Journal of Energy Chemistry最新文献

{"title":"Constructing a high-performance magnesium single-atom catalyst for the transfer hydrogenation of biomass-derived carbonyl compounds in ethanol","authors":"Lei Hu ,&nbsp;Mengxue Liu ,&nbsp;Baogang Sha ,&nbsp;Jiacheng Li ,&nbsp;Aiyong He ,&nbsp;Xing Tang ,&nbsp;Zhen Wu ,&nbsp;Lu Lin","doi":"10.1016/j.jechem.2025.08.064","DOIUrl":"10.1016/j.jechem.2025.08.064","url":null,"abstract":"<div><div>Endogenous hydrogen systems, consisting of metal–organic coordination catalysts and alcohols, have been widely applied for the transfer hydrogenation (TH) of biomass-derived carbonyl compounds in recent years. Metal-organic coordination catalysts showed satisfactory ability of TH in the secondary alcohols, but most of them could not effectively employ the cheaper primary alcohols as hydrogen donors. Furthermore, they commonly contained high metal contents, which also led to low catalytic efficiency in significant measure. In this work, we constructed a novel magnesium single-atom catalyst (Mg-NC) with merely 0.37 wt% Mg by means of a combined self-assembly and pyrolysis strategy. The characterization results indicated that Mg was atomically dispersed and it was coordinated with four pyridinic-N in Mg-NC. Due to the obvious electron transfer from Mg to its coordinated pyridinic-N, Mg–N₄ active centers displayed high Lewis acid-base strength with abundant content, which brought remarkable catalytic activity. When Mg-NC was used for the TH of 5-hydroxymethylfurfural (HMF) in ethanol (EtOH), 2,5-bis(hydroxymethyl)furan (BHMF) yield was up to 96.3 % with high productivity of 19.85 mol_BHMF mol_Mg⁻¹ h⁻¹ at 150 °C for 5 h. More interestingly, the process of TH over Mg-NC in EtOH was proved to proceed via the hydrogen radical mechanism. Additionally, Mg-NC exhibited powerful catalytic universality; it could not only utilize other primary alcohols (such as <em>n</em>-propanol and <em>n</em>-butanol) as hydrogen donors, but also catalyze the TH of other carbonyl compounds (such as furfural, 5-methylfurfural, benzaldehyde, cyclohexanone, and levulinic acid). Overall, this work offered some important clues and references to reinforce the hydrogen-supplying ability of primary alcohols in the TH of various biomass-derived carbonyl compounds to high-value fine chemicals.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 517-531"},"PeriodicalIF":14.9,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145109750","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}

{"title":"Self-healing of manganese Prussian blue analogues via thermodynamically driven in situ engineered nickel cages in electrochemical processes","authors":"Yichao Wang,&nbsp;Ning Jiang,&nbsp;Lingbo Yao,&nbsp;Shouyu Sun,&nbsp;Cheng Yang,&nbsp;Yu Liu","doi":"10.1016/j.jechem.2025.08.063","DOIUrl":"10.1016/j.jechem.2025.08.063","url":null,"abstract":"<div><div>Although manganese Prussian blue analogues (Mn-PBAs) offer advantages as cost-effective, high-energy-density cathode materials for sodium-ion batteries, their practical application is severely constrained by substantial capacity degradation during long-term cycling. This performance deterioration is closely associated with the structural instability of the material during the cycling process, which is mainly attributed to the gradual dissolution of the active material into the electrolyte and severe lattice distortion during Na⁺ intercalation/deintercalation. Fortunately, the aforementioned challenges can be effectively addressed by fabricating an in situ engineered nickel cage (ISE-NC) on Mn-PBAs (denoted as Mn-PBAs-NC). Experimental characterization combined with theoretical calculations reveals that this spontaneously formed nickel cage not only suppresses the diffusion of Mn-PBAs into the electrolyte but also acts as a structural stabilizer, significantly alleviating lattice distortion during cycling. This dual stabilization mechanism ensures remarkable cycling stability, with Mn-PBAs-NC delivering a retained capacity of 96.4 mA h g⁻¹ (80 % capacity retention) over 2,300 cycles at 2 C, elevating the cycle life of Mn-PBAs to unprecedented levels.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 532-541"},"PeriodicalIF":14.9,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156429","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}

