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Deciphering the role of ultra-low-loaded rhodium in NiFe-MIL-53 for superior oxygen evolution reaction

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Journal of Energy chemistry 2025年第1期100卷 77-86页

作者： Jinzhi Jia Jinhua Zhang Kailu Guo Lanyue Zhang Gening Du Hao You Junfeng Huang Mudong Tu Hua Li Yong Peng Wei Dou Cailing Xu State Key Laboratory of Applied Organic chemistry College of Chemistry and Chemical Engineering School of Materials and Energy Lanzhou University College of chemistry and Chemical engineering Luoyang Normal University

Designing highly active and stable electrocatalysts of oxygen evolution reaction （OER） is one of the crucial *** this study,a novel OER electrocatalyst,NiFe-MIL-53 modified with ultra-low rhodium（Rh@NiFe-MIL-53）,is successfully prepared via the hydrothermal ***-situ Raman spectroscopy and electrochemical impedance spectroscopy reveal that the doped Rh accelerates the phase transformation of NiFe-MIL-53 and the in-situ formed Rh@NiFeOOH is the actual active *** importantly,the enhanced reversibility of electrochemical reconstruction between NiFeOOH and NiFe（OH）2after doping Rh is beneficial for improving the electrochemical stability of the catalyst.X-ray photoelectron spectroscopy spectra show the strong electronic interaction between single-atom Rh and Ni/Fe in Rh@***,theoretical calculations confirm that the integration of single-atom Rh into the NiFeOOH successfully reduces the band gap,regulates the d-band center （εd）,accelerates the charge transfer,and optimizes the adsorption behavior of oxygen-containing intermediates,thereby lowering the energy barrier of rate-determining ***,the optimized Rh@NiFe-MIL-53 exhibits excellent OER activity （240 mV） with a small Tafel slope of 48.2 mV dec-1and long-term durability (over1270 h at 10 m A cm-2and 110 h at 200 mA cm-2).This work presents a new perspective on designing highly efficient OER electrocatalysts.

关键词： NiFe-MIL-53 Rh Electrochemical reconstruction Catalytic mechanism Oxygen evolution reaction

De novo synthesis of atropisomeric benzofurans via Cu/SPDO complex catalyzed asymmetric formal [3 + 2] annulation

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Science China chemistry 2025年第1期 174-180页

作者： Fan-Xiao Meng Xing-Yu Wang Ka Lu Ju-Song Yang Fu-Min Zhang Ai-Jun Ma Bao Du Yong-Qiang Tu State Key Laboratory of Applied Organic chemistry College of Chemistry and Chemical Engineering Lanzhou University school of chemistry and Chemical engineering Shanghai Jiao Tong University school of Biotechnology and Health sciences Wuyi University

Herein, the de novo synthesis of atropisomeric benzofurans through the Cu/spirocyclic-pyrrolidine-oxazoline(SPDO) complex catalyze asymmetric formal [3 + 2] cycloaddition between quinones and ynamides is explored, producing a range of structurally diverse axially chiral benzofurans in satisfactory yields with good to excellent enantioselectivities. Furthermore, density functional theory calculations were applied to explain the possible reaction mechanism.

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Photoinduced radical sulfur dioxide insertion with asymmetric cyclization of alkenes: accessing β-chiral sulfones bearing S-stereocentric cyclic sulfinamides

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Science China chemistry 2025年第01期 257-263页

作者： Jiapian Huang Chenxin Wang Xu Wang Xiaoyu Zhou Wei Xiao Jie Wu school of Pharmaceutical and Chemical engineering & Institute for Advanced Studies Taizhou University State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences school of chemistry and Chemical engineering Henan Normal University

The generation of various β-chiral sulfones bearing chiral cyclic sulfinamides through photoredox-catalyzed sulfur dioxide insertion with asymmetric radical cyclization is described. This method features a broad substrate scope and excellent stereospecificity. Computational studies reveal that the dispersion interaction between sulfinyl group and CH2SO2Ph group plays a crucial role in the stereoselectivity control.

