Advanced Energy Materials最新文献

{"title":"Dual Active Sites Decorated Tungsten Trioxide for Photocatalytic Methane Oxidation","authors":"Shanshan Qiu, Xiaoxin Liu, Jiacheng Liang, Yuping Wu, Lijuan Zhang, Wensheng Zhang, Yuheng Jiang, Dongxue Han, Yingying Fan, Li Niu, Zhiyong Tang","doi":"10.1002/aenm.202406119","DOIUrl":"https://doi.org/10.1002/aenm.202406119","url":null,"abstract":"Photocatalytic oxidation of methane to formaldehyde offers an appealing pathway for utilizing the abundant methane resource, nevertheless, suffering from poor formaldehyde formation rate and selectivity. Here, nickel cluster decorated tungsten trioxide of three high surface energy facets is prepared for photocatalytic methane oxidation to formaldehyde with yield rate of 3.27 mmol g⁻¹ h⁻¹, selectivity of 98.2% and turnover number of 20.65. The dual photohole centers of nickel cluster and lattice oxygen both could activate methane for selective formaldehyde formation. The lattice oxygen involves whole methane oxidation process on the catalyst surface based on an active site mechanism, while nickel cluster promotes formation of methyl radical and facilitates a radical mechanism in aqueous phase near the surface. These dual active sites provide an effective strategy to oxidize methane to formaldehyde under photoirradiation with water and oxygen gas.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"37 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837203","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Transport Kinetics: A New Perspective on Failure of Garnet Solid Electrolytes","authors":"Hua Guo, Yingshuai Wang, Min Fan, Ming-Yan Yan, Wen-Peng Wang, Xi-Xi Feng, Ya-Hui Wang, Dongmei Dai, Bao Li, Fawei Tang, Sen Xin, Hongcai Gao, Yu-Guo Guo","doi":"10.1002/aenm.202500367","DOIUrl":"https://doi.org/10.1002/aenm.202500367","url":null,"abstract":"Solid-state rechargeable lithium-metal batteries with garnet-type (Li₇La₃Zr₂O₁₂) solid electrolytes (SEs) represent promising candidates of the next-generation high-energy batteries yet their practical use are hindered by a short cycle life usually due to dendrite nucleation and penetration through the garnet. In the previous works, the dendrite nucleation is ascribed to poor wettability of Li metal at the alkaline-residue-covered garnet surface, and high electronic conductivity of garnet that invites Li⁺-electron recombination at grain boundary. In this work, it is showed by constructing a mathematical model on a residue-free garnet particles, that grain size of the garnet has profound influence on Li⁺ transport kinetics, and therefore, the dendrite nucleation. Smaller garnet grains tend to show faster Li⁺ transport in the bulk yet they also involve higher Li⁺ flux diffusing across grain boundaries and Li-garnet interface, which are considered kinetically more sluggish. As a result, more Li-ions tend to accumulate at the grain boundary and the interface, which accounts for unstable local environment and a sharply reduced electron migration barrier, and together they invite dendrite nucleation. Based on the findings, a new asymmetric garnet SE is proposed that features high ionic conductivity and dendrite suppression ability.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"4 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837048","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Decoupled Ion Transport via Triadic Molecular Synergy in Flame-Retardant Quasi-Solid Electrolytes for Safe Lithium Metal Batteries","authors":"Kun Li, Anjun Hu, Ruizhe Xu, Wang Xu, Borui Yang, Ting Li, Yuanjian Li, Zhi Wei Seh, Jianping Long, Shimou Chen","doi":"10.1002/aenm.202501236","DOIUrl":"https://doi.org/10.1002/aenm.202501236","url":null,"abstract":"Ionic liquids (IL)-based quasi-solid polymer electrolytes (QSPEs) hold promise for safe lithium metal batteries owing to their tunable electrochemical properties and processability. However, traditional design strategy has ignored the interdependencies among “component-function-interface”, leading to compromised practical applications hindered by sluggish lithium-ion transport kinetics and safety concerns. Herein, a triadic molecular synergy paradigm is proposed to decouple lithium-ion conduction mechanisms in flame-retardant QSPEs. Pentaerythritol tetraacrylate-lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) provides the structural framework, while the IL (1-butyl-3-methylimidazole bis (trifluoromethylsulfonyl) imide, BmimTFSI) as a plasticizer softens the polymer chains by weakening the intermolecular forces to provide an additional ion-transport pathway while imparting flame-retardant properties. Additionally, the highly electronegative fluorine atoms of the additive (2-(perfluorohexyl)ethyl methacrylate, PFMA) promote LiTFSI dissociation through electron cloud