Wenhan Ou, Samuel D. Marks, Rafael Ferreira de Menezes, Rong He, Zihan Zhang, Collin Sindt, Jonathan Thurston, Cherno Jaye, Bruce Cowie, Lars Thomsen, Zengqing Zhuo, Jinghua Guo, Wanli Yang, Ziyue Dong, Robert Tenent, Kayla G. Sprenger, Michael F. Toney
{"title":"Unveiling the Mechanism of Mn Dissolution Through a Dynamic Cathode‐Electrolyte Interphase on LiMn2O4","authors":"Wenhan Ou, Samuel D. Marks, Rafael Ferreira de Menezes, Rong He, Zihan Zhang, Collin Sindt, Jonathan Thurston, Cherno Jaye, Bruce Cowie, Lars Thomsen, Zengqing Zhuo, Jinghua Guo, Wanli Yang, Ziyue Dong, Robert Tenent, Kayla G. Sprenger, Michael F. Toney","doi":"10.1002/aenm.202404652","DOIUrl":"https://doi.org/10.1002/aenm.202404652","url":null,"abstract":"Understanding the formation and evolution of the cathode‐electrolyte interphase (CEI), which forms at the interface between the cathode and electrolyte, is crucial for revealing degradation mechanisms in cathode materials, especially for developing strategies to stabilize the interphase in the strongly oxidizing conditions that evolve at high operating voltages in next‐generation Li‐ion batteries. However, The present understanding of the CEI is challenged by its complex and dynamic nature. In this work, near‐edge X‐ray absorption fine structure spectroscopy, electrochemical characterization, and reactive molecular dynamics simulations are combined to reveal a mechanism for CEI formation and evolution above model LiMn<jats:sub>2</jats:sub>O<jats:sub>4</jats:sub> (LMO) thin‐film electrodes in contact with conventional carbonate‐based electrolytes. It is found that Mn dissolution from LMO can be understood in terms of repetitive Mn<jats:sub>3</jats:sub>O<jats:sub>4</jats:sub> formation and dissolution behavior during cycling, which is closely connected to electrolyte decomposition and a key aspect of the CEI formation and growth. The behavior of the CEI in this model system offers detailed insight into the dynamic chemistry of the interphase, underscoring the important role of electrolyte composition and cathode surface structure in interphase degradation.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418057","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":"Constructing Compact Hybrid Buffer Interface via Ion Agglomeration Zone Electrolyte for Stable Zn Metal Battery","authors":"Yefei Chen, Weidong He, Kangning Zhao, Xingyun Luo, Jiafeng Zhang, Yongzhong Wu, Xiaopeng Hao","doi":"10.1002/aenm.202405738","DOIUrl":"https://doi.org/10.1002/aenm.202405738","url":null,"abstract":"The development of aqueous Zn batteries is plagued by longevity limited at practical condition, due to the unstable electrode‐electrolyte interface. Here, this work designs an extended‐scale ion agglomeration zone (EIAZ) electrolyte to obtain anion combined with cation structures and reduce water activity. The electrolyte nanostructure features nanometer‐scale depleted water zones in which ion pairs are densely packed together to form EIAZ, which facilitates compact hybrid buffer interface formed via a collective ion transmission process and ionic co‐opetition relationship. The convergence and densification models of buffer interface for Zn surface is the result of cations adaptive adsorption that mitigates the concentration polarization of interfacial Zn<jats:sup>2+</jats:sup> and prevents water contact with electrodes, constituting an indispensable premise for stabilizing both anode and cathode interface. Moreover, unique electrolyte nanostructure achieves Zn crystallographic optimization and fast interfacial reaction kinetics, generating ultralong cycling stability of 5500 h. Therefore, zinc‐organic batteries can exert outstanding stability for over 3000 cycles and 1000 cycles under high current (10 A g<jats:sup>‒1</jats:sup>) and high mass loading (14 mg cm<jats:sup>−2</jats:sup>). Impressively, pouch cell shows an excellent capacity retention of 99.8% with 26.1 mAh after 250 cycles. This study offers a novel perspective for designing electrolyte nanostructures and electrode interfaces for