Carbon Energy最新文献

Unlocking Iron Redox Depth for High-Energy Layered Sodium Oxide Cathodes 解锁高能量层状氧化钠阴极的铁氧化还原深度

IF 24.2 1区材料科学

Carbon Energy Pub Date : 2026-03-29 Epub Date: 2025-12-17 DOI: 10.1002/cey2.70142

Yadong Song, Wujie Dong, Zhuoran Lv, Bingyuan Han, Jiaming Li, Xin Wang, Xinxin Wang, Jingjing Chen, Chenlong Dong, Zhiyong Mao, Lianqi Zhang

{"title":"Unlocking Iron Redox Depth for High-Energy Layered Sodium Oxide Cathodes","authors":"Yadong Song, Wujie Dong, Zhuoran Lv, Bingyuan Han, Jiaming Li, Xin Wang, Xinxin Wang, Jingjing Chen, Chenlong Dong, Zhiyong Mao, Lianqi Zhang","doi":"10.1002/cey2.70142","DOIUrl":"10.1002/cey2.70142","url":null,"abstract":"High-capacity O3-type layered NiFeMn-based oxides are promising cathodes for sodium-ion batteries, though their practical deployment is constrained by the inherent limitations of Fe redox chemistry. Traditional designs generally enforcing stoichiometric symmetry (Ni ═ Mn) yield low Fe redox activity. Herein, we propose a valence engineering strategy that breaks conventional Ni/Mn stoichiometry to reconfigure Fe's local chemical environment and unlock unprecedented redox depth. Density functional theory (DFT) calculations reveal that the designed NaNi0.35Fe0.225Mn0.425O₂ cathode exhibits a reduced Bader charge on Fe (1.598 vs. 1.638 in NaNi1/3Fe1/3Mn1/3O2) and elevated Fe 3d orbital energy, signifying enhanced Fe redox activity. This configuration enables an exceptional Fe2.60+/Fe3.88+ redox (1.28 e− per Fe), delivering a reversible capacity of 184.3 mAh g−1 within 2–4.2 V at 0.2 C, markedly exceeding the benchmark NaNi1/3Fe1/3Mn1/3O2 (161.3 mAh g−1) with low reaction depth of Fe3.01+/Fe3.61+. The intensified cationic redox reaction enables an ultrahigh energy density of 596 Wh kg−1. The NaNi0.35Fe0.225Mn0.425O2 cathode demonstrates robust performance over a broad temperature range from −15°C to 60°C. In situ and ex situ characterizations unveil a reversible O3 ↔ P3 ↔ OP2 phase transition with minimal volume change (1.88%) that circumvents detrimental deleterious O′3 intermediates and intragranular cracking. This work establishes valence engineering as a paradigm to consolidate cationic redox reaction in high-energy layered sodium oxide cathodes.","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"8 3","pages":""},"PeriodicalIF":24.2,"publicationDate":"2026-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.70142","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147668430","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}

引用次数: 0

Synergistic Fe–Si Dual-Site Pathway Engineering in Biomass-Derived Carbon Matrix for High-Performance Oxygen Reduction Reaction 生物质衍生碳基质中高效氧还原反应的协同铁硅双位点途径工程

IF 24.2 1区材料科学

Carbon Energy Pub Date : 2026-03-29 Epub Date: 2025-12-22 DOI: 10.1002/cey2.70154

Min Su Cho, Yanmei Zang, Sung Joon Park, Byeong-Seon An, Ho Jin Lee, Ashishi Gaur, Ghulam Ali, Mingony Kim, Kyung Yoon Chung, Sungbin Park, Yung-Eun Sung, Daehae Kim, Ki Jae Kim, Chang Woo Myung, HyukSu Han