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Dual modulation of homogeneous nanomaterialization and electrochemical activation enhancing zinc ion storage

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Science China chemistry 2025年第01期 385-393页

作者： Jianwei Wang Huan Wang Kangning Wang Wenhui Wang Wenlin Zhang Yanzhong Zhen school of chemistry & Chemical engineering Yan'an University

Vanadium-based electrode materials are widely investigated,but the low specific capacity and slow electrochemical kinetics in aqueous zinc-ion batteries still limit their commercial ***,the VS2/Ca V4O9material with the morphology of nanoflower was synthesized by a one-step hydrothermal *** to the blocky structure of pure VS2material,the VS2/Ca V4O9material is composed of thinner homogeneous *** open structures could provide abundant electrochemical active sites and ion transport channels,and then promote the electrochemical reaction *** addition,they can also buffer the bulk strain during the reaction *** improve the utilization of vanadium elements,an in-situ electrochemical activation strategy is used to explore the storage performance of the VS2/Ca V4O9material,the different activation voltage range of 0.4–1.6 and 0.4–1.4 V are selected,*** with the longer activation plateau of activated-VS2,the VS2/Ca V4O9cathode could quickly reach the activation state in the range of 1.4–1.6 V and cause the release of additional Zn storage sites *** VS2/Ca V4O9cathode delivers a higher power density of 37,000 W kg-1and a significant energy density of 423 Wh *** the high current density of 15 A g-1,the VS2/Ca V4O9cathode still has a discharge capacity of 183.9m Ah g-1after 5,000 cycles,and the capacity decay rate per cycle is only 0.0042%.Continuous cyclic voltammetry （CV） curves,electrochemical impedance spectroscopy （EIS） measurements,density functional theory （DFT） calculation and galvanostatic intermittent titration technique （GITT） measurements demonstrate that the VS2/Ca V4O9cathode has a faster ion diffusion/charge transfer ***,the assembled flexible device has an excellent mechanical stability.

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Small modifications of endo-functionalized cavities lead to large changes in molecular interaction in water

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Science China chemistry 2025年第1期 369-376页

作者： Song-Meng Wang Hao Nian Yan-Fang Wang Li-Shuo Zheng Yu-Tao Zheng Yi-Wei Dong Liping Huang Xiaoping Wang Wei Jiang Liu-Pan Yang Department of chemistry Southern University of Science and Technology school of chemistry and Pharmaceutical sciences State Key Laboratory for Chemistry and Molecular Engineering of Medicinal ResourcesGuangxi Normal University school of Pharmaceutical Science Hengyang Medical School University of South China

Studying molecular recognition in aqueous environments is crucial for understanding biological processes. Herein, we present a series of N-doped endo-functionalized anthracene-based cavities by introducing inward-directed pyridine units. The subtle modifications can significantly affect the binding properties of these receptors, which is similar to the mutations in biological systems. Combining theoretical calculations and molecular recognition experiments demonstrated that these “mutations” have an impact on the hydrophobicity and charge distribution of the hosts, consequently significantly influencing molecular *** is crucial for understanding the intricate mechanisms of molecular-level interactions in biological receptors.

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High-temperature-tolerant flexible supercapacitors: Gel polymer electrolytes and electrode materials

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Journal of Energy chemistry 2025年第1期100卷 426-457页

作者： Chong Peng Xinyi Huang Mingwei Zhao Shuling Liao Quanhong Yang Nianjun Yang Siyu Yu school of chemistry & Chemical engineering Southwest University Nanoyang Group Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage School of Chemical Engineering and Technology and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin University Department of chemistry & IMO-IMOMEC Hasselt University

The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and electrode materials stand as two key components that significantly impact the efficacy of hightemperature-tolerant FSCs(HT-FSCs). They should not only exhibit high electrochemical performance and excellent flexibility, but also withstand intense thermal stress. Considerable efforts have been devoted to enhancing their thermal stability while maintaining high electrochemical and mechanical performance. In this review, the fundamentals of HT-FSCs are outlined. A comprehensive overview of state-of-the-art progress and achievements in HT-FSCs, with a focus on thermally stable gel polymer electrolytes and electrode materials is provided. Finally, challenges and future perspectives regarding HT-FSCs are discussed, alongside strategies for elevating operational temperatures and *** review offers both theoretical foundations and practical guidelines for designing and manufacturing HT-FSCs, further promoting their widespread adoption across diverse fields.

关键词： Flexible supercapacitors High-temperature tolerance Gel polymer electrolytes Electrode materials

Ru doping triggering reconstruction of cobalt phosphide for coupling glycerol electrooxidation with seawater electrolysis

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Journal of Energy chemistry 2025年第1期100卷 317-326页

作者： Binglu Deng Jie Shen Jinxing Lu Chuqiang Huang Zhuoyuan Chen Feng Peng Yunpeng Liu school of Materials Science and Hydrogen Energy Foshan University school of chemistry and Chemical engineering Guangzhou University Guangdong Key Laboratory for Hydrogen Energy Technologies