high‐performance Zn batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"10 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418059","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":"In Situ High‐Temperature Phase Elucidation of Secondary Particles and Segregating Nanoparticles with Surface Coating‐Networking Architecture for High‐Voltage Cathode Life at High Rate","authors":"Manikandan Palanisamy, Matthew M. Mench","doi":"10.1002/aenm.202404368","DOIUrl":"https://doi.org/10.1002/aenm.202404368","url":null,"abstract":"Secondary microparticles are synthesized using a Mn<jats:sub>1.5</jats:sub>Ni<jats:sub>0.5</jats:sub>(OH)<jats:sub>2</jats:sub>CO<jats:sub>3</jats:sub> precursor, which undergoes thermal decomposition and calcination, releasing CO<jats:sub>2</jats:sub> and H<jats:sub>2</jats:sub>O gaseous species. In situ high‐temperature phase elucidation confirms the least degree of disordered phase LiMn<jats:sub>1.5</jats:sub>Ni<jats:sub>0.5</jats:sub>O<jats:sub>4</jats:sub> cathode without rock‐salt impurity phase and having insignificant content of Mn<jats:sup>3+</jats:sup> to stable Fd m structure. Raman spectrum shows a band at 590 cm<jats:sup>−1</jats:sup> (F<jats:sub>2g</jats:sub><jats:sup>(3)</jats:sup>) without splitting, confirming spinel compound derived with disordered phase. Microscopic analyses reveal secondary microparticles and segregated primary nanoparticles having surface coating‐conducting network architecture. Cyclic voltammograms of primary nanoparticles show well‐resolved two redox peaks at 4.7 V compared to secondary microparticles, confirming superior kinetic reversibility for Ni<jats:sup>2+</jats:sup> to Ni<jats:sup>3+</jats:sup> and Ni<jats:sup>3+</jats:sup> to Ni<jats:sup>4+</jats:sup> redox process. At 20C discharge, segregated primary nanoparticles exhibit a discharge flat voltage profile at 4.3 V and deliver a high reversible capacity of 100 mAh g<jats:sup>−1</jats:sup> for the 12th cycle and 86 mAh g<jats:sup>−1</jats:sup> for the 1000th cycle, while secondary microparticles deliver 70 mAh g<jats:sup>−1</jats:sup> for 12th cycle and declined its cycle operation at 250th cycle with the capacity of < 5 mAh g<jats:sup>−1</jats:sup>. Results confirm a strong potential for use as a highly durable, cobalt‐free, high‐voltage cathode capable of high‐rate discharge in LIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"11 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418061","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}
Qianqian Cheng, Zutao Sheng, Mingjie Li, Wenjing Ye, Sangshan Peng, Guang Zeng, Qing He
{"title":"Supramolecular Interaction‐Driven Amorphization of Poly(aryl piperidine) Membranes for Enhanced Proton Conductivity","authors":"Qianqian Cheng, Zutao Sheng, Mingjie Li, Wenjing Ye, Sangshan Peng, Guang Zeng, Qing He","doi":"10.1002/aenm.202405436","DOIUrl":"https://doi.org/10.1002/aenm.202405436","url":null,"abstract":"Non‐fluorinated polymer membranes offer a commercially feasible solution for redox flow batteries (RFBs), yet their practical applications have been hampered by inherent challenges such as chemical instability and low ionic conductivity. In this study, the development of a series of ether‐bond‐free poly(aryl piperidine) membranes that address these limitations by introducing enhanced disorder in polymer chain packing through supramolecular interactions with organic acids, is presented. These interactions effectively disrupt densely packed polymer chains, transforming proton‐inaccessible crystalline regions into accessible amorphous ones. By eliminating chemically unstable aryl ether bonds and avoiding additional chemical modifications, these membranes exhibit remarkable long‐term chemical stability. The presence of abundant interchain gaps further facilitates rapid proton‐selective transport. As a result, the engineered membranes demonstrate sustained performance in vanadium RFBs, maintaining stable operation for over 1000 charge/discharge cycles, and achieving an impressive energy efficiency of 80% at a high current density of 280 mA cm<jats:sup>−</jats:sup><jats:sup>2</jats:sup>. The combination of experimental data and theoretical modeling suggests that the membrane's outstanding performance arises from the interconnected and widely distributed interchain gaps, which exhibit a pore‐limiting diameter of ≈8 Å. These findings offer a robust design strategy for developing chemically stable, high‐performance non‐fluorinated membranes for RFBs and related energy conversion devices.