migration, simultaneously immobilizing TFSI⁻ anions and suppressing cationic competition through strong PFMA−Bmim⁺ coordination. As a proof-of-concept, this synergistic design achieves a high lithium-ion transference number (0.72), forms a stable lithium fluoride-dominated interphases, and enhances battery safety via a condensed-phase flame-retardant mechanism. Experimental validation demonstrates that the designed quasi-solid electrolyte significantly enhances cycling stability in Li symmetric cells, Li||LiFePO₄ and Li||LiNi_0.8Co_0.1Mn_0.1O₂ cells. The proposed molecular engineering strategy establishes a paradigm for developing high-performance QSPEs in lithium metal batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"37 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837195","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Understanding the Metal-Center Mediated Adsorption and Redox Mechanisms in a FeMn(NbTa)2O6 Columbite Material for Anion Exchange Membrane Water Electrolyzers","authors":"Patrick M. Bacirhonde, Devendra Shrestha, Kyoungin Kang, Esensil Man Hia, Nikhil Komalla, Nelson Y. Dzade, Merve Buldu-Akturk, Michelle P. Browne, Milan Babu Poudel, Dong Jin Yoo, Eun-Suk Jeong, Ahmed Yousef Mohamed, Byoung Gun Han, Deok-Yong Cho, Matthew T. Curnan, Geun Ho Gu, Jeong Woo Han, Chan Hee Park","doi":"10.1002/aenm.202404479","DOIUrl":"https://doi.org/10.1002/aenm.202404479","url":null,"abstract":"The rising demand for sustainable green hydrogen production necessitates efficient and cost-effective water-splitting electrocatalysts. Inspired by the catalytic activities of columbite-tantalite, this study combines a scalable cutting-edge synthesis approach with atomic-level structures and metal-center-mediated mechanisms to unravel its operational performance and stability. Using ad in situ X-ray absorption fine structure combined with Density Functional Theory (DFT), the results reveal distinctive valence band peaks and moderate charge transfer from Mn and Fe sites, enabling stable adsorption and reduced activation barriers. In contrast, the high-valence Nb and Ta centers at the B-sites promote favorable <i>d</i>-band alignment, enhancing orbital overlap with oxygen <i>p-</i>orbitals. This facilites electronic delocalization, lowers charge accumulation, and reduces activation barriers of intermediates species. Fe and Mn at the A-sites exhibit strong redox reactivity and optimal adsorption for OH* and O*, supporting efficient electron fransfers. Solvation effects modeled via VASPsol further stabilize key intermediates, especially O*, reducing the energy barrier for water dissociation. Notably, FeMn(NbTa)₂O₆-columbite catalysts stand out with a cell voltage of 1.81 V at a current density of 700 mA cm⁻², compared to 40% Pt/C-RuO₂ (1.75 V) at the same current density in the anion exchange membrane water electrolyzer (AEMWE). Also, the FeMn(NbTa)₂O₆-columbite exhibits long-term stability at 800 mA cm⁻², surpassing the benchmark 40% Pt Vulcan-RuO₂ after 200 h in AEMWE. This work significantly advances current research and establishes a design rule for selecting metal compositions in the development of advanced electrocatalysts in alkaline water electrolyzers.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"118 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832475","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Engineering Orbital Hybridization in Advanced Electrocatalysts for Energy Conversion: Fundamentals, Modulations, and Perspectives","authors":"Xian-Wei Lv, Jiaxing Gong, Shuyu Wang, Xuhuan Yan, Congkai Sun, Xiuli Hu, Zhuangzhuang Lai, Yuping Liu, Haifeng Wang, Zhong-Yong Yuan, Jianxin Geng","doi":"10.1002/aenm.202501129","DOIUrl":"https://doi.org/10.1002/aenm.202501129","url":null,"abstract":"Catalytic coordinates are essentially the dynamic interactions of frontier orbitals when interacting with electrocatalysts and adsorbates under optimal reaction conditions. Flexible modifications in orbital hybridization enable intrinsic control over both the thermodynamics and kinetics of electrochemical reactions. However, systematic depictions of this phenomenon in electrocatalysis are currently lacking, despite being extremely important. In this tutorial review, a comprehensive interpretation of orbital hybridization involved in the catalyst system and its role in electrocatalysis is provided. This review starts with the fundamentals of orbital hybridization, covering basic theories (valence bond theory, hybrid orbit theory, molecular orbital theory, and frontier orbital theory), classifications (binary- and multi-orbital interactions), and descriptors (such as orbital overlap degree, energy level matching, and Fermi energy level). It further introduces the key roles of orbital hybridization in manipulating the intrinsic activity, selectivity, and stability of electrocatalysts, as well as extending the device lifespan. Recent advances in tuning orbital hybridization for enhanced electrochemical reactions (e.g., HER, OER, ORR, NRR, and CO₂RR) through various strategies (external field modulation, electronic structure modulation, geometric structure modulation, and coordination microenvironment regulation). Challenges and perspectives for future research related to orbital hybridization are discussed at the end.