Journal of Energy Chemistry最新文献_第4页

Cu+ optimizes the FeHCF coordination environment to enhance high-voltage energy storage Cu+优化FeHCF协同环境，增强高压储能能力

IF 14.9 1区化学

Journal of Energy Chemistry Pub Date : 2025-09-09 DOI: 10.1016/j.jechem.2025.08.074

Zu-Tao Pan , Yao Xu , Ling-Bin Kong

{"title":"Cu+ optimizes the FeHCF coordination environment to enhance high-voltage energy storage","authors":"Zu-Tao Pan , Yao Xu , Ling-Bin Kong","doi":"10.1016/j.jechem.2025.08.074","DOIUrl":"10.1016/j.jechem.2025.08.074","url":null,"abstract":"<div><div>Prussian blue analogs (PBAs) are considered one of the excellent cathode materials for sodium-ion batteries due to their low cost and high theoretical specific capacity, especially sodium-rich iron-based PBAs (FeHCF) can provide higher energy density. FeHCF has a poor charge/discharge platform stability at high voltages (FeC6 moiety), which is mainly affected by its coordination environment. In this research, Cu+ (six-coordinated), which is close to the ionic radius of Fe2+, was used for substitution, the FeC6 vacancies of FeHCF were reduced, and the coordination environment was optimized. The low Cu+-substituted FeHCF (Cu+0.625) has an optimal electrochemical performance at 8.5 mA/g with a reversible specific capacity of 142 mA h/g and FeC6 moiety contribution of more than 68 mA h/g, which is superior to that of unmodified and other Cu2+-substituted FeHCFs. In situ tests demonstrate the reversible structural stability of the Cu+0.625, supporting the stability of their high-voltage platform capacity. This Cu+ substitution strategy further enriches the approach to optimize the coordination environment of sodium-rich FeHCF.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 752-759"},"PeriodicalIF":14.9,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156492","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Deciphering the function mechanism of high-valence tantalum doping in O3-types layered cathode for sodium-ion battery 钠离子电池o3型层状阴极中掺杂高价钽的作用机理

IF 14.9 1区化学

Journal of Energy Chemistry Pub Date : 2025-09-09 DOI: 10.1016/j.jechem.2025.08.078

Zixuan Huang , Zhi Long , Cheng Li , Kai Liu , Qingqing Zhang , Shiqiang Liu , Yayu Guo , Weili Sun , Wenyu Mu , Xixi Shi , Hongzhou Zhang , Na Zhang , Dawei Song , Lianqi Zhang

{"title":"Deciphering the function mechanism of high-valence tantalum doping in O3-types layered cathode for sodium-ion battery","authors":"Zixuan Huang , Zhi Long , Cheng Li , Kai Liu , Qingqing Zhang , Shiqiang Liu , Yayu Guo , Weili Sun , Wenyu Mu , Xixi Shi , Hongzhou Zhang , Na Zhang , Dawei Song , Lianqi Zhang","doi":"10.1016/j.jechem.2025.08.078","DOIUrl":"10.1016/j.jechem.2025.08.078","url":null,"abstract":"<div><div>O3-types layered cathode materials in sodium-ion batteries (SIBs) suffer from the obvious lattice distortion induced by the complex phase transitions during Na+ intercalation/deintercalation process, leading to severe structural collapse and performance degradation. Herein, a series of high valence tantalum (Ta5+) doped Na(Ni0.4Fe0.2Mn0.4)1−xTaxO2 (x = 0/0.0025/0.005/0.01) secondary spherical particles are firstly developed, where Ta5+ doping enables the refined primary grain with a tightly stacked rod-like morphology. Comprehensive structural analysis via Neutron powder diffraction (NPD) and Synchrotron radiation X-ray diffraction (SXRD) reveals an expanded NaO2 slab and a reduction in Na site vacancy. The potential charge compensation mechanism is further illustrated by X-ray absorption spectroscopy (XAS) and X-ray photoelectron spectroscopy (XPS), unveiling a partial reduction from Ni3+ to Ni2+ with Ta5+ doping. In situ X-ray diffraction (in situ XRD) suggests that the decorated sample undergoes a volume change as low as 0.8 %, in contrast with the pristine one (1.5 %). Thus, the optimized sample with x = 0.005 retains an enhanced capacity retention up to 70.4 % at 1 C after 300 cycles in half-cell and delivers a high energy density of 251 Wh kg−1 (0.1 C) and with a good capacity retention of 81.0 % at 1 C after 200 cycles in full-cell. Our findings provide new insights into the mechanism of high valence Ta5+ doping in stabilizing layered oxides cathode materials for SIBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 742-751"},"PeriodicalIF":14.9,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156493","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dipole-induced built-in electric field manipulation for regulating Zn electrodeposition topology in high-performance aqueous Zn ion storage 偶极感应内建电场操纵调节高性能水锌离子存储中锌电沉积拓扑结构