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"183 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418058","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":"Boosting the Efficiency and Mechanical Stability of Organic Solar Cells Through a Polymer Acceptor by Reducing the Elastic Modulus","authors":"Yan Wang, Han Yu, Dan Zhao, Wei Liu, Baoze Liu, Xin Wu, Danpeng Gao, Dong Zhang, Shoufeng Zhang, Xianglang Sun, Chunlei Zhang, Chaoyue Zhao, Yuchen Fu, Wei Song, Shaokuan Gong, Yuang Fu, Chung Hang Kwok, Ziyi Ge, Xinhui Lu, Xihan Chen, Shuang Xiao, Wai-Yeung Wong, Yu Chai, He Yan, Zonglong Zhu","doi":"10.1002/aenm.202404499","DOIUrl":"https://doi.org/10.1002/aenm.202404499","url":null,"abstract":"Organic solar cells (OSCs) are regarded as one of the most promising flexible power sources due to their lightweight and flexible properties, with the improvement of photovoltaic and mechanical performance. To improve the current density and power conversion efficiency (PCE), mPh4F-TS (TS) and PYSe2F-T (PA) are introduced into the binary host, PM6/mPh4F-TT (PM6/TT) as third components. It is demonstrated that the corresponding ternary devices, in both rigid and flexible devices, achieved superior efficiencies (19.6%/17.7% for PM6/TT+TS, and 19.2%/17.4% for PM6/TT+PA) outperform the binary counterparts (18.3%/16.4%). However, distinct differences in mechanical performance are observed between the polymer acceptor (PA) and small-molecular acceptor (TS). The PM6/TT+PA significantly improved the mechanical stability of flexible devices with a lower elastic modulus of 3.6 GPa, while the PM6/TT+TS resulted in the opposite effect with a higher elastic modulus of 5.5 GPa. Through in-depth investigation, a clear correlation between the elastic modulus, crack density, and mechanical stability of the active layer blends is successfully established, revealing the key role of reducing the elastic modulus in enhancing the mechanical stability of flexible OSCs. This study provides important guidance for the development of flexible photovoltaic devices with both high efficiency and mechanical robustness.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"20 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401385","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":"Cd Single Atom as an Electron Mediator in an S-Scheme Heterojunction for Artificial Photosynthesis of H2O2","authors":"Xiaowen Ruan, Minghua Xu, Chunsheng Ding, Jing Leng, Guozhen Fang, Depeng Meng, Wei Zhang, Zhifeng Jiang, Sai Kishore Ravi, Xiaoqiang Cui, Jiaguo Yu","doi":"10.1002/aenm.202405478","DOIUrl":"https://doi.org/10.1002/aenm.202405478","url":null,"abstract":"Developing conductor-mediated S-scheme heterojunction photocatalysts imitating natural photosynthetic systems emerges as a promising approach to hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production. However, achieving precise coupling between two semiconductors with a charge shuttle and modulating the interfacial interactions still remain a significant bottleneck. Herein, we propose a catalyst architecture with a Cd single atom mediated S-scheme heterojunction formed by interfacing CdS and TiO<sub>2</sub> nanoparticles. This catalyst exhibits an H<sub>2</sub>O<sub>2</sub> production rate as high as 60.33 µmol g<sup>−1 </sup>min<sup>−1</sup> under UV–vis light irradiation, which is attributed to the efficient charge transport at the interface of CdS and TiO<sub>2</sub> thanks to the Cd single atom mediated S-scheme. In-situ X-ray photoelectron spectroscopy (XPS) and electron spin resonance (ESR) spin-trapping tests confirm the S-scheme charge transfer route. Femtosecond transient absorption (fs-TA) spectroscopy and other ex-situ characterizations further corroborate the efficient charge transport across the catalyst interface. This work offers a new perspective on constructing single atoms mediated heterojunctions to enhance photocatalytic performance.