Traditional strong metal-support interactions (SMSIs) induced by encapsulated reducible oxide overlayers on metal nanoparticles can suppress sintering but has a strong negative impact on the catalytic activity because of decreased availability of active sites. Herein, we design three SMSIs configurations on Pt-TiO2 via crystal-phase engineering. These configurations comprised encapsulated Pt nanoparticle (NPs) with TiO2−x overlayer on anatase, weakly embedded Pt clusters on P25, and deeply embedded PtOx-induced Pt single-atom (SA) structure on rutile. These configurations exhibited Pt species at multiple scales, ranging from NPs to SAs. Among them, Pt supported rutile TiO2 sample (Pt-TiO2(R)-H) achieved extremely low CO selectivity (2.05%, 200 °C) and optimal H2 production performance due to the enhanced SMSIs from Pt–Ti coordination in the deeply embedded PtOx region. This Pt–Ti coordination facilitated the electron transfer from Pt to Ti and induced dual-function centers of electron-deficient Ptδ+–Pt2+ pairs (0 < δ < 2, where Ptδ+ represent Pt SAs) for methanol decomposition and electron-rich Ti3+–oxygen vacancies for water dissociation. Such unique configuration altered the MSR reaction pathway and the kinetic rates of each elementary step in these reaction pathways were systematically analyzed. This work proposes an SMSIs configuration induced by a deeply embedded structure, which mitigates the negative impact on catalytic activity from encapsulated overlayers, meanwhile providing a strategy for developing high-loading Pt SAs catalysts.
{"title":"Boosting methanol steam reforming performance via crystal-phase-driven strong metal-support interactions: From encapsulated Pt nanoparticles to deeply embedded PtOx-induced Pt single atoms","authors":"Zheng Wei, Shengfang Shi, Fei Dong, Hekun Jia, Zhiling Chen, Hongqi Wang, Bifeng Yin","doi":"10.1016/j.jechem.2025.12.054","DOIUrl":"10.1016/j.jechem.2025.12.054","url":null,"abstract":"<div><div>Traditional strong metal-support interactions (SMSIs) induced by encapsulated reducible oxide overlayers on metal nanoparticles can suppress sintering but has a strong negative impact on the catalytic activity because of decreased availability of active sites. Herein, we design three SMSIs configurations on Pt-TiO<sub>2</sub> via crystal-phase engineering. These configurations comprised encapsulated Pt nanoparticle (NPs) with TiO<sub>2−</sub><em><sub>x</sub></em> overlayer on anatase, weakly embedded Pt clusters on P25, and deeply embedded PtO<em><sub>x</sub></em>-induced Pt single-atom (SA) structure on rutile. These configurations exhibited Pt species at multiple scales, ranging from NPs to SAs. Among them, Pt supported rutile TiO<sub>2</sub> sample (Pt-TiO<sub>2</sub>(R)-H) achieved extremely low CO selectivity (2.05%, 200 °C) and optimal H<sub>2</sub> production performance due to the enhanced SMSIs from Pt–Ti coordination in the deeply embedded PtO<em><sub>x</sub></em> region. This Pt–Ti coordination facilitated the electron transfer from Pt to Ti and induced dual-function centers of electron-deficient Pt<em><sup>δ</sup></em><sup>+</sup>–Pt<sup>2+</sup> pairs (0 < <em>δ</em> < 2, where Pt<em><sup>δ</sup></em><sup>+</sup> represent Pt SAs) for methanol decomposition and electron-rich Ti<sup>3+</sup>–oxygen vacancies for water dissociation. Such unique configuration altered the MSR reaction pathway and the kinetic rates of each elementary step in these reaction pathways were systematically analyzed. This work proposes an SMSIs configuration induced by a deeply embedded structure, which mitigates the negative impact on catalytic activity from encapsulated overlayers, meanwhile providing a strategy for developing high-loading Pt SAs catalysts.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"116 ","pages":"Pages 262-278"},"PeriodicalIF":14.9,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146025035","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}
Pub Date : 2026-05-01Epub Date: 2026-01-18DOI: 10.1016/j.jechem.2026.01.011
Jun Cong , Shaohua Luo
This review summarizes the cutting-edge applications of artificial intelligence (AI) technology in the development and performance optimization of key materials for sodium-ion batteries (SIBs), with a primary focus on its breakthrough advancements in the innovation of cathode and anode materials. It highlights the pivotal role of AI in accelerating the discovery and optimization process of high-performance SIB materials. In the research and development of cathode materials, AI technology, through machine learning and deep learning algorithms, assists in the design of layered oxides and poly-anion compounds, optimizes the ratio of transition metals and crystal structure, and enhances the kinetics of Na+ intercalation/deintercalation and structural stability. In terms of anode materials, AI technology leverages data-driven high-throughput screening strategies and microstructural modulation models to drive breakthroughs in key performance metrics such as sodium storage capacity and rate capability for hard carbon, alloy-based, and conversion-type anode materials. AI technology successfully establishes a new development paradigm of “data-driven, mechanism-embedded”, achieving full-chain coverage from atomic-scale material design to system-level performance optimization, significantly reducing development cycle and costs. Based on a summary of the current application status of AI technology in the development of SIBs materials, this review further analyzes the challenges that this field is facing, and at the same time looks forward to the development opportunities of the in-depth integration of AI and experimental research and development, providing innovative methodological support and direction guidance for promoting the industrialization process of high-performance SIBs.
