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molten salt electrochemical modulation of Ni/Co nanoparticles onto N-doped carbon for oxygen reduction

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Journal of Energy Chemistry 2022年第11期31卷 212-217,I0007页

作者： Xinxin Liang Jialin Chen Biao Hong Tingting Wan Wei Weng Wei Xiao College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power SourcesWuhan UniversityWuhan 430072HubeiChina Zijin School of Geology and Mining Fujian Key Laboratory of Green Extraction and High-value Utilization of Energy MetalsFuzhou UniversityFuzhou 350108FujianChina Queen Marry University of London Engineering School Northwestern Polytechnical UniversityXi’an 710129ShaanxiChina

Activation of oxygen over non-precious materials has been an imperative task to develop efficient electrochemical energy storage and conversion such as fuel cells and metal-air batteries.Herein,a molten salt electrochemical modulation of metal-nitrogen-carbon based compounds(M–N–C)is achieved.By electrochemical treatment of polydopamine-coated NiCo_(2)O_(4)(NiCo_(2)O_(4)@PDA)in molten Li_(2)CO_(3)-Na_(2)CO_(3)-K_(2)CO_(3)at 500℃,Ni/Co bimetal-nitrogen-carbon catalyst(denoted as Ni/Co@NC)consisting of Ni-Co nanoparticles anchoring on porous nitrogen-doped carbon is constructed and evaluated as electrocatalysts towards the oxygen reduction reaction(ORR).Experimental and calculation results confirm that alloying of Ni-Co and nitrogen doping to carbon enhances the rate-determining transformation of*OH intermediate during ORR.The Ni/Co@NC hence shows an ORR activity comparable with the commercial Pt/C.

关键词： Oxygen reduction Metal-nitrogen-carbon Electrochemistry molten salt Bimetal modulation

molten salt assisted fabrication of Fe@Fe_(SA)-N-C oxygen electrocatalyst for high performance Zn-air battery

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Journal of Energy Chemistry 2021年第10期30卷 612-621,I0016页

作者： Wenjun Zhang Kaicai Fan Cheng-Hao Chuang Porun Liu Jian Zhao Dongchen Qi Lingbo Zong Lei Wang Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technology Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life ScienceMOEState Key Laboratory of Eco-chemical EngineeringCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina Key Laboratory of Rubber-Plastics Ministry of Education/Shandong Provincial Key Laboratory of Rubber-PlasticsQingdao University of Science and TechnologyQingdao 266042ShandongChina Centre for Clean Environment and Energy School of Environment and ScienceGriffith UniversityQueensland 4222Australia Department of Physics Tamkang UniversityTamsui 251New Taipei City 251301TaiwanChina School of Chemistry and Physics Centre for Materials ScienceQueensland University of TechnologyBrisbaneQueensland 4001Australia

Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.

关键词： molten salt Oxygen reduction reaction Long-term durability Zn-air batteries

molten-salt synthesis of porous La0.6Sr0.4Co0.2Fe0.8O2.9 perovskite as an efficient electrocatalyst for oxygen evolution

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Nano Research 2018年第9期11卷 4796-4805页

作者： Sanzhao Song Jing Zhou Shuo Zhang Linjuan Zhang Jiong Li Yu Wang Ling Han Youwen Long Zhiwei Hu Jian-Oiang Wang Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai 201800 China University of Chinese Academy of Sciences Beijing 100049 China Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China Collaborative Innovation Center of Quantum Matter Beijing 100190 China Max Planck Institute for Chemical Physics of Solids Nothnitzer Strasse 40 Dresden 01187 Germany

The development of an efficient and low-cost electrocatalyst for the oxygen evolution reaction （OER） via an eco-efficient route is a desirable, although challenging, outcome for overall water splitting. Herein, an iron-rich La0.6Sr0.4Co0.2Fe0.8O2.9 （LSCF28） perovskite with an open porous topographic structure was developed as an electrocatalyst by a straightforward molten-salt synthesis approach. It was found that porosity correlates with both the iron content and the molten-salt approach. Benefiting from the large surface area, high activity of the porous internal surface, and the optimal electronic configuration of redox sites, this inexpensive material exhibits high performance with a large mass activity of 40.8A·g^-1 at a low overpotential of 0.345 V in 0.1 M KOH, surpassing the state-of-the-art precious metal IrO2 catalyst and other well-known perovskites, such as Ba0.5Sr0.5Co0.8Fe0.2O3 and SRCoO2.7. Our work illustrates that the molten- salt method is an effective route to generate porous structures in perovskite oxides, which is important for energy conversion and storage devices.