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"63 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401384","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":"Tailoring Electronic and Morphology Features of Iron-Doped Ni2P Nanoflowers for Enhanced Ammonia Electrosynthesis in Solid Electrolyte Reactors","authors":"Qi Zhang, Congcong Ni, Ning Deng, Xin Huang","doi":"10.1002/aenm.202405442","DOIUrl":"https://doi.org/10.1002/aenm.202405442","url":null,"abstract":"Electrochemical nitrate (NO<sub>3</sub><sup>−</sup>) reduction to ammonia (NH<sub>3</sub>) presents a promising route for both wastewater treatment and ammonia generation but still suffers from sluggish catalytic activity, insufficient mass transfer, and the reliance on high-concentration supporting electrolytes. This work reports an innovative and efficient ammonia electrosynthesis reactor by integrating a self-assembled iron-doped Ni<sub>2</sub>P (Fe-Ni<sub>2</sub>P/NF) nanoflower cathode with a solid-electrolyte (SE). The SE design eliminates the need for supporting electrolytes, providing a highly efficient ion-conducting pathway and enabling the direct production of NH<sub>3</sub> from NO<sub>3</sub><sup>−</sup>. Through tailoring the electronic and surface characteristics of Fe-Ni<sub>2</sub>P/NF, this reactor achieves complete NO<sub>3</sub><sup>−</sup> reduction, 96.7% NH<sub>3</sub> selectivity, and 81.8% faradaic efficiency with a NO<sub>3</sub><sup>−</sup> concentration of 100 m<span>m</span> at a current density of 100 mA m<sup>−2</sup>. Density functional theory (DFT) calculations reveal that phosphating and Fe doping synergistically enhance NO<sub>3</sub><sup>−</sup> adsorption and increase the availability of active hydrogen, thus favoring NH<sub>3</sub> production at a low energy barrier of 0.695 eV. Additionally, the superhydrophilicity of the Fe-Ni<sub>2</sub>P/NF nanoflower catalyst promotes mass transfer by facilitating electrolyte access and ensuring rapid gas bubble release. This study provides a sustainable and scalable method for converting NO<sub>3</sub><sup>−</sup>-laden wastewater into valuable ammonia products.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"61 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401383","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}
Seonghyun Lee, Taehun Kim, Kanghyeon Kim, Gawon Song, Junsung Park, Minseon Lee, Hyeseung Jung, Kyobin Park, Seung Hyun Choi, Juyeop Song, Kyu Tae Lee
{"title":"Mechano-Electrochemical Healing at the Interphase Between LiNi0.8Co0.1Mn0.1O2 and Li6PS5Cl in All-Solid-State Batteries","authors":"Seonghyun Lee, Taehun Kim, Kanghyeon Kim, Gawon Song, Junsung Park, Minseon Lee, Hyeseung Jung, Kyobin Park, Seung Hyun Choi, Juyeop Song, Kyu Tae Lee","doi":"10.1002/aenm.202405782","DOIUrl":"https://doi.org/10.1002/aenm.202405782","url":null,"abstract":"Sulfide-based all-solid-state batteries (ASSBs) are emerging as promising alternatives to lithium-ion batteries due to their high energy density and enhanced safety. However, sulfide solid electrolytes, such as Li<sub>6</sub>PS<sub>5</sub>Cl (LPSCl), face significant chemo-mechanical challenges at the interface with layered oxide cathodes, including Li[Ni<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>]O<sub>2</sub> (NCM811). During cycling, oxidative decomposition of LPSCl leads to interfacial void formation and mechanical contact loss, which significantly degrade ionic conduction. Strategies such as coating stable passivation layers have been explored to suppress LPSCl decomposition, but these approaches often involve trade-offs, including increased cost, complex synthesis, and elevated interfacial resistance. Herein, the concept of