{"title":"Artificial intelligence empowering innovation in key materials for sodium-ion batteries: Machine learning driven design and optimization of cathode and anode materials","authors":"Jun Cong , Shaohua Luo","doi":"10.1016/j.jechem.2026.01.011","DOIUrl":"10.1016/j.jechem.2026.01.011","url":null,"abstract":"<div><div>This review summarizes the cutting-edge applications of artificial intelligence (AI) technology in the development and performance optimization of key materials for sodium-ion batteries (SIBs), with a primary focus on its breakthrough advancements in the innovation of cathode and anode materials. It highlights the pivotal role of AI in accelerating the discovery and optimization process of high-performance SIB materials. In the research and development of cathode materials, AI technology, through machine learning and deep learning algorithms, assists in the design of layered oxides and poly-anion compounds, optimizes the ratio of transition metals and crystal structure, and enhances the kinetics of Na<sup>+</sup> intercalation/deintercalation and structural stability. In terms of anode materials, AI technology leverages data-driven high-throughput screening strategies and microstructural modulation models to drive breakthroughs in key performance metrics such as sodium storage capacity and rate capability for hard carbon, alloy-based, and conversion-type anode materials. AI technology successfully establishes a new development paradigm of “data-driven, mechanism-embedded”, achieving full-chain coverage from atomic-scale material design to system-level performance optimization, significantly reducing development cycle and costs. Based on a summary of the current application status of AI technology in the development of SIBs materials, this review further analyzes the challenges that this field is facing, and at the same time looks forward to the development opportunities of the in-depth integration of AI and experimental research and development, providing innovative methodological support and direction guidance for promoting the industrialization process of high-performance SIBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"116 ","pages":"Pages 434-453"},"PeriodicalIF":14.9,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170726","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}
Pub Date : 2026-05-01Epub Date: 2026-01-16DOI: 10.1016/j.jechem.2026.01.009
Qian Huo , Fu Li , Mengxin Duan , Mo Qiu , Qingxin Guan , Wei Li
Photothermal catalytic CO2 reduction to ethanol is a key pathway for carbon cycle utilization, but its development is limited by the bottlenecks of product selectivity regulation and low C–C coupling efficiency. In this study, a graphene oxide (rGO)-supported high-density Cu/Cu2O heterojunction catalyst was constructed via a “one-pot hydrothermal-high-temperature hydrogen calcination” strategy, leveraging the confinement and electronic modulation effects of “rGO fences” to achieve a significant leap in catalytic performance. Charge density difference and density of states (DOS) analyses reveal that a strong built-in electric field directed from Cu to Cu2O is formed at the heterojunction interface, which efficiently promotes the separation and transfer of charge carriers and optimizes the adsorption of intermediates by regulating the d-band center. Under light irradiation, the localized surface plasmon resonance (LSPR) effect of Cu synergizes with the built-in electric field to enhance the “hot electron” injection efficiency. In situ Fourier transform infrared spectroscopy (in situ FT-IR) and density functional theory (DFT) calculations confirm that the rate-determining step (RDS) energy barrier of the C–C asymmetric coupling pathway of *CO/*CHO at the interface is only 0.92 eV, which is significantly lower than that of side reaction pathways. Under optimal reaction conditions (160 °C, 2 MPa, CO2/H2 = 1:3), the catalyst achieves an ethanol yield of 3250 μmol g−1 h−1 and a liquid-phase selectivity of 93%, providing new insights for the design of efficient catalysts for CO2 conversion to C2+ products.
{"title":"Interfacial engineering of high-density Cu/Cu2O junctions for enhanced CO2-to-ethanol photothermal conversion","authors":"Qian Huo , Fu Li , Mengxin Duan , Mo Qiu , Qingxin Guan , Wei Li","doi":"10.1016/j.jechem.2026.01.009","DOIUrl":"10.1016/j.jechem.2026.01.009","url":null,"abstract":"<div><div>Photothermal catalytic CO<sub>2</sub> reduction to ethanol is a key pathway for carbon cycle utilization, but its development is limited by the bottlenecks of product selectivity regulation and low C–C coupling efficiency. In this study, a graphene oxide (rGO)-supported high-density Cu/Cu<sub>2</sub>O heterojunction catalyst was constructed via a “one-pot hydrothermal-high-temperature hydrogen calcination” strategy, leveraging the confinement and electronic modulation effects of “rGO fences” to achieve a significant leap in catalytic performance. Charge density difference and density of states (DOS) analyses reveal that a strong built-in electric field directed from Cu to Cu<sub>2</sub>O is formed at the heterojunction interface, which efficiently promotes the separation and transfer of charge carriers and optimizes the adsorption of intermediates by regulating the d-band center. Under light irradiation, the localized surface plasmon resonance (LSPR) effect of Cu synergizes with the built-in electric field to enhance the “hot electron” injection efficiency. In situ Fourier transform infrared spectroscopy (in situ FT-IR) and density functional theory (DFT) calculations confirm that the rate-determining step (RDS) energy barrier of the C–C asymmetric coupling pathway of *CO/*CHO at the interface is only 0.92 eV, which is significantly lower than that of side reaction pathways. Under optimal reaction conditions (160 °C, 2 MPa, CO<sub>2</sub>/H<sub>2</sub> = 1:3), the catalyst achieves an ethanol yield of 3250 μmol g<sup>−1</sup> h<sup>−1</sup> and a liquid-phase selectivity of 93%, providing new insights for the design of efficient catalysts for CO<sub>2</sub> conversion to C<sub>2+</sub> products.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"116 ","pages":"Pages 514-524"},"PeriodicalIF":14.9,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170783","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}