{"title":"Unified physics-informed subspace identification and transformer learning for lithium-ion battery state-of-health estimation","authors":"Yong Li ,&nbsp;Hao Wang ,&nbsp;Chenyang Wang ,&nbsp;Liye Wang ,&nbsp;Chenglin Liao ,&nbsp;Lifang Wang","doi":"10.1016/j.jechem.2025.08.060","DOIUrl":"10.1016/j.jechem.2025.08.060","url":null,"abstract":"<div><div>The growing use of lithium-ion batteries in electric transportation and grid-scale storage systems has intensified the need for accurate and highly generalizable state-of-health (SOH) estimation. Conventional approaches often suffer from reduced accuracy under dynamically uncertain state-of-charge (SOC) operating ranges and heterogeneous aging stresses. This study presents a unified SOH estimation framework that integrates physics-informed modeling, subspace identification, and Transformer-based learning. A reduced-order model is derived from simplified electrochemical dynamics, providing an interpretable and computationally efficient representation of battery behavior. Subspace identification across a wide SOC and SOH range yields degradation-sensitive features, which the Transformer uses to capture long-range aging dynamics via multi-head self-attention. Experiments on LiFePO₄ cells under joint-cell training show consistently accurate SOH estimation, with a maximum error of 1.39 %, demonstrating the framework’s effectiveness in decoupling SOC and SOH effects. In cross-cell validation, where training and validation are performed on different cells, the model maintains a maximum error of 2.06 %, confirming strong generalization to unseen aging trajectories. Comparative experiments on LiFePO₄ and public LiCoO₂ datasets confirm the framework’s cross-chemistry applicability. By extracting low-dimensional, physically interpretable features via subspace identification, the framework significantly reduces training cost while maintaining high SOH estimation accuracy, outperforming conventional data-driven models lacking physical guidance.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 350-369"},"PeriodicalIF":14.9,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145108141","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}

{"title":"Synergistic lock-anchor engineered diketopyrrolopyrrole-COFs for efficient photocatalytic uranium extraction","authors":"Fengtao Yu ,&nbsp;Xiaolong Zhang ,&nbsp;Jie Xu ,&nbsp;Guihong Wu ,&nbsp;Huiying Lei ,&nbsp;Zhiwu Yu ,&nbsp;Jianding Qiu ,&nbsp;Jianli Hua","doi":"10.1016/j.jechem.2025.08.061","DOIUrl":"10.1016/j.jechem.2025.08.061","url":null,"abstract":"<div><div>As a key low-carbon energy source, nuclear power plays a vital role in the global transition toward sustainable energy. Photocatalytic uranium extraction from seawater (UES) offers a promising solution to ensure long-term uranium supply but is challenged by ultra-low uranium concentrations and ion interference. To overcome these issues, we design three diketopyrrolopyrrole-based covalent organic frameworks (COFs) via a synergistic π-extended lock and carboxyl-functionalized anchor molecular engineering strategy. Among them, TPy-DPP-COF features a covalently locked π-conjugated structure that enhances planarity, optimizes energy alignment, and minimizes exciton binding energy, thereby promoting charge transfer and suppressing recombination. Concurrently, carboxyl groups enable uranyl-specific coordination and create local electric fields to facilitate charge separation. These features contribute to the outstanding performance of TPy-DPP-COF, which achieves a high uranium adsorption capacity of 16.33 mg g⁻¹ in natural seawater under irradiation, with only 29.3 % capacity loss after 10 cycles, surpassing industrial benchmarks. Density functional theory (DFT) calculations and experimental studies reveal a synergistic photocatalysis-adsorption pathway, with DPP units acting as active sites for uranium reduction. This work highlights a molecular design strategy for developing efficient COF-based photocatalysts for practical marine uranium recovery.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 284-293"},"PeriodicalIF":14.9,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145107749","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}