关键词： iron-rich perovskite oxygen evolution reaction energy storage and conversion molten salt

Experimental Study on the molten salt at Micron Scale during the Melting Process

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Journal of Thermal Science 2024年第1期33卷 70-85页

作者： TIAN Ziqian LIAO Zhirong XU Chao FANG Yongzhe JIANG Kaijun YUAN Mengdi Key Laboratory of Power Station Energy Transfer Conversion and System Ministry of Education of ChinaSchool of Energy Power and Mechanical EngineeringNorth China Electric Power UniversityBeijing 102206China

The investigation of the melting behaviors of the molten salt at micron scale during the melting process is critical for explaining the solid-liquid phase transition mechanism.In this paper,a novel experimental system and analysis method were proposed to study the melting process with three heating rates in the range of1-10℃/min of the solar salt at micron scale.The solid-liquid boundary morphology and phase transition kinetics of molten salt particles were focused on.Meanwhile,the correlations between liquid fraction,temperature and time under different heating rates were studied.The solid-liquid boundary morphology was depicted by the visualized experimental set-up,and the instantaneous liquid volume fraction during the non-isothermal phase transition was obtained.Then,the correlation between temperature and liquid volume fraction was proposed to reveal the evolution of the solid-liquid boundary with temperature at different heating rates.Furthermore,the non-isothermal phase transition kinetic equation was established by introducing a constant parameter(V_(a,b)),and more kinetic parameters such as 1g V_(a,b) and-lg V_(a,b)/b were studied.The results showed that the exponent b is not sensitive to the heating rate with a range of 3-5 for solar salt particles.However,the heating rate influences the value of V_(a,b) and presents a positive relationship.Besides,the non-isothermal phase transition kinetic equations at different heating rates in the range of 1-10℃/min can be quickly predicted by the proposed improved experimental test method.This study could fill the research insufficiency and provide significant guidance for future research on the solid-liquid transition mechanism of molten salts at micron scale.

关键词： molten salt non-isothermal phase transition solid-liquid boundary morphology liquid volume fraction micron scale melting process

Efficient molten salt CO_(2)capture and selective electrochemical transformation processes toward carbon neutrality:advances,challenges,and prospects

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Science China Chemistry 2023年第11期66卷 3116-3135页

作者： Bowen Deng Huayi Yin Kaifa Du Dihua Wang School of Resource and Environmental Sciences Hubei International Scientific and Technological Cooperation Base of Sustainable Resource and EnergyWuhan UniversityWuhan 430072China

Atmospheric carbon dioxide(CO_(2))concentration has reached record levels due to excessive anthropogenic CO_(2)emissions from massive industrial productions.Renewable-energy-driven CO_(2)electroreduction is an effective method of directly converting CO_(2)into various value-added chemicals or materials without subsequent geological disposal treatment.Owing to their promising thermal stability,wide electrochemical window,tunable oxo-basicity,and nontoxic nature,molten salt electrolytes endow intrinsic advantages,such as fast CO_(2)absorption and selective electrochemical transformation,among different electrolyte species,wherein advanced carbon materials,CO,and hydrocarbons can be generated at relatively high current densities.Herein,we review the recent advances in molten salt CO_(2)capture and electrochemical transformation(MSCC-ET)technologies,including reaction mechanisms,CO_(2)absorption kinetics,electrode reaction kinetics,and product selectivity.This review highlights feasible strategies for regulating nanostructures,carbon product crystallinity,energy efficiency,overall CO_(2)conversion efficiency,and MSCC-ET adaptability toward practical flue gases.Moreover,suitable cost-effective inert anode candidates for the oxygen evolution reaction are discussed.

关键词： carbon dioxide electroreduction CO_(2)capture molten salt electrode reaction energy efficiency

Preparation of RE-containing magnesium alloys via molten-salt-mediated magnesiothermic reduction

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Journal of Magnesium and Alloys 2023年第3期11卷 981-990页

作者： Zhimin Zhang Xuchen Lu Yan Yan State Key Laboratory of Multi-phase Complex systems Institution of Process EngineeringChinese Academy of ScienceHaidian DistrictBeijing 100190PR China

RE-containing magnesium alloys were prepared via molten-salt-mediated magnesiothermic reduction by using RE_(2)O_(3)(RE=Y,Nd and Gd)and Mg metal as raw materials.The thermomechanical analysis of the magnesiothermic reduction reactions in molten salt was investigated.Then the molten-salt-mediated magnesiothermic reduction process was studied from three different perspectives.After that,the RE-containing magnesium alloy was characterized by using chemical analysis,XRD analysis and SEM analysis.The magnesiothermic reduction was a liquid-liquid reaction with relatively weak driving force.During the melting process and the magnesiothermic reduction process,magnesium metal and the obtained alloy went up and down as a whole in molten salt,which improved the process safety without introducing chloride inclusions.Meanwhile,the hydrolysis of the RECl_(3^(-))containing molten salt occurred at elevated temperature,which severely impeded the magnesiothermic reduction process.After the magnesiothermic reduction at 750°C for 2.0 h,the content of RE and the common impurity elements in the obtained RE-containing alloy met the both requirements of the commercial WE43A and WE43B.