Pub Date : 2026-05-01Epub Date: 2026-01-12DOI: 10.1016/j.jechem.2025.12.058
Tianmei Xu, Jiafeng Zhu, Tianlong Wu, Yang Zheng, Xinmeng Li, Juan Ding, Jiulin Wang, Yudai Huang
Lithium-sulfur batteries (LSBs) are an attractive option for high-energy-density applications due to their high theoretical capacity and low cost. However, their development is impeded by the shuttle effect and sluggish redox kinetics of lithium polysulfides (LiPSs). To solve those problems, it is necessary to develop advanced electrocatalysts that can effectively decouple these different pathways while providing complementary active sites. Herein, this work constructs site-specific and spatio-temporal ordered transport Co-MnO heterojunctions via interface engineering, where MnO adsorbs LiPSs and Co promotes the sulfur reduction reaction (SRR). Experimental and theoretical results confirm that MnO adsorption creates a localized high-concentration LiPSs microenvironment for Co sites. The highly active Co then rapidly converts adsorbed LiPSs, suppressing diffusion and preventing site inactivation. This tandem mechanism lowers reaction energy barriers, improves Li2S nucleation/dissolution kinetics, and enhances LiPSs conversion and overall reaction kinetics. The discharge capacity of LSB with Co-MnO modified-separator reaches 972.6 mAh g−1 at 0.5 C, which remains at 488.0 mAh g−1 after 1000 cycles at 2 C. Even at a high sulfur loading of 6.535 mg cm−2, the discharge capacity remains at 641.2 mAh g−1 after 200 cycles at 0.2 C. Moreover, Co-MnO simultaneously regulates the uniform lithium deposition and Li+ flux to enhance the Li||Li symmetrical cell stably cycled at 2 mA cm−2 and 2 mAh cm−2 for 600 h. This study proposes a strategic design for bimetallic tandem reaction electrocatalysts applied to LSBs separators, paving the way for the development of multifunctional separator materials and thereby advancing the performance of next-generation energy storage systems.
锂硫电池（LSBs）由于其高理论容量和低成本而成为高能量密度应用的一个有吸引力的选择。然而，它们的发展受到多硫化锂（LiPSs）的穿梭效应和缓慢的氧化还原动力学的阻碍。为了解决这些问题，有必要开发先进的电催化剂，能够有效地解耦这些不同的途径，同时提供互补的活性位点。本研究通过界面工程构建了特定位点和时空有序输运的Co-MnO异质结，其中MnO吸附LiPSs， Co促进硫还原反应（SRR）。实验和理论结果证实，MnO吸附为Co位点创造了局部高浓度的LiPSs微环境。高活性的Co随后迅速转化吸附的LiPSs，抑制扩散并防止位点失活。这种串联机制降低了反应能垒，改善了Li2S成核/溶解动力学，提高了LiPSs转化和整体反应动力学。Co-MnO改性LSB在0.5℃下的放电容量达到972.6 mAh g−1，在2℃下循环1000次后放电容量仍为488.0 mAh g−1，即使在高硫负荷为6.535 mg cm−2时，在0.2℃下循环200次后放电容量仍为641.2 mAh g−1。Co-MnO同时调节均匀的锂沉积和Li+通量，以增强Li||Li对称电池在2 mA cm - 2和2 mAh cm - 2下稳定循环600 h。本研究提出了应用于LSBs分离器的双金属串联反应电催化剂的战略设计，为多功能分离器材料的开发铺平了道路，从而提高了下一代储能系统的性能。
{"title":"Spatio-temporal ordered transport and site decoupling tandem synergistic catalysis enabling high-load lithium-sulfur batteries","authors":"Tianmei Xu, Jiafeng Zhu, Tianlong Wu, Yang Zheng, Xinmeng Li, Juan Ding, Jiulin Wang, Yudai Huang","doi":"10.1016/j.jechem.2025.12.058","DOIUrl":"10.1016/j.jechem.2025.12.058","url":null,"abstract":"<div><div>Lithium-sulfur batteries (LSBs) are an attractive option for high-energy-density applications due to their high theoretical capacity and low cost. However, their development is impeded by the shuttle effect and sluggish redox kinetics of lithium polysulfides (LiPSs). To solve those problems, it is necessary to develop advanced electrocatalysts that can effectively decouple these different pathways while providing complementary active sites. Herein, this work constructs site-specific and spatio-temporal ordered transport Co-MnO heterojunctions via interface engineering, where MnO adsorbs LiPSs and Co promotes the sulfur reduction reaction (SRR). Experimental and theoretical results confirm that MnO adsorption creates a localized high-concentration LiPSs microenvironment for Co sites. The highly active Co then rapidly converts adsorbed LiPSs, suppressing diffusion and preventing site inactivation. This tandem mechanism lowers reaction energy barriers, improves Li<sub>2</sub>S nucleation/dissolution kinetics, and enhances LiPSs conversion and overall reaction kinetics. The discharge capacity of LSB with Co-MnO modified-separator reaches 972.6 mAh g<sup>−1</sup> at 0.5 C, which remains at 488.0 mAh g<sup>−1</sup> after 1000 cycles at 2 C. Even at a high sulfur loading of 6.535 mg cm<sup>−2</sup>, the discharge capacity remains at 641.2 mAh g<sup>−1</sup> after 200 cycles at 0.2 C. Moreover, Co-MnO simultaneously regulates the uniform lithium deposition and Li<sup>+</sup> flux to enhance the Li||Li symmetrical cell stably cycled at 2 mA cm<sup>−2</sup> and 2 mAh cm<sup>−2</sup> for 600 h. This study proposes a strategic design for bimetallic tandem reaction electrocatalysts applied to LSBs separators, paving the way for the development of multifunctional separator materials and thereby advancing the performance of next-generation energy storage systems.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"116 ","pages":"Pages 302-312"},"PeriodicalIF":14.9,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146074925","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}
Pub Date : 2026-05-01Epub Date: 2025-12-30DOI: 10.1016/j.jechem.2025.12.036
Yarui Ji , Xijia Zhou , Yaohui Zhu , Xuyi Lu , Muniran Tuluhong , Haichao Zhang , Zhirong Yang , Deqiu Zou