{"title":"Temporally stepwise crystallization via dual-additive orchestration: resolving the crystallinity-domain size paradox for high-efficiency organic photovoltaics","authors":"Huan Wang ,&nbsp;Zemin He ,&nbsp;Xingpeng Liu ,&nbsp;Jingming Xin ,&nbsp;Ziqi Geng ,&nbsp;Kuan Yang ,&nbsp;Yutong Zhang ,&nbsp;Yan Zhang ,&nbsp;Mingzhi Duan ,&nbsp;Bei Qin ,&nbsp;Qiuju Liang ,&nbsp;Jiangang Liu","doi":"10.1016/j.jechem.2025.08.059","DOIUrl":"10.1016/j.jechem.2025.08.059","url":null,"abstract":"<div><div>Achieving simultaneous enhancement of crystallinity and optimal domain size remains a fundamental challenge in organic photovoltaics (OPVs), where conventional crystallization strategies often trigger excessive aggregation of small-molecule acceptors. This work pioneers a kinetic paradigm for resolving the crystallinity-domain size trade-off in organic photovoltaics through dual-additive-guided stepwise crystallization. By strategically pairing 1,2-dichlorobenzene (<em>o</em>-DCB, low binding energy to Y6) and 1-fluoronaphthalene (FN, high binding energy), we achieve temporally decoupled crystallization control: <em>o</em>-DCB first mediates donor-acceptor co-crystallization during film formation, constructing a metastable network, whereupon FN induces confined Y6 crystallization within this framework during thermal annealing, refining nanostructure without over-aggregation. Morphology studies reveal that this synergy enhances crystallinity of (100) diffraction peaks by 21 %–10 % versus single-additive controls (<em>o</em>-DCB/FN alone), while maintaining optimal domain size. These morphological advantages yield balanced carrier transport (<em>μ</em>_h/<em>μ</em>_e = 1.23), near-unity exciton dissociation (98.53 %), and a champion power conversion efficiency (PCE) of 18.08 % for PM6:Y6, significantly surpassing single-additive devices (<em>o</em>-DCB: 17.20 %; FN: 17.53 %). Crucially, the dual-additive strategy demonstrates universal applicability across diverse active layer systems, achieving an outstanding PCE of 19.27 % in PM6:L8-BO-based devices, thereby establishing a general framework for morphology control in high-efficiency OPVs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 370-383"},"PeriodicalIF":14.9,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145108142","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}

{"title":"Highly stable lithium metal batteries enabled by nanometric anion aggregates reinforced solvation structure in locally concentrated ionic liquid electrolytes","authors":"Haifeng Tu ,&nbsp;Zhiyong Tang ,&nbsp;Haiyang Zhang ,&nbsp;Zhicheng Wang ,&nbsp;Jiangyan Xue ,&nbsp;Shiqi Zhang ,&nbsp;Zheng Liu ,&nbsp;Yiwen Gao ,&nbsp;Peng Ding ,&nbsp;Yi Yang ,&nbsp;Guangye Wu ,&nbsp;Suwan Lu ,&nbsp;Lingwang Liu ,&nbsp;Guan Wu ,&nbsp;Qing Wang ,&nbsp;Byoungwoo Kang ,&nbsp;Jingjing Xu ,&nbsp;Hong Li ,&nbsp;Xiaodong Wu","doi":"10.1016/j.jechem.2025.08.053","DOIUrl":"10.1016/j.jechem.2025.08.053","url":null,"abstract":"<div><div>The practical application of lithium metal batteries (LMBs) requires electrolytes that simultaneously ensure high safety and interfacial stability. Although locally concentrated ionic liquid electrolytes (LCILEs) exhibit exceptional electrochemical stability and compatibility with electrode electrolyte interfaces (EEIs), two major challenges persist: (i) safety risks caused by excessive low-flash-point diluents, and (ii) insufficient understanding of how diluents modulate solvation structures. Herein, we introduce a low-diluent-content LCILE system composed of lithium bis(fluorosulfonyl)imide (LiFSI) salt, N-methyl-N-propyl-pyrrolidinium bis(fluorosulfonyl)imide (Pyr₁₃FSI) ionic liquid, and trifluoromethanesulfonate (TFS) diluent. The TFS diluent strengthens ion-ion interactions by lowering the dielectric constant of the electrolyte, resulting in the formation of a unique nanometric anion aggregates (N-AGGs) reinforced solvation structure. These large anionic clusters exhibit accelerated redox decomposition kinetics, facilitating the rapid formation of a thin, dense, and low-impedance EEI. Consequently, the Li/LiNi_0.6Co_0.2Mn_0.2O₂ coin cell achieves 87.8 % capacity retention over 300 cycles at 4.3 V, while a practical 1.4 Ah Li/NCM622 pouch cell retains 84.5 % capacity after 80 cycles at 4.5 V. Furthermore, the electrolyte demonstrates exceptional safety, and 2 Ah Li metal pouch cells successfully pass rigorous nail penetration tests without any ignition or explosion. This work not only provides a design strategy for intrinsically safe and high-performance electrolytes but also highlights the critical role of anion cluster decomposition kinetics in shaping EEI formation.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 251-260"},"PeriodicalIF":14.9,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145108146","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}