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"90 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832455","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Influence of Diffusion Field Alterations on Reactant and Intermediate Adsorption in Oxygen Reduction Pathways","authors":"Guangxing Yang, Jie Chen, Jiahui Chen, Dongqin Liu, Jiayu Yuan, Zenan Wu, Zhiting Liu, Qiao Zhang, Hao Yu, Feng Peng","doi":"10.1002/aenm.202500558","DOIUrl":"https://doi.org/10.1002/aenm.202500558","url":null,"abstract":"The oxygen reduction reaction (ORR) on platinum (Pt) electrodes in acidic electrolytes can occur via two pathways, with the four‐electron pathway typically dominating. While much of the existing literature has focused on structure‐activity relationships to explain the switching between these pathways, the influence of mesoscopic mass transport—specifically related to modifications in the diffusion field—has received limited attention. In this study, the loading of Pt nanoparticles is systematically varied to create materials with comparable physicochemical properties but differing interparticle distances (IPD). Electrochemical impedance spectroscopy revealed that modifications in interparticle distance significantly alter the O<jats:sub>2</jats:sub> diffusion field, which subsequently impacts the adsorption of H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> and dictates the reaction pathways. Notably, increasing the IPD from 58.6 to 117.0 nm led to a substantial increase in H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> selectivity in acidic conditions, rising from 4.6 to 81.5%. The findings highlight the pivotal role of diffusion field modifications in influencing reactant and intermediate adsorption, thereby shaping the mechanisms of electrocatalysis.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"17 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832481","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhancing Volumetric Energy Density in Lithium–Sulfur Batteries through Highly Dense, Low Tortuosity Sulfur Electrodes","authors":"Lili Shi, Cassidy S. Anderson, Arthur Y. Baranovskiy, Jian Qin, Yaobin Xu, Rajankumar L. Patel, Chaojiang Niu, Dianying Liu, Rengarajan Pelapur, Eveline G. Booy, Adam Stokes, Zhao Liu, Jie Bao, Jie Xiao, Jun Liu, Dongping Lu","doi":"10.1002/aenm.202405890","DOIUrl":"https://doi.org/10.1002/aenm.202405890","url":null,"abstract":"Recent advancements in Lithium–sulfur (Li─S) batteries have significantly improved cell-specific energy, while challenges persist in improving volumetric energy and cell cycle life. In this study, a design principle is elucidated to enhance sulfur utilization in high-density and high-sulfur-content electrodes using a liquid-templated shear-rolling method. The findings indicate that a vascular-like hierarchical electrode structure and compatible liquid electrolytes are critical for improving electrolyte permeability in dense electrodes, achieving high sulfur utilization (&gt;1200 mAh g⁻¹) under practical conditions (47% cathode porosity, S loading 4.5 mg cm⁻², S content 70%, E/S 4 mL g⁻¹). Li─S pouch cells are demonstrated with an exceptionally high volumetric energy density (668 Wh L⁻¹) and extended cycle life by integrating the optimized electrode structures and electrolytes. This study advances understanding and design of high volumetric energy Li─S cells. Additionally, the proposed templated shear-rolling technique shows potential for application in the fabrication of other high-energy electrodes.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832457","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Layer‐by‐Layer Processed Pseudo‐Bilayer Heterojunctions Advance the Performance of Organic Solar Cells","authors":"Donghui Li, Austin M. Kay, Drew B. Riley, Oskar J. Sandberg, Ardalan Armin, Paul Meredith","doi":"10.1002/aenm.202500816","DOIUrl":"https://doi.org/10.1002/aenm.202500816","url":null,"abstract":"Recent progress in organic (semiconductor) solar cells (OSCs) has led to power conversion efficiencies (PCEs) reaching 20%, with predictions that 25% may be possible. Additional to PCE improvements, significant efforts have been made to address the engineering challenges that have traditionally limited OSCs small area devices often with poor temporal stability. Layer‐by‐layer (LbL) processing