IF 14.9 1区化学

Journal of Energy Chemistry Pub Date : 2025-09-09 DOI: 10.1016/j.jechem.2025.08.070

Xin Wang , Zhiyuan Liu , Kaifa Dong , Pengyun Xie , Kanjun Sun , Hui Peng , Guofu Ma , Ziqiang Lei

{"title":"Dipole-induced built-in electric field manipulation for regulating Zn electrodeposition topology in high-performance aqueous Zn ion storage","authors":"Xin Wang , Zhiyuan Liu , Kaifa Dong , Pengyun Xie , Kanjun Sun , Hui Peng , Guofu Ma , Ziqiang Lei","doi":"10.1016/j.jechem.2025.08.070","DOIUrl":"10.1016/j.jechem.2025.08.070","url":null,"abstract":"<div><div>Aqueous Zn-ion storage offers high capacity and safety, but practical use is hindered by dendrite formation, side reactions, and hydrogen evolution, affecting stability and efficiency. Herein, tetramethylol acetylenediurea (TA) is proposed as an effective electrolyte additive that modulates the Zn2+ deposition environment via coordination competition. The polar functional groups of TA restructure the solvation sheath, while its molecular dipoles generate localized electric fields that accelerate Zn2+ migration and promote directional (002)-oriented deposition. These effects collectively suppress side reactions and enhance Zn plating/stripping reversibility. The four hydroxyl (–OH) and conjugated ketone groups (C=O) in the TA molecule have strong coordination ability (Lewis basicity) and can form a stable [Zn(TA)(H2O)n]2+ with Zn2+, reducing the number of free water molecules and the proportion of active water in the solvation sheath. The TA molecules are adsorbed onto the Zn anode surface, leading to the redistribution of the local spatial electric field and homogenization of ion flux dynamics. Its conjugated planar structure can induce Zn2+ to preferentially deposit along the (002) crystal plane. Zn//Zn symmetric cell using TA-containing ZnSO4 electrolyte exhibits stable cycling for more than 2240 h at 1 mA cm−2, 1 mAh cm−2. The Zn//activated carbon (AC) full-cell can stably cycle 30,000 cycles at 5 A g−1 with a capacity retention rate of 90 %. This study provides important insights into electrolyte engineering strategies for stabilizing Zn anodes, highlighting the potential of molecular design additives in next-generation Zn2+ energy storage systems.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 453-464"},"PeriodicalIF":14.9,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145119484","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Selective hydrogenation of CO2 to propene-abundant light olefins over ZnZrOx/ultra-small H-SAPO-34 crystals composite ZnZrOx/超小H-SAPO-34晶体复合材料上CO2选择性加氢制备富丙烯轻烯烃

IF 14.9 1区化学

Journal of Energy Chemistry Pub Date : 2025-09-09 DOI: 10.1016/j.jechem.2025.08.079

Lu Qin , Qian Zhang , Bo Zhou , Sen Wang , Pengfei Wang , Mei Dong , Tianfu Zhang , Lin Xu , Yu Wang , Ting Fan , Jianguo Wang , Weibin Fan