{"title":"Redefining atomistic simulations of all-solid-state batteries through machine learning interatomic potentials","authors":"Qian Chen,&nbsp;Siwen Wang,&nbsp;Chen Ling","doi":"10.1016/j.jechem.2025.08.058","DOIUrl":"10.1016/j.jechem.2025.08.058","url":null,"abstract":"<div><div>All-solid-state batteries (ASSBs) represent a next-generation energy storage technology, offering enhanced safety, higher energy density, and improved cycling stability compared to conventional liquid-electrolyte-based lithium-ion batteries. Understanding and optimizing the complex chemistries and interfaces that underpin ASSB performance present significant challenges from both experimental and modeling perspectives. In particular, atomistic simulations face difficulties in capturing the complex structure, disorder, and dynamic evolution of materials and interfaces under practically relevant conditions. While established methods such as density functional theory and classical force fields have provided valuable insights, some questions remain difficult to address, particularly those involving large system sizes or long timescales. Recently, machine learning interatomic potentials (MLIPs) have emerged as a transformative tool, enabling atomistic simulations at length and time scales that were previously challenging to access with conventional approaches. By delivering near first-principles accuracy with much greater efficiency, MLIPs open new avenues for large-scale, long-timescale, and high-throughput simulations of solid-state battery materials. In this review, we present a comparative overview of density functional theory, classical force fields, and MLIPs, highlighting their respective strengths and limitations in ASSB research. We then discuss how MLIPs enable simulations that reach longer timescales, larger system sizes, and support high-throughput calculations, providing unique insights into ion transport and interfacial evolution in ASSBs. Finally, we conclude with a summary and outlook on current challenges and future opportunities for expanding MLIP capabilities and accelerating their impact in solid-state battery research.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 666-687"},"PeriodicalIF":14.9,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145156491","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}

{"title":"Enhanced mechanical strength and improved Li+ transport in PEO-based electrolytes via scalable bicontinuous PMIA porous membrane","authors":"Honggui He ,&nbsp;Chuqing Tang ,&nbsp;Zhaozhao Peng ,&nbsp;Mengjie Fan ,&nbsp;Ming Jiang ,&nbsp;Dan Li ,&nbsp;Weimin Kang ,&nbsp;Xiaoyin Wang ,&nbsp;Nanping Deng ,&nbsp;Lu Gao ,&nbsp;Xupin Zhuang","doi":"10.1016/j.jechem.2025.08.045","DOIUrl":"10.1016/j.jechem.2025.08.045","url":null,"abstract":"<div><div>The low ionic conductivity and poor mechanical strength of polyethylene oxide (PEO)-based electrolytes severely restrict their practical application. To address this problem, this work designs a scalable, high-strength (24.3 MPa) bicontinuous porous poly (m-phthaloyl-m-phenylenediamine) (PMIA) membrane integrated into PEO/LiTFSI (PL), thus forming a PMIA/PEO/LiTFSI (PPL) composite electrolyte. Compared to the PL electrolyte, the PPL electrolyte reinforced by a bicontinuous porous PMIA membrane exhibits significantly enhanced mechanical strength, reaching 13.4 MPa. In addition, the amide groups on PMIA strongly coordinate with LiTFSI and form hydrogen bonds with PEO, promoting Li salt dissociation and reducing the Li⁺ migration barrier. This creates efficient, fast Li⁺ transport channels at the PMIA/PL interfaces, effectively promoting the uniform Li⁺ deposition and minimizing lithium dendrite formation. The PPL electrolyte achieves high ionic conductivity (1×10⁻⁴ S cm⁻¹ at 30 °C) and Li⁺ transference number (<em>t</em>_Li⁺=0.43). The assembled LiFePO₄/Li battery demonstrates excellent cycling stability, retaining 80% capacity after 2000 cycles at 2 C, while the Li/Li symmetric cell operates stably for over 900 h at 0.3 mA cm⁻². Therefore, the scalable porous PMIA membrane effectively enhances both the mechanical strength and Li⁺ transport in PEO-based electrolytes, offering a viable strategy for their commercial-scale implementation.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 183-197"},"PeriodicalIF":14.9,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145107747","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}