{"title":"Synergistic Fe–Si Dual-Site Pathway Engineering in Biomass-Derived Carbon Matrix for High-Performance Oxygen Reduction Reaction","authors":"Min Su Cho, Yanmei Zang, Sung Joon Park, Byeong-Seon An, Ho Jin Lee, Ashishi Gaur, Ghulam Ali, Mingony Kim, Kyung Yoon Chung, Sungbin Park, Yung-Eun Sung, Daehae Kim, Ki Jae Kim, Chang Woo Myung, HyukSu Han","doi":"10.1002/cey2.70154","DOIUrl":"10.1002/cey2.70154","url":null,"abstract":"Anion exchange membrane fuel cells (AEMFCs) offer a sustainable energy solution with non-precious metal catalysts, reduced degradation, and fuel flexibility. However, the sluggish oxygen reduction reaction (ORR) at the cathode and durability concerns impede commercialization. To address these challenges, this study presents a dual-atomic SiFe–N–C catalyst derived from pinecones, a naturally abundant biomass resource. The catalyst features a nitrogen-rich porous carbon matrix that stabilizes Si–Fe dual-atomic sites during pyrolysis. Advanced analyses confirm Fe–Si and Fe–N bonds, which synergistically enhance ORR activity by optimizing electronic structures and intermediate adsorption energies. The SiFe–N–C catalyst surpasses Pt/C and Fe–N–C single-atom benchmarks with superior ORR activity and excellent long-term durability supported by high resistance to CO poisoning as well as methanol crossover. It also demonstrates a promising electrochemical performance as a catalytic material for the separator of Li–S battery. Mechanistic studies reveal that the Si–Fe dual-atomic configuration promotes an efficient Fe–O–O–Si pathway, reducing energy barriers and offering a cost-effective, high-performance solution for electrochemical energy conversion and storage applications.","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"8 3","pages":""},"PeriodicalIF":24.2,"publicationDate":"2026-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.70154","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147668701","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}

引用次数: 0

Back Cover Image, Volume 8, Number 3, March 2026 封底图片，第八卷，第三期，2026年3月

IF 24.2 1区材料科学

Carbon Energy Pub Date : 2026-03-29 DOI: 10.1002/cey2.70216

{"title":"Back Cover Image, Volume 8, Number 3, March 2026","authors":"","doi":"10.1002/cey2.70216","DOIUrl":"10.1002/cey2.70216","url":null,"abstract":"Back cover image: The oxygen evolution reaction (OER) has long been the bottleneck in water splitting for green hydrogen production—sluggishness, intensive energy and prone to catalyst degradation. This review explores a paradigm shift in OER catalysis through the recently discovered Oxide Path Mechanism (OPM). Unlike conventional mechanisms (AEM or LOM) that suffer from either poor activity or rapid catalyst degradation (Scaling relation or Lattice Oxygen involvement), OPM enables direct O-O radical coupling while maintaining catalyst integrity. Through systematic integration of advanced in-situ characterization techniques—including ICP-MS, In-Situ XPS, In-Situ FTIR and Mössbauer spectroscopy—researchers can now observe these mechanisms under operational conditions. The review demonstrates how OPM-based catalysts achieving long term stability, offer a practical solution to the longstanding activity-stability trade-off, bringing industrial-scale green hydrogen production closer to economic viability.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture>\u0000 </div>\u0000 </figure>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"8 3","pages":""},"PeriodicalIF":24.2,"publicationDate":"2026-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.70216","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147668966","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}

引用次数: 0

Boosting C=O Bond Scissoring Over a Pyridinic Nitrogen-Modified Cu–MoC Interface for High-Efficiency CO2 Hydrogenation to CO 吡啶氮修饰Cu-MoC界面上C=O键剪切促进CO2高效加氢成CO

IF 24.2 1区材料科学

Carbon Energy Pub Date : 2026-03-29 Epub Date: 2026-01-04 DOI: 10.1002/cey2.70165

Haiquan Liao, Caikang Wang, Xueyuan Pan, Hao Sun, Yanlin Liao, Mingzhe Ma, Guowu Zhan, Mengmeng Fan, Linfei Ding, Jingcheng Xu, Yali Wang, Kang Sun, Xiangzhou Yuan, Jianchun Jiang