{"title":"Selective hydrogenation of CO2 to propene-abundant light olefins over ZnZrOx/ultra-small H-SAPO-34 crystals composite","authors":"Lu Qin , Qian Zhang , Bo Zhou , Sen Wang , Pengfei Wang , Mei Dong , Tianfu Zhang , Lin Xu , Yu Wang , Ting Fan , Jianguo Wang , Weibin Fan","doi":"10.1016/j.jechem.2025.08.079","DOIUrl":"10.1016/j.jechem.2025.08.079","url":null,"abstract":"<div><div>Significant increase of specific target olefin selectivity in CO2 hydrogenation is not only scientifically interesting but also practically valuable because of the reduction of separation cost. Here, a new composite catalyst is fabricated with surface oxygen vacancy-abundant ZnZrOx(H) solid solution and ultra-small H-SAPO-34(US) molecular sieve crystals. This catalyst shows a propene selectivity in hydrocarbons of 51.2 % that accounts for about 63 % of light olefins, along with a CO2 conversion of 13.5 %, at 350 °C and 3.0 MPa. A combination of in situ spectroscopy, isotope-labelled experiments, DFT calculations, and AIMD simulations reveals that an increase of surface oxygen vacancies in ZnZrOx(H) induces formation of a coordinatively unsaturated (Zr-O)n-Zn-(Ov)m configuration, which elevates Zn site electron density and enhances the electronic interaction of Zn-3d and H-1s orbitals. This promotes the H2 dissociation and facilitates methanol intermediate formation. The ultra-small H-SAPO-34(US) crystals with a size of 100–200 nm effectively suppresses alkenes hydrogenation and subsequent aromatization in the methanol conversion process. As a result, more propene was produced.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 542-552"},"PeriodicalIF":14.9,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156427","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dual‑salt electrolyte design enabled by synergistic solvation and interfacial regulation for fast charging of lithium‑ion batteries 双盐电解质设计，通过协同溶剂化和界面调节实现锂离子电池的快速充电

IF 14.9 1区化学

Journal of Energy Chemistry Pub Date : 2025-09-09 DOI: 10.1016/j.jechem.2025.08.071

Jun-Sen Jiang , Lan-Fang Que , Rui-Chi Li , Fu-Da Yu , Xuan Wang , Ji-Huai Wu , Can-Zhong Lu , Yi-Ming Xie

{"title":"Dual‑salt electrolyte design enabled by synergistic solvation and interfacial regulation for fast charging of lithium‑ion batteries","authors":"Jun-Sen Jiang , Lan-Fang Que , Rui-Chi Li , Fu-Da Yu , Xuan Wang , Ji-Huai Wu , Can-Zhong Lu , Yi-Ming Xie","doi":"10.1016/j.jechem.2025.08.071","DOIUrl":"10.1016/j.jechem.2025.08.071","url":null,"abstract":"<div><div>To address the performance limitations of conventional LiPF6-carbonate electrolytes under extreme temperatures and high-rate charging, lithium difluoro(oxalato)borate (LiDFOB) is introduced into the LiPF6-carbonate electrolyte to form a dual-salt system. The optimization mechanism enhancing the fast-charging capability of LiNi0.52Co0.2Mn0.28O2 (NCM523) cathode is systematically explored. Molecular dynamics simulations and electrochemical characterization demonstrate the reconstruction of Li+ solvation structures, expanding the voltage window and reducting Li+ desolvation barriers. In addition, the incorporation of LiDFOB induces the generation of a LiF/LixBOyFz-enriched cathode-electrolyte interphase, which effectively suppresses the dissolution of transition metals. In situ impedance measurements reveal the accelerated interfacial charge transfer kinetics. As expected, the NCM523 cathode achieves an 82 % state-of-charge (SOC) in 12 min at 5 C (25 °C) with 87 % capacity retention after 100 cycles, and exhibits a 65 % higher discharge capacity at 1 C than the baseline at −20 °C. The 1 Ah pouch cells based on LiNi0.52Co0.2Mn0.28O2 cathodes, graphite anodes, and 0.5 wt% LiDFOB-modified electrolyte demonstrate fast-charging capabilities: charging 97 % of the pouch cell capacity within 30 min (2 C) and 80 % within 15 min (4 C) at 25 °C. This study offers a practical electrolyte design strategy that enhances the fast-charging performance of lithium-ion batteries (LIBs) over a wide temperature range (from −20 to 25 °C).</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 484-494"},"PeriodicalIF":14.9,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145119568","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Designing an air electrode for dual ceramic cells using an ionic Lewis acid strength polarization distribution strategy 采用离子路易斯酸强度极化分布策略设计双陶瓷电池空气电极