{"title":"A comprehensive review of remaining useful life prediction methods for lithium-ion batteries: Models, trends, and engineering applications","authors":"Yang Li ,&nbsp;Haotian Shi ,&nbsp;Shunli Wang ,&nbsp;Qi Huang ,&nbsp;Chunmei Liu ,&nbsp;Shiliang Nie ,&nbsp;Xianyi Jia ,&nbsp;Tao Luo","doi":"10.1016/j.jechem.2025.08.056","DOIUrl":"10.1016/j.jechem.2025.08.056","url":null,"abstract":"<div><div>Under complex working conditions, accurate prediction of the remaining useful life (RUL) of lithium-ion batteries is of great significance to ensure the stable operation of energy storage systems, the safe driving of electric vehicles, and the continuous power supply of electronic devices. This paper systematically describes the RUL prediction methods of lithium-ion batteries and comprehensively summarizes the development status and future trends in this field. First, the battery degradation mechanisms and lightweight data acquisition are analyzed. Secondly, a systematic classification model is constructed for the more widely used lithium battery RUL prediction methods, and the application characteristics and implementation limitations of different methods are analyzed in detail. An innovative classification framework for hybrid methods is proposed based on the depth of physical-data interaction. Then, collaborative modelling of calendar ageing and cyclic ageing is discussed, revealing their coupled effects and corresponding RUL prediction methods. Finally, the technical bottlenecks faced by the current RUL prediction of lithium batteries are identified, potential solutions are proposed, and the future development trends are outlined.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 384-414"},"PeriodicalIF":14.9,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145108150","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}

{"title":"Tandem catalysis over Cu@Co/CoFe-P metal-alloy heterostructure achieving ampere-level nitrate-to-ammonia electrosynthesis","authors":"Laiji Xu ,&nbsp;Wei Guo ,&nbsp;Simeng Yu ,&nbsp;Zhenlin Mo ,&nbsp;Jiangzhou Qin ,&nbsp;Yiwen Chen ,&nbsp;Baojun Liu","doi":"10.1016/j.jechem.2025.08.057","DOIUrl":"10.1016/j.jechem.2025.08.057","url":null,"abstract":"<div><div>The electrocatalytic reduction of nitrate to ammonia (NO₃⁻RR) offers a sustainable alternative to energy-intensive industrial NH₃ synthesis. Tandem catalysis has shown promise in overcoming the multi-step complexity of NO₃⁻RR, yet challenges remain in optimizing performance and elucidating tandem mechanisms. Herein, we report a Cu@Co/CoFe-P tandem electrocatalyst featuring a phosphorus-doped heterostructure with dual active sites (Cu-P and Co/CoFe-P). This catalyst achieves an exceptional NH₃ yield of 175.40 mg h⁻¹ cm⁻² and a record-high current density exceeding 2 A cm⁻², with the electro-synthesized NH₃ directly converted into NH₄Cl. In situ spectroscopic analysis and density functional theory (DFT) calculations reveal a novel desorption-reactivation tandem mechanism: (1) the Cu-P domain preferentially reduces NO₃⁻ to *NO₂, which desorbs as stable NO₂⁻; (2) the Co/CoFe-P domain subsequently reactivates NO₂⁻, and converts it efficiently into NH₃. Moreover, phosphorus doping enhances *H supply, while Fe alloying with Co promotes NO₂⁻ hydrogenation, ensuring an efficient and synchronized tandem pathway for NO₃⁻RR. The proposed *NO₂ desorption-reactivation mechanism deepens the understanding of NO₃⁻RR tandem process, thereby paving the way for designing more efficient tandem electrocatalysts.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 329-338"},"PeriodicalIF":14.9,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145107754","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}