{"title":"Boosting C=O Bond Scissoring Over a Pyridinic Nitrogen-Modified Cu–MoC Interface for High-Efficiency CO2 Hydrogenation to CO","authors":"Haiquan Liao, Caikang Wang, Xueyuan Pan, Hao Sun, Yanlin Liao, Mingzhe Ma, Guowu Zhan, Mengmeng Fan, Linfei Ding, Jingcheng Xu, Yali Wang, Kang Sun, Xiangzhou Yuan, Jianchun Jiang","doi":"10.1002/cey2.70165","DOIUrl":"10.1002/cey2.70165","url":null,"abstract":"Reverse water-gas shift (RWGS) reaction-aided sustainable CO2 conversion has emerged as one promising and effective approach for simultaneously mitigating climate change and solidifying energy security. Molybdenum carbide-based catalysts demonstrate excellent selectivity for sustainably transforming CO2 into CO product, but harsh carburization syntheses and insufficient catalytic activity and stability significantly hinder their related commercial applications. Herein, a facile “inside-out” synthesis strategy was proposed to fabricate dispersed Cu clusters on sub-2 nm α-MoC nanoislands confined in pyridinic nitrogen-doped carbon (Cu-MoC/NC). This catalyst achieves the highest CO2 conversion rate of 2583.4 mmolCO2 gcat−1 h−1 compared to those of all reported Mo-based catalysts, and maintains excellent catalytic stability for 500 h under a low H2 partial pressure. Combined with X-ray absorption spectroscopy (XAS) and density functional theory (DFT) calculations, the electronegativity of pyridinic nitrogen intensifies the electron deficiency of α-MoC and strengthens the chemisorption of Cu clusters on α-MoC nanoislands surface, facilitating the electronic interaction and stability of Cu–MoC interface. This pyridinic nitrogen-modified Cu–MoC interface promotes the CO2 bridged adsorption at the interface and thus boosts C=O bond scissoring, inducing the transition of rate-limiting step and energy barrier reduction of the key intermediates. This interfacial engineering provides a sustainable and efficient strategy for improving both catalytic activity and stability of RWGS reaction to transform CO2 into value-added fuels and chemicals.","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"8 3","pages":""},"PeriodicalIF":24.2,"publicationDate":"2026-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.70165","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147668002","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}

引用次数: 0

Strategies to Enhance Ionic Conductivity of Na3Zr2Si2O12 Solid Electrolyte for Advanced Solid-State Sodium Batteries 提高先进固态钠电池用Na3Zr2Si2O12固体电解质离子电导率的策略

IF 24.2 1区材料科学

Carbon Energy Pub Date : 2026-03-29 Epub Date: 2026-01-04 DOI: 10.1002/cey2.70157

Jiawen Hu, Zixing Chen, Xi Wang, Changsheng Ding, Yongfeng Li, Yanfeng Gao

{"title":"Strategies to Enhance Ionic Conductivity of Na3Zr2Si2O12 Solid Electrolyte for Advanced Solid-State Sodium Batteries","authors":"Jiawen Hu, Zixing Chen, Xi Wang, Changsheng Ding, Yongfeng Li, Yanfeng Gao","doi":"10.1002/cey2.70157","DOIUrl":"10.1002/cey2.70157","url":null,"abstract":"Solid-state sodium batteries (SSSBs) have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety, higher energy density, and substantial resources and low cost of sodium. Na3Zr2Si2PO12 (NZSP) solid electrolyte is attracting considerable interest owing to its excellent thermal and chemical stability and favorable compatibility with Na metal anode and high-voltage cathode. However, two main challenges of poor room-temperature ionic conductivity and high interfacial resistance limit the application of NZSP electrolyte in SSSBs. So far, intensive efforts have been devoted to developing modification strategies to improve the room-temperature ionic conductivity of NZSP. This review aims to provide a comprehensive summary and discussion of some optimization strategies for enhancing the room-temperature ionic conductivity of the NZSP solid electrolyte. These optimization strategies are categorized into foreign-ion doping or substitution, sintering behavior modulation, and regulation of chemical composition based on precursors, and their optimization mechanisms are also elaborated. Finally, the prospects of NZSP-based solid electrolytes are presented. This review is expected to offer better guidance for designing and developing high-performance NZSP-based solid electrolytes for accelerating the practical application of SSSBs.","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"8 3","pages":""},"PeriodicalIF":24.2,"publicationDate":"2026-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.70157","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147668077","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}

引用次数: 0

Recent Progress of Na3MnTi(PO4)3 Cathode for Sodium-Ion Batteries: Mechanism, Synthesis, and Optimization Strategy 钠离子电池用Na3MnTi(PO4)3正极材料的研究进展：机理、合成及优化策略

IF 24.2 1区材料科学

Carbon Energy Pub Date : 2026-03-29 Epub Date: 2025-12-15 DOI: 10.1002/cey2.70162