IF 14.9 1区化学

Journal of Energy Chemistry Pub Date : 2025-09-09 DOI: 10.1016/j.jechem.2025.08.069

Ying Zhang , Yibei Wang , Zhilin Liu , Yaowen Wang , Zhen Wang , Youcheng Xiao , Bingbing Niu , Xiyang Wang , Guntae Kim , Wenquan Wang , Tianmin He

{"title":"Designing an air electrode for dual ceramic cells using an ionic Lewis acid strength polarization distribution strategy","authors":"Ying Zhang , Yibei Wang , Zhilin Liu , Yaowen Wang , Zhen Wang , Youcheng Xiao , Bingbing Niu , Xiyang Wang , Guntae Kim , Wenquan Wang , Tianmin He","doi":"10.1016/j.jechem.2025.08.069","DOIUrl":"10.1016/j.jechem.2025.08.069","url":null,"abstract":"<div><div>Ceramic cells promise ideal energy conversion and storage devices, making the development of efficient and robust air electrodes crucial for their application. In this study, a Ba0.4Sr0.5Cs0.1Co0.7Fe0.2Nb0.1O3−δ (BSCCFN) air electrode, based on Ba0.5Sr0.5Co0.8Fe0.2O3−δ (BSCF), is designed using a perovskite A-B-site ionic Lewis acid strength (ISA) polarization distribution strategy and is successfully applied in both oxygen-ion conducting solid oxide fuel cells (O-SOFCs) and proton-conducting reversible protonic ceramic cells (R-PCCs). When BSCCFN is used as the air electrode in O-SOFCs, a peak power density (PPD) of 1.45 W cm−2 is achieved at 650 °C, whereas in R-PCCs, a PPD of 1.13 W cm−2 and a current density of −1.8 A cm−2 at 1.3 V are achieved at the same temperature and show stable reversibility over 100 h. Experimental measurements and theoretical calculations demonstrate that low-ISA Cs+ doping accelerates the reaction kinetics of both oxygen ions and protons, while high-ISA Nb5+ doping enhances electrode stability. The synergistic effect of Cs+ and Nb5+ co-doping in the BSCCFN electrode lies in the ISA polarization distribution, which weakens the Co/Fe–O bond covalency, thereby promoting oxygen vacancy formation and facilitating the conduction of oxygen ions and protons.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 505-516"},"PeriodicalIF":14.9,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145119567","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A theory perspective of the polysulfide absorbing materials for room-temperature sodium-sulfur batteries 室温钠硫电池用多硫吸收材料的理论展望

IF 14.9 1区化学

Journal of Energy Chemistry Pub Date : 2025-09-08 DOI: 10.1016/j.jechem.2025.08.066