mechano-electrochemical healing at the LPSCl–NCM811 interface is introduced to address these issues. During charging, voids form due to LPSCl decomposition; however, this mechanical contact loss can be reversed through a healing mechanism during discharge at ≈2.2 V (vs Li/Li<sup>+</sup>). This process, driven by the lithiation of elemental sulfur − a decomposition product of LPSCl − restores interfacial contact and enhances ionic conduction. Consequently, mechano-electrochemical healing achieves stable capacity retention over 300 cycles and superior rate capability even under pressure-free conditions. These findings underscore the potential of electrochemical formation cycling as a practical strategy for improving the mechano-electrochemical performance of ASSBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"12 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385844","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}
Yuehan Cao, Wang Yu, Yi Li, Jie Meng, Kaibo Zheng, Chuan Huang, Xin Yang, Yuantao Yang, Fan Dong, Ying Zhou
{"title":"Engineering Ultrafast Photo-Induced Charge and Carbon Intermediates Transfer at Interface to Break the Activity-Selectivity Trade-Off in Direct Conversion of Methane to Methanol (Adv. Energy Mater. 6/2025)","authors":"Yuehan Cao, Wang Yu, Yi Li, Jie Meng, Kaibo Zheng, Chuan Huang, Xin Yang, Yuantao Yang, Fan Dong, Ying Zhou","doi":"10.1002/aenm.202570032","DOIUrl":"https://doi.org/10.1002/aenm.202570032","url":null,"abstract":"<p><b>Methane Conversion</b></p><p>In article number 2404871, Ying Zhou and co-workers introduce a breakthrough in photocatalytic methane-to-methanol conversion using BiOI/BN heterojunction nanosheets, employing interface engineering to enhance ultrafast charge transfer and stabilize the backtracking of intermediate to produce methanol. This achieves 15.5% methane conversion and 86.4% methanol selectivity under ambient conditions for 24 hours.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 6","pages":""},"PeriodicalIF":24.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.202570032","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143389041","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Haoxin Fan, Xinhao Wan, Shougang Sun, Xuemei Zhou, Xiuming Bu, Jianqi Ye, Rui Bai, Hengwei Lou, Yao Chen, Jie Gao, Jian Zhang, Wei Gao, Dan Wen
{"title":"Revealing the Role of Ru‐O‐Ce Interface Coupling in CeO2‐Ru Aerogel for Boosting Hydrogen Evolution Kinetics","authors":"Haoxin Fan, Xinhao Wan, Shougang Sun, Xuemei Zhou, Xiuming Bu, Jianqi Ye, Rui Bai, Hengwei Lou, Yao Chen, Jie Gao, Jian Zhang, Wei Gao, Dan Wen","doi":"10.1002/aenm.202405681","DOIUrl":"https://doi.org/10.1002/aenm.202405681","url":null,"abstract":"Designing heterogeneous interface to enhance the kinetics for electrocatalysts is a highly efficient but challenging pathway toward hydrogen evolution reaction (HER) in water electrolysis. Herein, the heterogeneous coupling of CeO<jats:sub>2</jats:sub> quantum dots onto porous Ru aerogel through interfacial Ru‐O‐Ce bridge is proposed to construct CeO<jats:sub>2</jats:sub>‐Ru aerogel as the superior HER electrocatalyst with ultra‐low overpotentials. In situ characterizations and theoretical calculations reveal the electron distribution at the heterogeneous Ru‐O‐Ce bridge to boost hydrogen bonding at Ru sites, and the faster water adsorption and dissociation at the CeO<jats:sub>2</jats:sub> sites to enhance the HER kinetics. Furthermore, CeO<jats:sub>2</jats:sub>‐Ru aerogel is employed as excellent cathodes for both acidic and alkaline water electrolyzers with ampere‐level current density and stably operated over 500 hours. Thus, the synergistic effect for CeO<jats:sub>2</jats:sub>‐Ru aerogel through the Ru‐O‐Ce bridge tunes the HER catalytic mechanism and reinforces the activity, realizing highly efficient hydrogen generation in water electrolysis.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"32 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385302","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}