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Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2025年第1期100卷 226-233页

作者： Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang Key Laboratory of Green chemical engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical Technology School of Chemical Engineering & Pharmacy Wuhan Institute of Technology Key Laboratory of Pesticide & chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education College of Chemistry Central China Normal University College of Materials Science and engineering Fuzhou University

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction（OER）. Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER process. However, most of them undergo incomplete reconstruction with limited thickness of reconstruction layer, leading to low component utilization and arduous exploration of real catalytic mechanism. Herein, we identify the dynamic behaviors in complete reconstruction of Co-based complexes during OER. The hollow phytic acid（PA） cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability, in favor of the fast and complete reconstruction. A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co（Fe）(OH)xand subsequent potential-driven oxidation to Co（Fe）OOH. The obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm-2and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER activity. The work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Complete reconstruction Co-based complex Precatalysts Oxygen evolution reaction

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

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

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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Prominent cycling reversibility and kinetics enabled by CaTiO3 protective layer on Zn metal for aqueous Zn-ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 245-258页

作者： Gaeun Lee Yong Nam Ahn Seongjoon So Chanwoo Park Jong-Seong Bae Taehyun Park Il Tae Kim Jaehyun Hur school of chemical Biological and Battery Engineering Gachon University Seongnam Busan Center Korea Basic Science Institute

Aqueous Zn-ion batteries （AZIBs） have received considerable attention owing to their various advantages such as safety,low cost,simple battery assembly conditions,and high ionic ***,they still suffer from serious problems,including uncontrollable dendrite growth,corrosion,hydrogen evolution reaction （HER） from water decomposition,electrode passivation,and unexpected *** creation of a uniform artificial nanocrystal layer on the Zn anode surface is a promising strategy for resolving these ***,we propose the use of a perovskite CaTiO3（CTO） protective layer on Zn（CTO@Zn） as a promising approach for improving the performance of *** CTO artificial layer provides an efficient pathway for Zn ion diffusion towards the Zn metal because of the high dielectric constant （εr=180） and ferroelectric characteristics that enable the alignment of dipole moments and redistribute the Zn2+ions in the CTO *** avoiding the direct contact of the Zn anode with the electrolyte solution,the uneven dendrite growth,corrosion,parasitic side reactions,and HER are mitigated,while CTO retains its mechanical and chemical robustness during ***,CTO@Zn demonstrates an improved lifespan in a symmetric cell configuration compared with bare ***@Zn shows steady overpotential （～68 m V） for 1500 h at 1 mA cm-2/0.5 mA h cm-2,excelling bare ***,when paired with the V2O5-C cathode,the CTO@Zn//V2O5-C full battery delivers 148.4 mA h g-1（based on the mass of the cathode） after 300 *** study provides new insights into Zn metal anodes and the development of high-performance AZIBs.

关键词： Artificial layer Dielectric constant Zn metal anode Zinc aqueous battery

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

Quickly obtaining densely dispersed coherent particles in steel matrix and its related mechanical property

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 111-118页

作者： Xiaoxiao Wang Qingsong Huang school of chemical engineering Sichuan UniversityChengdu 610065China

Densely distributed coherent nanoparticles(DCN)in steel matrix can enhance the work-hardening ability and ductility of steel *** the routes to this end can be generally classified into the liquid-solid route and the solid-solid ***,the formation of DCN structures in steel requires long processes and complex *** far,obtaining steel with coherent particle enhancement in a short time remains a bottleneck,and some necessary steps remain ***,we show a high-efficiency liquid-phase refining process reinforced by a dynamic magnetic ***-Y-Mn-O particles had an average size of around(3.53±1.21)nm and can be obtained in just around 180 *** small nanoparticles were coherent with the matrix,implying no accumulated dislocations between the particles and the steel *** findings have a potential application for improving material machining capacity,creep resistance,and radiation resistance.

关键词： ferritic steels coherent particles microstructure compression test work hardening

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Low-cost and fluoride-free synthesis of MFI zeolite nanosheets with enhanced stability for benzene alkylation with ethanol

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Journal of Energy Chemistry 2025年第1期100卷 458-468页

作者： Peng Zhu Cun Liu Yiren Yu Guoshu Gao Yumeng Zhao Xiongfu Zhang Guodong Liu Guohui Yang State Key Laboratory of Fine chemicals School of Chemical Engineering Dalian University of Technology State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented *** obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.

关键词： MFI zeolite ZSM-5 Nanosheets Scale-up synthesis Aromatic alkylation

From waste to wealth:Coal tar residue derived carbon materials as low-cost anodes for potassium-ion batteries

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 464-475页

作者： Zhonghua Lu Jun Shen Xin Zhang Lingcong Chao Liang Chen Ding Zhang Tao Wei Shoudong Xu College of chemical engineering and Technology Taiyuan University of TechnologyTaiyuan 030024China College of Chemistry Taiyuan University of TechnologyTaiyuan 030024China school of chemical engineering and pharmacy Wuhan Institute of TechnologyWuhan 430205China school of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212003China

Carbon materials are widely recognized as highly promising electrode materials for various energy storage system *** tar residues(CTR),as a type of carbon-rich solid waste with high value-added utilization,are crucially important for the development of a more sustainable *** this study,we employed a straightforward direct carbonization method within the temperature range of 700-1000℃to convert the worthless solid waste CTR into economically valuable carbon materials as anodes for potassium-ion batteries(PIBs).The effect of carbonization temperature on the microstructure and the potassium ions storage properties of CTR-derived carbons(CTRCs)were systematically explored by structural and morphological characterization,alongside electrochemical performances *** on the co-regulation between the turbine layers,crystal structure,pore structure,functional groups,and electrical conductivity of CTR-derived carbon carbonized at 900℃(CTRC-900H),the electrode material with high reversible capacity of 265.6m Ah·g^(-1)at 50 m A·g^(-1),a desirable cycling stability with 93.8%capacity retention even after 100 cycles,and the remarkable rate performance for PIBs were ***,cyclic voltammetry(CV)at different scan rates and galvanostatic intermittent titration technique(GITT)have been employed to explore the potassium ions storage mechanism and electrochemical kinetics of *** indicate that the electrode behavior is predominantly governed by surface-induced capacitive processes,particularly under high current densities,with the potassium storage mechanism characterized by an“adsorption-weak intercalation”*** work highlights the potential of CTR-based carbon as a promising electrode material category suitable for high-performance PIBs electrodes,while also provides valuable insights into the new avenues for the high value-added utilization of CTR.

关键词： coal tar residue carbon materials anode potassium-ion batteries high value-added

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