Immersion cooling has emerged as a promising advanced thermal management technology for electronic devices and energy storage systems, owing to its high heat transfer efficiency, safety, and energy-saving potential. However, its large-scale application is hindered by multiple challenges: conventional coolants suffer from low thermal conductivity, low specific heat capacity, narrow boiling point range, and environmental risks. Additionally, inadequate design of cooling surface structures and cooling systems further restricts its development. To address these issues, this review comprehensively summarizes recent advances in two core aspects of immersion cooling: coolant modification and cooling surface structure and system optimization. Firstly, strategies for coolant modification are discussed, including enhancing the thermal conductivity and specific heat capacity of single-phase coolants, as well as regulating the wide temperature range and conducting molecular modification of fluorinated fluids in two-phase immersion cooling to mitigate environmental concerns. Subsequently, optimization of cooling surface structures and systems is detailed, such as surface coatings for device protection, adjustment of surface roughness to enhance boiling heat transfer, integration of flow-guiding baffles, and design of inlet/outlet channels. These optimizations effectively improve the overall cooling efficiency. Furthermore, representative applications of immersion cooling in data centers, lithium-ion batteries (LIBs), solar photovoltaic (PV) panels, and electric motors are reviewed to illustrate its practical value. Finally, after comparing the performance of various coolant modification and cooling structure optimization strategies and summarizing existing limitations, the current technical challenges, improvement methods, and future development directions of immersion cooling technology are proposed. Future efforts should focus on leveraging artificial intelligence (AI) technology and reinforcement learning, conducting lifecycle assessments, and developing recyclable coolants to realize sustainable and economically viable immersion cooling systems. Meanwhile, optimizing material selection and system design parameters will further improve the overall efficiency of thermal management systems. Immersion cooling exhibits significant potential in reducing energy consumption, cutting carbon emissions, and enhancing safety, providing new insights for its future engineering applications.
{"title":"Immersion cooling technology: Coolants and modification, cooling surface structure and system optimization","authors":"Yarui Ji , Xijia Zhou , Yaohui Zhu , Xuyi Lu , Muniran Tuluhong , Haichao Zhang , Zhirong Yang , Deqiu Zou","doi":"10.1016/j.jechem.2025.12.036","DOIUrl":"10.1016/j.jechem.2025.12.036","url":null,"abstract":"<div><div>Immersion cooling has emerged as a promising advanced thermal management technology for electronic devices and energy storage systems, owing to its high heat transfer efficiency, safety, and energy-saving potential. However, its large-scale application is hindered by multiple challenges: conventional coolants suffer from low thermal conductivity, low specific heat capacity, narrow boiling point range, and environmental risks. Additionally, inadequate design of cooling surface structures and cooling systems further restricts its development. To address these issues, this review comprehensively summarizes recent advances in two core aspects of immersion cooling: coolant modification and cooling surface structure and system optimization. Firstly, strategies for coolant modification are discussed, including enhancing the thermal conductivity and specific heat capacity of single-phase coolants, as well as regulating the wide temperature range and conducting molecular modification of fluorinated fluids in two-phase immersion cooling to mitigate environmental concerns. Subsequently, optimization of cooling surface structures and systems is detailed, such as surface coatings for device protection, adjustment of surface roughness to enhance boiling heat transfer, integration of flow-guiding baffles, and design of inlet/outlet channels. These optimizations effectively improve the overall cooling efficiency. Furthermore, representative applications of immersion cooling in data centers, lithium-ion batteries (LIBs), solar photovoltaic (PV) panels, and electric motors are reviewed to illustrate its practical value. Finally, after comparing the performance of various coolant modification and cooling structure optimization strategies and summarizing existing limitations, the current technical challenges, improvement methods, and future development directions of immersion cooling technology are proposed. Future efforts should focus on leveraging artificial intelligence (AI) technology and reinforcement learning, conducting lifecycle assessments, and developing recyclable coolants to realize sustainable and economically viable immersion cooling systems. Meanwhile, optimizing material selection and system design parameters will further improve the overall efficiency of thermal management systems. Immersion cooling exhibits significant potential in reducing energy consumption, cutting carbon emissions, and enhancing safety, providing new insights for its future engineering applications.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"116 ","pages":"Pages 91-122"},"PeriodicalIF":14.9,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146074929","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}
Pub Date : 2026-05-01Epub Date: 2026-01-28DOI: 10.1016/j.jechem.2026.01.032
Ruifu Li, Hongsheng Han, Huihua Li, Huang Zhang
Aqueous zinc-ion batteries (AZIBs) are emerging as a viable option for grid-scale energy storage, but their energy density is currently capped by the limitations of conventional cathode materials. While phosphate-based cathodes, due to their high operational voltage and exceptional structural stability, represent a step forward, their capacity remains constrained by single-electron redox processes. This review advocates multi-electron redox chemistry as the crucial pathway to overcome this limitation. Focusing on vanadium-based phosphates with their multiple accessible oxidation states, we examine key challenges including low electronic conductivity, vanadium dissolution, and evaluate advanced strategies such as defect engineering and elemental doping. By showcasing recent advances in NASICON-type and related structures capable of multi-electron redox reactions, we outline a roadmap for developing next-generation phosphate cathodes, laying the groundwork for the development of high-performance AZIBs.