of active layers has emerged as a promising approach to tackle these challenges, with numerous state‐of‐the‐art OSCs processed using LbL reported. In this Perspective, recent developments are developed in enhancing OSC efficiency and stability, with a particular focus on the working mechanisms of pseudo‐bilayer heterojunctions (P‐BHJ) and the practical aspects of fabricating high‐performance devices using LbL techniques. By providing insights into LbL processing and the resultant film morphology, it is hoped to contribute to the ongoing efforts to improve OSC efficiency, stability, and scalability and to explore their potential for broader applications such as for example for indoor light harvesting or agrivoltaics.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"26 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827448","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Zn2+ Mediator with Ultrahigh Capacity over 8 m Enabled by H1.07Ti1.73O4 Ion Sieve for Stable Zinc Metal Batteries","authors":"Lin Huang, Xing Wang, Zihao Li, Shuyue Li, Lei Dong, Juan Wang, Keyu Xie","doi":"10.1002/aenm.202501068","DOIUrl":"https://doi.org/10.1002/aenm.202501068","url":null,"abstract":"Interfacial engineering is universally acknowledged as a dependable methodology to address the aqueous zinc metal interface issues. Although it is quite effective, the introduction of a modification layer impedes interfacial ion transport kinetics to some extent. Addressing this trade-off between stability and ion flux is critical for advancing zinc-based energy storage systems. Herein, a layered titanate (H_1.07Ti_1.73O₄, HTO) medium layer enabling fast Zn²⁺ transport and ultrahigh Zn²⁺ concentration on the zinc anode surface is proposed. It is demonstrated that HTO uniquely facilitates Zn²⁺ enrichment through the exchange of interlayer H⁺ ions, achieving an exceptionally high Zn²⁺ adsorption concentration of 8.35 <span>m</span>, far exceeding that of electrolyte (2 <span>m</span> ZnSO₄). The HTO layer serves as a dynamic ion transport bridge, establishing a continuous conductive pathway, and its inherent negative charge to selectively block sulfate anion (SO₄²⁻) penetration, thus exhibiting dual functionality as an ion conductor and anion sieve. The protected anode (Zn@HTO) exhibits exceptional stability, achieving nearly 2300 h cycling stability at a current density of 0.5 mA cm⁻² and over 3900 h at 5 mA cm⁻². Furthermore, Zn@HTO//ZnVO full cell demonstrates prolonged operational stability. This strategy provides a significant stride in breaking through the limitation of electrolyte concentration, thereby enabling fast, stable electrochemical reactions.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"40 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827633","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Proactive Lithium Dendrite Regulation Enabled by Manipulating Separator Microstructure Using High-Fidelity Phase-Field Simulation","authors":"Yajie Li, Yiping Wang, Bin Chen, Yuxiao Lin, Geng Zhang, Maxim Avdeev, Siqi Shi","doi":"10.1002/aenm.202500503","DOIUrl":"https://doi.org/10.1002/aenm.202500503","url":null,"abstract":"Separator microstructure manipulation is a promising and universal solution to undesirable dendrite growth in Li batteries, which can be operative at the very beginning of electrodeposition. However, the relationships between dendrite morphology, Li⁺ distribution and separator microstructures remain unclear. The traditionally believed two-phase system of electrode and electrolyte is also extended to three- or four-phase system with separator matrix and the generally accompanied coating nanoparticles, adding extra difficulties to the rational design of separators. Here, this study proposes a quantified separator microstructure manipulation strategy by reconstructing a high-fidelity phase-field model for multi-phase systems, in which the effective Li⁺ diffusion coefficient and electric conductivity are coupled with dynamic multi-phase evolution. Separators within the scope of experimental modification (i.e., 40–50% porosity, inner-pore roughness of 1.5–2.7, and multi-layer structure) are predicted effective for dendrite regulation, indicating the feasibility of the proposed strategy. It is further revealed that the uniformity of coating nanoparticles plays a more significant role in dendrite regulation than the commonly suggested uniformity of separator matrix. By filling the gap between separator microstructure, Li⁺ distribution and Li dendrite morphology, this research paves the way for proactive lithium dendrite regulation regardless of specific battery system.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"27 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827628","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}