Shanshan Lv, Peng Wei, Fan Wu, Kang Liang, Fangyuan Cheng, Jian Peng, Yurong Ren

{"title":"Recent Progress of Na3MnTi(PO4)3 Cathode for Sodium-Ion Batteries: Mechanism, Synthesis, and Optimization Strategy","authors":"Shanshan Lv, Peng Wei, Fan Wu, Kang Liang, Fangyuan Cheng, Jian Peng, Yurong Ren","doi":"10.1002/cey2.70162","DOIUrl":"10.1002/cey2.70162","url":null,"abstract":"Sodium-ion batteries (SIBs) have exhibited significant commercial potential, benefiting from the abundance and global distribution of sodium resources. Among the diverse cathode materials under exploration for SIBs, Na3MnTi(PO4)3 (NMTP) stands out as a highly promising candidate for practical applications, which combines the structural stability and high-voltage characteristics inherent to NASICON-type materials. In recent years, substantial advancements have been achieved in the research of NMTP. However, a comprehensive and up-to-date specialized review dedicated to its research progress and prospects remains lacking. This review, therefore, aims to systematically discuss the development and outlook of NMTP cathode material. Initially, the manuscript delves into the crystal structure and sodium-storage mechanism of NMTP. Subsequently, the synthesis methods, electrochemical properties, and optimization strategies are explored. Finally, the review outlines current challenges and suggests potential future research directions for NMTP.","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"8 3","pages":""},"PeriodicalIF":24.2,"publicationDate":"2026-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.70162","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147668296","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}

引用次数: 0

Coupling of 0D/1D Grain Boundaries Inducing Extreme Charge Rearrangement/Magnetic Resonance for Ultrabroadband Electromagnetic Wave Absorption 0D/1D晶界耦合诱导极端电荷重排/超宽带电磁波吸收磁共振

IF 24.2 1区材料科学

Carbon Energy Pub Date : 2026-03-29 Epub Date: 2025-12-18 DOI: 10.1002/cey2.70126

Jie Huang, Liuying Wang, Renbing Wu, Weichao Wang, Chaoqun Ge, Haoke Yang, Xu Tang, Wenyu Jiao, Gu Liu, Bin Wang

{"title":"Coupling of 0D/1D Grain Boundaries Inducing Extreme Charge Rearrangement/Magnetic Resonance for Ultrabroadband Electromagnetic Wave Absorption","authors":"Jie Huang, Liuying Wang, Renbing Wu, Weichao Wang, Chaoqun Ge, Haoke Yang, Xu Tang, Wenyu Jiao, Gu Liu, Bin Wang","doi":"10.1002/cey2.70126","DOIUrl":"10.1002/cey2.70126","url":null,"abstract":"Ferrite–carbon composites effectively absorb electromagnetic (EM) waves via coupled mechanisms. However, the dynamic evolution of intrinsic polarization and magnetic loss mechanisms following interfacial coupling has long been overlooked, impeding broadening of the ultra-broadband EM wave absorption performance in heterostructures. Herein, via surface ligand modulation, in situ growth of 0D Fe3O4 quantum dots (QDs) on the surface of 1D carbon nanotubes triggers grain boundary coupling. The energy rebalancing effect at the interface induces an extreme charge rearrangement within the Fe3O4 QDs. This rearrangement enhances dipole orientation hysteresis and charge accumulation, resulting in charge and interfacial polarization losses. Meanwhile, for subcritical Fe3O4 QDs, short-range magnetic resonance and magnetic exchange–triggered magnetic resonance transfer synergistically enhance the magnetic loss. Through charge rearrangement/magnetic resonance induced by 0D/1D grain boundary coupling, an effective bandwidth of nearly 10 GHz is achieved at a minimal thickness of 2 mm, covering the X and Ku bands. This strategy provides an effective paradigm and novel theoretical insights for ultra-broadband electromagnetic wave absorption applications.","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"8 3","pages":""},"PeriodicalIF":24.2,"publicationDate":"2026-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.70126","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147668605","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}

引用次数: 0

Vertically Aligned Ion Pathways for Fast Conduction and Uniform Lithium Deposition in Solid-State Batteries 固态电池中快速传导和均匀锂沉积的垂直排列离子通道

IF 24.2 1区材料科学

Carbon Energy Pub Date : 2026-03-29 Epub Date: 2025-12-21 DOI: 10.1002/cey2.70152

Sha Peng, Jia Chen, Yu Li, Ying Tao, Lei Zhang, Jiyan Liu, Zhihong Liu, Xueqing Liu