{"title":"Multi-electron redox chemistry in phosphate cathodes for aqueous zinc batteries","authors":"Ruifu Li, Hongsheng Han, Huihua Li, Huang Zhang","doi":"10.1016/j.jechem.2026.01.032","DOIUrl":"10.1016/j.jechem.2026.01.032","url":null,"abstract":"<div><div>Aqueous zinc-ion batteries (AZIBs) are emerging as a viable option for grid-scale energy storage, but their energy density is currently capped by the limitations of conventional cathode materials. While phosphate-based cathodes, due to their high operational voltage and exceptional structural stability, represent a step forward, their capacity remains constrained by single-electron redox processes. This review advocates multi-electron redox chemistry as the crucial pathway to overcome this limitation. Focusing on vanadium-based phosphates with their multiple accessible oxidation states, we examine key challenges including low electronic conductivity, vanadium dissolution, and evaluate advanced strategies such as defect engineering and elemental doping. By showcasing recent advances in NASICON-type and related structures capable of multi-electron redox reactions, we outline a roadmap for developing next-generation phosphate cathodes, laying the groundwork for the development of high-performance AZIBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"116 ","pages":"Pages 586-594"},"PeriodicalIF":14.9,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170631","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}
Pub Date : 2026-05-01Epub Date: 2026-01-14DOI: 10.1016/j.jechem.2026.01.010
Guangbo Liu , Zhihao Lou , Qinghao Quan , Yu Dai , Yuanshuo Ma , Pengfei Wu , Xuejing Cui , Xin Chen , Xin Zhou , Luhua Jiang
Hydrazine-assisted water electrolysis is a promising route for hydrogen production, and efficient bi-functional electrodes for the anodic hydrazine oxidation reaction (HzOR) and the cathodic hydrogen evolution reaction (HER) simplify the devices and enhance the technological advantage. However, suffering from the incompatible adsorption of different intermediates and the sluggish reaction kinetics, the design of effective and durable bi-functional electrodes still faces challenges. Herein, a Lewis acid (WOx) of powerful electron-accepting ability stabilized single-atom Ir catalyst (Ir-SA@WOx), intriguing strong metal-support interaction (SMSI), is demonstrated to efficiently activate H2O and N2H4 molecules. Ir-SA@WOx shows exceptional activity for both HER and HzOR (26.31 and 44.79 A mgIr−1 at −100 mV), surpassing commercial Pt/C and Ir/C by factors of 41.8 and 27.6, respectively. A hydrazine-assisted water electrolyzer fabricated with Ir-SA@WOx achieves a current density of 100 mA cm−2 at an ultra-low cell voltage of 0.313 V and electricity consumption of merely 0.75 kWh m−3 H2, significantly lower than conventional water electrolysis systems (1.852 V, 4.43 kWh m−3 H2). In situ infrared absorption spectroscopy and theoretical calculations elucidate that the SMSI in Ir-SA@WOx reconstructs the electronic structure to facilitate the activation of the rigid water at the catalyst/electrolyte interface into free species, also optimizes H* adsorption and accelerates dehydrogenation kinetics of the potential-determining step of N2H3*-to-N2H2* at Ir-sites, thereby realizing high activity for both HER and HzOR. This work illustrates the tailoring of electronic structures via the SMSI effect for catalytic-activity enhancement, guiding the design of advanced bi-functional catalysts for energy-efficient hydrogen production.
