced metal oxide anodes for LIBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 18","pages":"13840–13850"},"PeriodicalIF":5.5,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145104016","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}