Chhail Bihari Soni , Vipin Kumar

{"title":"A theory perspective of the polysulfide absorbing materials for room-temperature sodium-sulfur batteries","authors":"Chhail Bihari Soni , Vipin Kumar","doi":"10.1016/j.jechem.2025.08.066","DOIUrl":"10.1016/j.jechem.2025.08.066","url":null,"abstract":"<div><div>Though the formation of polysulfide is desirable, as it contributes to the capacity build-up, it must not leak into the electrolyte. The loss of polysulfide causes capacity fade, a change in thelocal chemistry of the electrolyte, and anode poisoning. Constant efforts are in progress to find suitable polysulfide-absorbing materials; however, the magical polysulfide absorber is yet to be discovered or developed. Experimental methods alone often fall short in accelerating the investigations may be due to thecomplex Nature of the testing. This review focuses on the importance of computational methods, particularly density functional theory (DFT), in screening suitable polysulfide absorbers. It highlights the critical role of anchoring materials in improving Na-S battery performance, including pristine and doped graphene, metal–organic frameworks, carbon Nanofibers, vanadium disulfide, MXenes, and metal sulfides. By examining adsorption energies, charge transfer mechanisms, and catalytic properties, this review provides insights into the design of advanced materials that can effectively immobilize polysulfides and enhance battery stability. The review aims to guide future research efforts toward the development of high-performance RT Na-S batteries through a comprehensive understanding of the polysulfide-absorbing materials.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 584-604"},"PeriodicalIF":14.9,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156430","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Controllable phase-reconstruction strategy for LiFePO4 homogeneous regeneration: reaction mechanism, characterization and prospect LiFePO4均相再生的可控相重构策略：反应机理、表征及展望

IF 14.9 1区化学

Journal of Energy Chemistry Pub Date : 2025-09-06 DOI: 10.1016/j.jechem.2025.08.065

Zihao Zeng , Yi Chen , Chao Zhu, Hai Lei, Wei Sun, Yue Yang, Peng Ge

{"title":"Controllable phase-reconstruction strategy for LiFePO4 homogeneous regeneration: reaction mechanism, characterization and prospect","authors":"Zihao Zeng , Yi Chen , Chao Zhu, Hai Lei, Wei Sun, Yue Yang, Peng Ge","doi":"10.1016/j.jechem.2025.08.065","DOIUrl":"10.1016/j.jechem.2025.08.065","url":null,"abstract":"<div><div>The growing volume of end-of-life lithium-ion batteries (LIBs) represents both an urgent environmental challenge and a critical resource opportunity, especially for cathode materials. Among commercial cathodes, LiFePO4 (LFP) dominates the market due to its favorable properties; thus, a substantial amount of LFP cathode materials is expected to retire in the near future. The conventional hydrometallurgical method suffers from high costs and serious pollution. Direct regeneration technologies, especially solid-state sintering, provide a more efficient and environmentally benign alternative by repairing cathode structures through high-temperature solid-phase reactions without extra chemical reagents. Traditional solid-state sintering faces challenges in processing spent LFP from diverse sources, struggling to achieve the homogenization of physical–chemical properties and electrochemical performance. To address the limitations above, phase homogenization with a lattice reconstruction strategy has been investigated, which can enable effective lattice reconstruction and microstructural homogenization, demonstrating robust adaptability to spent samples from variable sources. This review systematically summarizes the mechanisms, detailed steps, characterization techniques, and advances in pre-oxidation optimization (including ion-doping and coated carbon layer modification), as well as future research directions for sustainable LFP recycling. Given this, this review is expected to offer theoretical guidance for achieving homogeneous regeneration of LFP cathode.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 553-571"},"PeriodicalIF":14.9,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156425","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Oxygenation promoting Se-coordination of amorphous adjacent Nb-Nb diatomic pairs for high-performance sodium-ion hybrid capacitors 用于高性能钠离子杂化电容器的氧化促进非晶相邻Nb-Nb双原子对的硒配位

IF 14.9 1区化学

Journal of Energy Chemistry Pub Date : 2025-09-06 DOI: 10.1016/j.jechem.2025.08.067

Wenxiu He , Fanyan Zeng , Bowen Liao , Qincheng Zheng , Dui Ma , Meilan Xie , Yang Pan