联氨辅助电解是一种很有前途的制氢途径，高效的双功能电极用于阳极联氨氧化反应（HzOR）和阴极析氢反应（HER），简化了装置，增强了技术优势。然而，由于不同中间体的不相容吸附和反应动力学缓慢，设计有效且耐用的双功能电极仍然面临挑战。本文中，路易斯酸（WOx）具有强大的电子接受能力，稳定了单原子Ir催化剂（Ir-SA@WOx），激发了强金属-载体相互作用（SMSI），有效地激活了H2O和N2H4分子。Ir-SA@WOx对HER和HzOR的活性（在- 100 mV下分别为26.31和44.79 A mgIr - 1），分别超过商业Pt/C和Ir/C的41.8和27.6倍。用Ir-SA@WOx制备的肼辅助水电解器在超低电池电压0.313 V下电流密度达到100 mA cm−2，耗电量仅为0.75 kWh m−3 H2，显著低于传统电解系统（1.852 V, 4.43 kWh m−3 H2）。原位红外吸收光谱和理论计算表明，Ir-SA@WOx中的SMSI重构了电子结构，促进了催化剂/电解质界面上刚性水活化为自由物质，优化了H*吸附，加速了ir位上N2H3*到n2h2 *的电位决定步骤的脱氢动力学，从而实现了HER和HzOR的高活性。这项工作说明了通过SMSI效应来调整电子结构以增强催化活性，指导了用于节能制氢的先进双功能催化剂的设计。
{"title":"Strong metal-support interaction in Lewis acid anchored iridium single-atoms boosts hydrazine oxidation-coupled hydrogen evolution","authors":"Guangbo Liu , Zhihao Lou , Qinghao Quan , Yu Dai , Yuanshuo Ma , Pengfei Wu , Xuejing Cui , Xin Chen , Xin Zhou , Luhua Jiang","doi":"10.1016/j.jechem.2026.01.010","DOIUrl":"10.1016/j.jechem.2026.01.010","url":null,"abstract":"<div><div>Hydrazine-assisted water electrolysis is a promising route for hydrogen production, and efficient bi-functional electrodes for the anodic hydrazine oxidation reaction (HzOR) and the cathodic hydrogen evolution reaction (HER) simplify the devices and enhance the technological advantage. However, suffering from the incompatible adsorption of different intermediates and the sluggish reaction kinetics, the design of effective and durable bi-functional electrodes still faces challenges. Herein, a Lewis acid (WO<em><sub>x</sub></em>) of powerful electron-accepting ability stabilized single-atom Ir catalyst (Ir-SA@WO<em><sub>x</sub></em>), intriguing strong metal-support interaction (SMSI), is demonstrated to efficiently activate H<sub>2</sub>O and N<sub>2</sub>H<sub>4</sub> molecules. Ir-SA@WO<em><sub>x</sub></em> shows exceptional activity for both HER and HzOR (26.31 and 44.79 A mg<sub>Ir</sub><sup>−1</sup> at −100 mV), surpassing commercial Pt/C and Ir/C by factors of 41.8 and 27.6, respectively. A hydrazine-assisted water electrolyzer fabricated with Ir-SA@WO<em><sub>x</sub></em> achieves a current density of 100 mA cm<sup>−2</sup> at an ultra-low cell voltage of 0.313 V and electricity consumption of merely 0.75 kWh m<sup>−3</sup> H<sub>2</sub>, significantly lower than conventional water electrolysis systems (1.852 V, 4.43 kWh m<sup>−3</sup> H<sub>2</sub>). In situ infrared absorption spectroscopy and theoretical calculations elucidate that the SMSI in Ir-SA@WO<em><sub>x</sub></em> reconstructs the electronic structure to facilitate the activation of the rigid water at the catalyst/electrolyte interface into free species, also optimizes H* adsorption and accelerates dehydrogenation kinetics of the potential-determining step of N<sub>2</sub>H<sub>3</sub>*-to-N<sub>2</sub>H<sub>2</sub>* at Ir-sites, thereby realizing high activity for both HER and HzOR. This work illustrates the tailoring of electronic structures via the SMSI effect for catalytic-activity enhancement, guiding the design of advanced bi-functional catalysts for energy-efficient hydrogen production.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"116 ","pages":"Pages 359-370"},"PeriodicalIF":14.9,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170825","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}
Pub Date : 2026-05-01Epub Date: 2025-12-27DOI: 10.1016/j.jechem.2025.12.034
Lina Hu , Zengyu Han , Ya Chen , Yaoda Liu , Lei Li , Jie Su , Zhengfei Dai , Dong-Shuang Wu
The development of pH‐robust electrocatalysts is highly desirable but challenging for the hydrogen evolution reaction (HER) in water electrolysis. Among the noble metal groups, ruthenium (Ru) holds the promise in balancing the cost and activity in HER, but it is restricted by the strong H adsorption and the sluggish Heyrovsky step. It appeals for a rational d-band manipulation to neutralize the hydrogen adsorption to promote the HER kinetics. Herein, we profiled a confined structure with RuCo alloy nanoparticles in N-doped carbon nanofiber (RuCo@NCNF) by a facile electrospinning-pyrolysis process for HER electrocatalysis. An electron transfer from Co to Ru is indicated in the RuCo@NCNF composite to enhance the electron-donating character of Ru active sites to couple the HER. Resultantly, the optimized Ru1Co2.5@NCNF catalyst stably exhibits the Pt-beyond HER activity in both alkaline (10 mV at 10 mA cm−2) and acidic electrolytes (23 mV at 10 mA cm−2), while delivering competitive HER performance in neutral electrolytes. Density functional theory (DFT) calculations also confirm that the Ru-Co electronic interactions can effectuate the d-band center downshift, moderating the adsorption energies of hydrogen (ΔGH*) and H2O for efficient hydrogen production. This study provides a reference for the rational design of Ru-based pH-robust HER electrocatalyst through confined nanoalloy structures.