Seawater electrolysis is a promising approach for sustainable energy without relying on precious ***,the large-scale seawater electrolysis is hindered by low catalytic efficiency and severe anode corrosion caused by the harmful *** contrast to the oxygen evolution reaction （OER）and chlorin ion oxidation reaction （ClOR）,glycerol oxidation reaction （GOR） is more thermodynamically and kinetically favorable ***,a Ru doping cobalt phosphide （Ru-CoP2） is proposed as a robust bifunctional electrocatalyst for seawater electrolysis and GOR,for the concurrent productions of hydrogen and value-added *** in situ and ex situ characterization analyses demonstrated that Ru doping featured in the dynamic reconstruction process from Ru-CoP2to Ru-CoOOH,accounting for the superior GOR *** coupling GOR with hydrogen evolution was realized by employing Ru-CoP2as both anode and cathode,requiring only a low voltage of 1.43 V at 100 mA cm-2,which was 250 m V lower than that in alkaline *** work guides the design of bifunctional electrocatalysts for energy-efficient seawater electrolysis coupled with biomass resource upcycling.

关键词： Glycerol electrooxidation Hydrogen evolution Ru doping Cobalt phosphide Bifunctional electrocatalysts

Synergistically enhanced ORR and HER performance on Co-N-C coupled in-situ generated PtCo intermetallic

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Journal of Energy chemistry 2025年第1期100卷 721-729页

作者： Guanyu Luo Min Song Lulu An Xiao Huang Qian Zhang Chenhao Zhang Tao Shen Shuang Wang Deli Wang Key Laboratory of Material chemistry for Energy Conversion and Storage (Huazhong University of Science and Technology) Ministry of Education School of Chemistry and Chemical Engineering Huazhong University of Science and Technology

Integrating multi-scale sites in a composite catalyst is vital to realize efficient ***,a synergistic composite catalyst consisting of Co atomic sites and in-situ generated PtCo intermetallic compounds （IMCs）(o-PtCo@CoNC) is proposed through Co pre-anchoring and subsequent impregnation-reduction *** loading of Co atoms provides a chance for in-situ generating PtCo ordered intermetallic *** remaining Co single atoms and PtCo IMCs construct synergistic electrocatalytic *** from the ordered structure,synergistic effect of Pt Co IMCs and Co single atoms,o-PtCo@CoNC exhibits excellent electrocatalytic performance for oxygen reduction reaction （ORR） and hydrogen evolution reaction （HER） with mass activity of 1.21 A mgPt-1（at 0.9 V） and5.70 A mgPt-1（at an overpotential of 100 mV）,***,o-PtCo@CoNC delivers negligible loss of half-wave potential and overpotential during long-term stability test in acid solutions,with 13 mV decay after 50,000 potential cycles for ORR and a 2.7 mV decay after 20,000 potential cycles for *** integration strategy of single-atomic sites coupled IMCs paves the way for enhancing the activity and durability of Pt-based electrocatalysts.

关键词： Electrolytic reduction

A surface engineering strategy for the stabilization of zinc metal anodes with montmorillonite layers toward long-life rechargeable aqueous zinc ion batteries

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Journal of Energy chemistry 2025年第1期100卷 94-105页

作者： Wenbo Wang Ruifeng Xu Xu Zhang Peiyu Wang Bao Yang Bingjun Yang Juan Yang Kailimai Su Pengjun Ma Yanan Deng Xianfeng Fan Wanjun Chen Key Laboratory for Electronic Materials College of Electrical Engineering Northwest Minzu University Resource chemistry and Energy Materials Research Center State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Institute for Materials and Processes School of Engineering University of Edinburgh

Rechargeable aqueous zinc-ion batteries （AZIBs） exhibit appreciable potential in the domain of electrochemical energy ***,there are serious challenges for AZIBs,for instance zinc dendrite growth,hydrogen evolution reaction （HER）,and corrosion side ***,we propose a surface engineering modification strategy for coating the montmorillonite （MMT） layer onto the surface of the Zn anode to tackle these issues,thereby achieving high cycling stability for rechargeable *** results reveal that the MMT layer on the surface of the Zn anode is able to provide ordered zincophilic channels for zinc ions migration,facilitating the reaction kinetics of zinc *** functional theory（DFT） calculations and water contact angle （CA） tests prove that MMT@Zn anode exhibits superior adsorption capacity for Zn2+and better hydrophobicity than the bare Zn anode,thereby achieving excellent cycling ***,the MMT@Zn||MMT@Zn symmetric cell holds the stable cycling over 5600 h at 0.5 mA cm-2and 0.125 m A h cm-2,even exceeding 1800 h long cycling under harsh conditions of 5 m A cm-2and 1.25 m A h *** MMT@Zn||V2O5full cell reaches over 3000 cycles at 2 A g-1with excellent rate ***,this surface engineering modification strategy for enhancing the electrochemical performance of AZIBs represents a promising application.

关键词： Surface engineering strategy Montmorillonite layer Protection mechanism of Zn anode Cycling stability Aqueous zinc ion batteries