{"title":"Oxygenation promoting Se-coordination of amorphous adjacent Nb-Nb diatomic pairs for high-performance sodium-ion hybrid capacitors","authors":"Wenxiu He , Fanyan Zeng , Bowen Liao , Qincheng Zheng , Dui Ma , Meilan Xie , Yang Pan","doi":"10.1016/j.jechem.2025.08.067","DOIUrl":"10.1016/j.jechem.2025.08.067","url":null,"abstract":"<div><div>Transition metal selenides as sodium-ion hybrid capacitor (SIHC) anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution. Herein, an atomistic amorphous strategy is proposed to construct adjacent Nb-Nb diatomic pairs with Se/O-coordination (Se4-Nb2-O2) in N-doped carbon-confined amorphous selenide clusters (a-Nb-Se/O@NC). Synergistic carbon confinement and hydrothermal oxygenation induce amorphization of Nb–Se bonds, eliminating crystalline rigidity while creating isotropic dual-ion transport channels and high-density active sites enriched with dangling bonds, thereby enhancing structural integrity and Na+ storage capacity. The unique Se/O-coordinated Nb-Nb diatomic configuration establishes an electron-delocalized system, where the low electronegativity of Se counterbalances electron withdrawal from coordinated O at Nb centers. These strengthen d-p orbital hybridization, reduce Na+ adsorption energy, and optimize charge transfer pathways and reaction kinetics in the amorphous clusters. Electrochemical tests reveal that the a-Nb-Se/O@NC anode delivers a high reversible capacity of 312.57 mAh g−1 and exceptional cyclic stability (103 % capacity retention) after 5000 cycles at 10.0 A g−1. Assembled SIHCs achieve outstanding energy/power densities (207.1 Wh kg−1/18966 W kg−1), surpassing most amorphous and crystalline counterparts. This work provides methodological insights for the design of electrodes in high-power storage devices through atomic modulation and electronic optimization of amorphous selenides.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 474-483"},"PeriodicalIF":14.9,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145119531","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cationic covalent framework microenvironment steering CuPt alloy toward record-breaking photoelectrochemical ethane synthesis from CO2 阳离子共价框架微环境引导CuPt合金走向破纪录的CO2光化学乙烷合成

IF 14.9 1区化学

Journal of Energy Chemistry Pub Date : 2025-09-04 DOI: 10.1016/j.jechem.2025.08.062

Fentahun Wondu Dagnaw , Karim Harrath , Tao Zheng , Yu-Ze Liu , Huiwen Xue , Wei Li , Ze-Yu Zhang , Zhen Li , Xu-Bing Li , Huaping Wang , Qing-Xiao Tong , Jing-Xin Jian

{"title":"Cationic covalent framework microenvironment steering CuPt alloy toward record-breaking photoelectrochemical ethane synthesis from CO2","authors":"Fentahun Wondu Dagnaw , Karim Harrath , Tao Zheng , Yu-Ze Liu , Huiwen Xue , Wei Li , Ze-Yu Zhang , Zhen Li , Xu-Bing Li , Huaping Wang , Qing-Xiao Tong , Jing-Xin Jian","doi":"10.1016/j.jechem.2025.08.062","DOIUrl":"10.1016/j.jechem.2025.08.062","url":null,"abstract":"<div><div>Photoelectrochemical CO2 reduction to multi-carbon products fuels remains challenged by inefficient C–C coupling and competing proton reduction reaction. Herein, we designed a cationic covalent organic framework (COF+) to create an electrostatic microenvironment that synergizes with CuPt alloy nanoparticles for selective ethylene/ethane production. By spatially decoupling CO2 enrichment from proton exclusion, the COF+/CuPt interface simultaneously facilitates CO2 accessibility while impeding H+ migration, suppressing the hydrogen evolution reaction (HER). This unique microenvironment stabilizes key anionic intermediates (*COO−, *OCCO−) and promotes *CO dimerization, steering electron transfer toward C–C coupling. The optimized system achieves a record-high Faradaic efficiency of 51.5 %±5.3 % for ethane and 10.6 %±2.5 % for ethylene with a total C2+ yield exceeding 62 % at −0.25 V vs. RHE and high stability (>300 min), representing the highest performance for photoelectrochemical CO2 reduction to ethane. The combined analyses of in situ spectroscopy and theoretical calculations reveal that electrostatic field effects lower the energy barrier for *OCCO formation while accelerating hydrogenation kinetics. Therefore, this work demonstrates that microenvironment modification of the active site by cationic covalent organic framework is a versatile strategy for solar-driven CO2 conversion into value-added hydrocarbons.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 339-349"},"PeriodicalIF":14.9,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145107755","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0