{"title":"Constructing the confined RuCo nanoalloys with modulated d-band centers for efficient pH-robust hydrogen evolution","authors":"Lina Hu , Zengyu Han , Ya Chen , Yaoda Liu , Lei Li , Jie Su , Zhengfei Dai , Dong-Shuang Wu","doi":"10.1016/j.jechem.2025.12.034","DOIUrl":"10.1016/j.jechem.2025.12.034","url":null,"abstract":"<div><div>The development of pH‐robust electrocatalysts is highly desirable but challenging for the hydrogen evolution reaction (HER) in water electrolysis. Among the noble metal groups, ruthenium (Ru) holds the promise in balancing the cost and activity in HER, but it is restricted by the strong H adsorption and the sluggish Heyrovsky step. It appeals for a rational <em>d</em>-band manipulation to neutralize the hydrogen adsorption to promote the HER kinetics. Herein, we profiled a confined structure with RuCo alloy nanoparticles in N-doped carbon nanofiber (RuCo@NCNF) by a facile electrospinning-pyrolysis process for HER electrocatalysis. An electron transfer from Co to Ru is indicated in the RuCo@NCNF composite to enhance the electron-donating character of Ru active sites to couple the HER. Resultantly, the optimized Ru<sub>1</sub>Co<sub>2.5</sub>@NCNF catalyst stably exhibits the Pt-beyond HER activity in both alkaline (10 mV at 10 mA cm<sup>−2</sup>) and acidic electrolytes (23 mV at 10 mA cm<sup>−2</sup>), while delivering competitive HER performance in neutral electrolytes. Density functional theory (DFT) calculations also confirm that the Ru-Co electronic interactions can effectuate the <em>d</em>-band center downshift, moderating the adsorption energies of hydrogen (Δ<em>G</em><sub>H*</sub>) and H<sub>2</sub>O for efficient hydrogen production. This study provides a reference for the rational design of Ru-based pH-robust HER electrocatalyst through confined nanoalloy structures.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"116 ","pages":"Pages 58-68"},"PeriodicalIF":14.9,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146025026","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}
Pub Date : 2026-05-01Epub Date: 2025-12-30DOI: 10.1016/j.jechem.2025.12.041
Linjun Zhong , Ziqiang Fan , Zhe Wang , Xinyue Wu , Jingan Liu , Junjun Liu , Junyang Zheng , Qing Chen , Lidan Xing , Jianhui Li , Yu Ying , Ronghua Zeng
Almost all commercial lithium-ion batteries (LIBs) with LiCoO2 (LCO) as cathode material are cycled from 3.0 to 4.2 V and their actual specific capacity just ranges from 140 to 160 mA h g−1, which is much lower than the theoretical specific capacity of LCO of 274 mA h g−1. To further improve the actual specific capacity of LCO, elevating the upper limit of its working voltage is necessary. However, as the upper limit of its working voltage is elevated to 4.5 V or higher, the LCO crystal will undergo severe irreversible phase transition, and the oxidization decomposition of electrolyte on the cathode’s surface will exacerbate, which will severely reduce the cycling lifespan of batteries, hindering the actual application of high voltage LCO. In this work, we find that 3,5-difluorophenylboronic acid pinacol ester (35-DAPE) is an effective cathode electrolyte interphase (CEI)-forming additive, which can form a robust and stable CEI layer rich in fluorophenyl-groups and B–F/B–O bonds on the surface of LCO cathode, inhibiting the dissolution of cobalt ions and maintain the structural stability of LCO crystal over cycles. The graphite||LCO pouch cells in a voltage range of 3.0–4.5 V with 35-DAPE display a capacity retention rate of 91.1 % after 150 cycles at room temperature, compared to that of 2.4 % in baseline electrolyte. Besides, rate performance at room temperature and discharging performance at low temperatures of graphite||LCO pouch cells can also be observed with an improvement after the introduction of 35-DAPE. In addition, this work has explained the decomposition mechanism of 35-DAPE and how its products improve the electrochemical performance of graphite||LCO pouch cells in detail, which not only advances the actual application of fluorophenylboronic acid pinacol ester additive in high voltage LIBs but also provides valuable insights for the design of functional electrolyte additives.
几乎所有以LiCoO2 （LCO）为正极材料的商用锂离子电池（LIBs）在3.0 ~ 4.2 V范围内循环，其实际比容量仅在140 ~ 160 mA h g−1之间，远低于LCO的理论比容量274 mA h g−1。为了进一步提高LCO的实际比容量，有必要提高其工作电压的上限。然而，当其工作电压上限提高到4.5 V或更高时，LCO晶体将发生严重的不可逆相变，阴极表面电解液氧化分解加剧，严重降低电池的循环寿命，阻碍了高压LCO的实际应用。在本研究中，我们发现3,5-二氟苯硼酸松醇酯（35-DAPE）是一种有效的阴极电解质界面（CEI）形成添加剂，它可以在LCO阴极表面形成坚固稳定的富含氟苯基和B-F / B-O键的CEI层，抑制钴离子的溶解，保持LCO晶体在循环过程中的结构稳定性。在3.0-4.5 V电压范围内，使用35-DAPE的石墨||LCO袋状电池在室温下循环150次后，容量保持率为91.1%，而在基线电解质下的容量保持率为2.4%。此外，引入35-DAPE后，石墨||LCO袋状电池的室温倍率性能和低温放电性能也得到了改善。此外，本工作详细解释了35-DAPE的分解机理及其产物如何改善石墨||LCO袋状电池的电化学性能，这不仅推进了氟苯硼酸蒎醇酯添加剂在高压锂离子电池中的实际应用，也为功能电解质添加剂的设计提供了有价值的见解。
{"title":"Interphase tailoring via fluorophenyl-boron integration for high-voltage LiCoO2 operation","authors":"Linjun Zhong , Ziqiang Fan , Zhe Wang , Xinyue Wu , Jingan Liu , Junjun Liu , Junyang Zheng , Qing Chen , Lidan Xing , Jianhui Li , Yu Ying , Ronghua Zeng","doi":"10.1016/j.jechem.2025.12.041","DOIUrl":"10.1016/j.jechem.2025.12.041","url":null,"abstract":"<div><div>Almost all commercial lithium-ion batteries (LIBs) with LiCoO<sub>2</sub> (LCO) as cathode material are cycled from 3.0 to 4.2 V and their actual specific capacity just ranges from 140 to 160 mA h g<sup>−1</sup>, which is much lower than the theoretical specific capacity of LCO of 274 mA h g<sup>−1</sup>. To further improve the actual specific capacity of LCO, elevating the upper limit of its working voltage is necessary. However, as the upper limit of its working voltage is