{"title":"Vertically Aligned Ion Pathways for Fast Conduction and Uniform Lithium Deposition in Solid-State Batteries","authors":"Sha Peng, Jia Chen, Yu Li, Ying Tao, Lei Zhang, Jiyan Liu, Zhihong Liu, Xueqing Liu","doi":"10.1002/cey2.70152","DOIUrl":"10.1002/cey2.70152","url":null,"abstract":"The random distribution of one-dimensional nanofillers in composite polymer electrolytes (CPEs) typically results in tortuous ion transport pathways, severely limiting ionic conductivity and Li⁺ flux uniformity. Herein, an innovative electric field-assisted strategy is proposed to construct vertically aligned ion channels in CPEs using lithiated halloysite nanotubes (HNTs–SO₃Li) embedded within a polyurethane acrylate/polyethylene glycol diacrylate (PUA/PEGDA) matrix. Under an alternating electric field, the nanotubes orient perpendicularly, forming continuous, low-tortuosity pathways that significantly enhance room-temperature ionic conductivity. The aligned structure not only shortens Li⁺ transport distances but also homogenizes ion flux at the electrode interface, effectively suppressing lithium dendrite growth. Electrochemical characterization reveals exceptional stability. Three-dimensional structural reconstruction and ion transport simulations further demonstrate that the ordered channels promote uniform Li⁺ distribution and faster ion kinetics compared to disordered systems. This study provides a scalable and efficient approach to designing high-performance CPEs for next-generation solid-state batteries, addressing critical challenges in ionic conductivity, interfacial stability, and dendrite suppression.","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"8 3","pages":""},"PeriodicalIF":24.2,"publicationDate":"2026-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.70152","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147668625","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}

引用次数: 0

Defect Suppression via Tailoring Functionalized Additives for Efficient and Stable CsPbI3 Perovskite Solar Cells 基于功能化添加剂的高效稳定cspbi3钙钛矿太阳能电池缺陷抑制研究

IF 24.2 1区材料科学

Carbon Energy Pub Date : 2026-03-29 Epub Date: 2025-10-31 DOI: 10.1002/cey2.70107

Haiyan Zhao, Chunyan Li, Yao Zhang, Zhongxun Yu, Jixiang Zhang, Xiaoan Tang, Zi Ouyang, Haipeng Yin, Yang Sun, Hao Du, Han Chen

引用次数: 0

Modulating Metal–Oxygen Bond Energy by Valence State Engineering in 2D High Entropy Oxides for Enhanced Water Electrolysis 利用价态工程在二维高熵氧化物中调制金属-氧键能以促进水电解

IF 24.2 1区材料科学

Carbon Energy Pub Date : 2026-03-29 Epub Date: 2025-12-18 DOI: 10.1002/cey2.70151

Tian Wu, Shasha Gao, Runlin Ma, Rui Zhang, Chaolong Wang, Dong Guo, Die Lu, Zhihong Tian, Menggai Jiao, Zhen Zhou, Gonglei Shao

{"title":"Modulating Metal–Oxygen Bond Energy by Valence State Engineering in 2D High Entropy Oxides for Enhanced Water Electrolysis","authors":"Tian Wu, Shasha Gao, Runlin Ma, Rui Zhang, Chaolong Wang, Dong Guo, Die Lu, Zhihong Tian, Menggai Jiao, Zhen Zhou, Gonglei Shao","doi":"10.1002/cey2.70151","DOIUrl":"10.1002/cey2.70151","url":null,"abstract":"Valence state engineering has emerged as a powerful strategy to optimize catalytic performance by modulating the electronic structure of metal active sites. However, the valence state regulation in high-entropy compounds (HECs) remains elusive due to their complex multi-element components and electronic interactions. Here, the valence states of different metals in two-dimensional (2D) high entropy oxide (HEO) (FeNiMoRuV)O2−x are precisely modulated through controlled pyrolysis of corresponding 2D high entropy hydroxide (HEHO) (FeNiMoRuV)(OH)2 under varying temperatures. Temperature-controlled pyrolysis selectively reduces the oxidation state of Ru, while simultaneously increasing the valence state of other constituent metals (Fe, Ni, Mo, and V), suggesting a competitive redox equilibrium. Notably, these low-valence Ru sites with oxygen vacancy in 2D HEO significantly reduce Ru–O bond energy and promote the generation of O–*O intermediates, thereby enabling oxygen evolution with a lattice oxygen mediated-oxygen vacancy site mechanism. 2D HEO with low-valence Ru exhibits superior electrolytic water performance (HER/OER) compared to HEHO and other HEO with high-valence Ru, achieving a current density of 1000 mA cm−2 at 1.923 V, which exceeds the commercial Pt/C||RuO2 system. Therefore, this study reveals the valence state regulatory mechanism of HECs and provides a solid hammer for the catalytic mechanism of valence state engineering.","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"8 3","pages":""},"PeriodicalIF":24.2,"publicationDate":"2026-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.70151","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147668604","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}

引用次数: 0