关键词： Magnesium alloy Rare earth Magnesiothermic reduction molten salt

molten salt Electrolytic Fabrication of TiC-CDC and Its Applications for Supercapacitor

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Journal of Materials Science & Technology 2017年第8期33卷 788-792页

作者： Chaopin Wan Rongxia Zhang Shulan Wang Xuan Liu Department of Chemistry School of Science Northeastern University Department of Materials Science and Engineering Carnegie Mellon University

Titanium carbide derived carbon（TiC-CDC） was prepared by the molten salt electrolytic method in molten salt NaCl–KCl at the potential of 1.3 V using TiC pellets as the anode. X-ray diffraction, scanning electron microscopy and Raman spectrum were used to characterize the composition, morphology and microstructure of TiC-CDC. The electrochemical performance of TiC-CDC for supercapacitor was investigated in 0.5 mol L-1Na2SO4 by cycle voltammograms, ac impedance spectrum and galvanostatic charge/discharge. TiC-CDC showed excellent electrochemical and capacitive performances and maintained a capacity value of 126.1 F g-1after 1000 cycles with a capacity retention rate of 97% at the current density of 3 Ag-1. The current work demonstrated the feasibility of molten salt electrolytic method for preparation of TiC-CDC and provided a non-polluting and environmentally friendly strategy for high performance supercapacitor fabrication.

关键词： Supercapacitor Electrochemistry molten salt

Synthesis of vanadium powder by magnesiothermic reduction of V_(2)O_(3)in a reactive molten salt

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Journal of Iron and Steel Research(International) 2023年第4期30卷 650-659页

作者： Da-peng Zhong Gui-shang Pei Jia-long Kang Jun-yi Xiang Cheng Pan Wu-an Gu Xue-wei Lv Lan-jie Li Chongqing Key Laboratory of Vanadium-Titanium Metallurgy and New Materials Chongqing UniversityChongqing 400044China Pangang Group Research Institute Co. Ltd.Panzhihua 617000SichuanChina College of Chemical Engineering Sichuan UniversityChengdu 610065SichuanChina The State Key Laboratory of Mechanical Transmissions Chongqing UniversityChongqing 400044China Chengde Iron and Steel Group Co. Ltd.HBIS Group Co.Ltd.Chengde 067102HebeiChina

As an important strategic metal,vanadium is generally used to prepare special steels,titanium alloys,and hydrogen storage materials.A new method of producing vanadium(metal)powder from V_(2)O_(3)using block Mg is presented herein.Using an auxiliary molten salt,V_(2)O_(3)was successfully transformed into V by Mg reduction.The by-product,MgO,was transformed into MgCl_(2)by adding ZrCl_(4),which prevented the generation of MgV_(2)O_(4)and allowed the reaction to proceed smoothly.The rod-like alloy phases,Zr_(0.03)V_(1.97),which formed in the presence of excess Mg,may hinder the diffusion of oxygen from the product.The recovery rate of vanadium after separation and purification was approximately 45%–50%,where the main loss occurred during ball milling.Under the optimal conditions(Mg content of 48.3%,reduction time of 1.5 h,and temperature of 850℃),the purity of vanadium exceeded 99 wt.%,and the O content decreased to 0.34 wt.%.

关键词： Deoxidation Vanadium powder Magnesiothermic reduction molten salt

Non-contact gaseous microplasma electrode as anode for electrodeposition of metal and metal alloy in molten salt

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Chinese Chemical Letters 2024年第4期35卷 166-169页

作者： Junhan Luo Qi Qing Liqin Huang Zhe Wang Shuang Liu Jing Chen Yuexiang Lu Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084China The MOE Key Laboratory of Resources and Environmental System Optimization College of Environmental Science and EngineeringNorth China Electric Power UniversityBeijing 102206China Nuclear Research Institute for Future Technology and Policy Seoul National UniversitySeoul 08826Republic of Korea

Microplasma based on glow discharge could act as a non-contact gaseous electrode and has attracted much attention in both fundamental research and application. Herein, with microplasma as the anode,the electrodeposition process of a series of metal and metal alloys in molten salt has been systemically studied. Four metal cations with different valence states, silver(Ag~+), nickel(Ni^(2+)), copper(Cu^(2+)), and iron(Fe^(3+)), could all be reduced on the solid cathode with high current efficiency and the corresponding metal products were of high purity. The electrodeposition of aluminum-lanthanum(Al-Ln) alloy on the aluminum cathode was also successfully carried out with microplasma as the anode, and the same alloy was obtained by using the conventional anode electrode. These results indicated that microplasma anode based on non-contact direct-current(DC) glow discharge is a promising electrode to be applied in molten salt electrolysis.

关键词： Microplasma Anode molten salt Electrodeposition Al-Ln alloy