elevated to 4.5 V or higher, the LCO crystal will undergo severe irreversible phase transition, and the oxidization decomposition of electrolyte on the cathode’s surface will exacerbate, which will severely reduce the cycling lifespan of batteries, hindering the actual application of high voltage LCO. In this work, we find that 3,5-difluorophenylboronic acid pinacol ester (35-DAPE) is an effective cathode electrolyte interphase (CEI)-forming additive, which can form a robust and stable CEI layer rich in fluorophenyl-groups and B–F/B–O bonds on the surface of LCO cathode, inhibiting the dissolution of cobalt ions and maintain the structural stability of LCO crystal over cycles. The graphite||LCO pouch cells in a voltage range of 3.0–4.5 V with 35-DAPE display a capacity retention rate of 91.1 % after 150 cycles at room temperature, compared to that of 2.4 % in baseline electrolyte. Besides, rate performance at room temperature and discharging performance at low temperatures of graphite||LCO pouch cells can also be observed with an improvement after the introduction of 35-DAPE. In addition, this work has explained the decomposition mechanism of 35-DAPE and how its products improve the electrochemical performance of graphite||LCO pouch cells in detail, which not only advances the actual application of fluorophenylboronic acid pinacol ester additive in high voltage LIBs but also provides valuable insights for the design of functional electrolyte additives.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"116 ","pages":"Pages 220-229"},"PeriodicalIF":14.9,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146025034","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}
Pub Date : 2026-05-01Epub Date: 2026-01-28DOI: 10.1016/j.jechem.2026.01.029
Yi Tan , Xiaokang Chen , Jian Yuan , Guan Sheng , Wei-Qiao Deng , Ghim Wei Ho , Hao Wu
The conversion of nitric oxide (NO), a gaseous pollutant with an intermediate nitrogen oxidation state, into value-added ammonium nitrate (NH4NO3) via redox processes offers a sustainable alternative to conventional disposal methods, which are hampered by competing pathways that yield undesirable byproducts. Herein, we decouple the synthesis of NH4NO3 into electrochemical NO oxidation (NOOR) and reduction (NORR) by employing H-terminated and Cu-metallated porphyrinic metal–organic framework catalysts (H-PMOF and Cu-PMOF, respectively), leveraging their tailored coordination environments and varied NO adsorption configurations. The H-PMOF favors O-atom adsorption via hydrogen bonding, whereas the Cu-PMOF strengthens N-atom adsorption through CuN interactions. They promote NOOR to NO3− and NORR to NH4+, respectively, achieving greater Faradaic efficiencies and yield rates compared to their respective counterparts. When integrated in one electrolyzer, they enable direct synthesis of NH4NO3 by generating 662.4 µmol of NO3− and 409.5 µmol of NH4+ hourly. Molecular dynamics simulations reveal differences in adsorption modes, while computational results identify the rate-determining dehydrogenation (*HNO3 → *NO3 for NOOR) and hydrogenation steps (*NO → *NHO for NORR), with both catalysts exhibiting reduced energy barriers. This work presents a strategy for directing NO redox reactions through coordination engineering, paving the way for sustainable nitrogen valorization.
{"title":"Electrocatalytic ammonium nitrate synthesis through integrating nitric oxide redox reactions over porphyrinic metal–organic frameworks","authors":"Yi Tan , Xiaokang Chen , Jian Yuan , Guan Sheng , Wei-Qiao Deng , Ghim Wei Ho , Hao Wu","doi":"10.1016/j.jechem.2026.01.029","DOIUrl":"10.1016/j.jechem.2026.01.029","url":null,"abstract":"<div><div>The conversion of nitric oxide (NO), a gaseous pollutant with an intermediate nitrogen oxidation state, into value-added ammonium nitrate (NH<sub>4</sub>NO<sub>3</sub>) via redox processes offers a sustainable alternative to conventional disposal methods, which are hampered by competing pathways that yield undesirable byproducts. Herein, we decouple the synthesis of NH<sub>4</sub>NO<sub>3</sub> into electrochemical NO oxidation (NOOR) and reduction (NORR) by employing H-terminated and Cu-metallated porphyrinic metal–organic framework catalysts (H-PMOF and Cu-PMOF, respectively), leveraging their tailored coordination environments and varied NO adsorption configurations. The H-PMOF favors O-atom adsorption via hydrogen bonding, whereas the Cu-PMOF strengthens N-atom adsorption through Cu<img>N interactions. They promote NOOR to NO<sub>3</sub><sup>−</sup> and NORR to NH<sub>4</sub><sup>+</sup>, respectively, achieving greater Faradaic efficiencies and yield rates compared to their respective counterparts. When integrated in one electrolyzer, they enable direct synthesis of NH<sub>4</sub>NO<sub>3</sub> by generating 662.4 µmol of NO<sub>3</sub><sup>−</sup> and 409.5 µmol of NH<sub>4</sub><sup>+</sup> hourly. Molecular dynamics simulations reveal differences in adsorption modes, while computational results identify the rate-determining dehydrogenation (*HNO<sub>3</sub> → *NO<sub>3</sub> for NOOR) and hydrogenation steps (*NO → *NHO for NORR), with both catalysts exhibiting reduced energy barriers. This work presents a strategy for directing NO redox reactions through coordination engineering, paving the way for sustainable nitrogen valorization.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"116 ","pages":"Pages 558-565"},"PeriodicalIF":14.9,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170628","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}
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