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Mitigating the Reconstruction of Metal Sulfides for Ultrastable Oxygen Evolution at high current density

CCS Chemistry 2024年第1期6卷 137-148页

作者： Shuai Niu Tang Tang Yuanju Qu Yuyun Chen Hao Luo Hui Pan Wen-Jie Jiang Jianan Zhang Jin-Song Hu Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190 Joint Key Laboratory of the Ministry of Education Institute of Applied Physics and Materials EngineeringUniversity of MacaoMacao SAR 999078 Department of Chemical Engineering University of MelbourneParkvilleVictoria 3010 College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049 Dalian National Laboratory for Clean Energy Dalian 116023

Metal sulfides are emerging highly active electrocatalysts for the oxygen evolution reaction(OER),but still suffer from the instability caused by their inevitable reconstruction,especially at industrial-level current density.Here,it is discovered that Fe-incorporated Ni3S2 nanowires can deliver extraordinary durability with an ultralow potential degradation rate of 0.006 mV/h in alkaline electrolytes made with fresh water and seawater at a benchmark of 500 mA cm^(-2) while meeting the industrial activity requirement for overpotential less than 300 mV(290 mV).Systematic experiments and theoretical simulations suggest that after forming the S-doped NiFeOOH shell to boost intrinsic activity,Fe incorporation effectivelymitigates the reconstruction of the Ni_(3)S_(2) nanowire core by restraining Ni oxidation and S dissolution,justifying the performance.This work highlights the significance of circumventing reconstruction and provides a strategy to explore practical chalcogenides-based OER electrocatalysts.

关键词： oxygen evolution reaction sulfur-doped NiFeOOH NiFe sulfides nanowire ultrastable high current density

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Aligned porous carbon film with ultralow loadings of Pt single atoms and clusters for high-current-density hydrogen generation

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Nano Research 2023年第1期16卷 256-263页

作者： Rui Liu Zhichao Gong Minmin Yan Gonglan Ye Huilong Fei Advanced Catalytic Engineering Research Center of the Ministry of Education State Key Laboratory for Chemo/Biosensing and Chemometricsand College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

The development of electrocatalysts toward the hydrogen evolution reaction(HER)with high-current-density capability is critical for the practical application of water splitting for hydrogen production.While Pt-based materials are regarded as the most efficient HER catalysts,they suffer from scarcity and high price.Thus,it is of vital importance to lower the loading of Pt while maintaining high activity.Here,we report the fabrication of a monolithic aligned porous carbon film electrode co-modified with Pt single atoms and Pt nanoclusters(Pt SA/NC-AF)containing ultralow Pt content(0.038 wt.%)via a facile electrochemical deposition process.Benefiting from the aligned porous structure of the carbon film and the high exposure of the Pt species,the optimized Pt SA/NCAF electrode exhibits outstanding HER performance in 0.5 M H_(2)SO_(4)with exceptional intrinsic activity(turnover frequency(TOF)=904.9 s^(−1)atη=100 mV)and ultrahigh mass activity(888.6 A·mg_(Pt)^(−1)atη=100 mV).Further,it can deliver an industrially relevant current density of 1,000 mA·cm−2 at an overpotential as low as 139 mV.This work provides a feasible avenue for the rational design of metal single-atom and nanocluster catalysts and additionally promotes the application of ultralow-loading noble metal-based catalysts in high-rate hydrogen production.

关键词： monolithic electrodes single atoms clusters hydrogen evolution reaction high current density

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RuO_(2)/TiO_(2)/MXene with multi-heterojunctions coating on carbon cloth for high-activity chlorine evolution reaction at large current densities

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Nano Research 2024年第6期17卷 4764-4772页

作者： Yuhao Duan Liuxu Wei Chenyu Cai Junbao Mi Fuyuan Cao Jiaze Chen Xiaolong Li Xiujiang Pang Bin Li Lei Wang Key Laboratory of Eco-chemical Engineering Ministry of EducationInternational Science and Technology Cooperation Base of Eco-chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266042China

The chlorine evolution reaction(CER)is a crucial step in the production of chlorine gas and active chlorine by chlor-alkali electrolysis.currently,the endeavor to fabricate electrodes capable of yielding high current density at minimal overpotential remains a central challenge in advancing the realm of chlorine evolution reactions.Here,we grow TiO_(2)and RuO_(2)on MXene@carbon cloth(CC)through the favorable affinity and induced deposition effect between the surface functional groups of MXene and the metal.A self-supported electrode(RuTiO_(2)/MXene@CC)with strong binding at the electrocatalyst-support interface and weak adhesion at electrocatalyst-bubble interface is constructed.The RuTiO_(2)/MXene@CC can reduce the electron density of RuO_(2)by regulating the electron redistribution at the heterogeneous interface,thus enhancing the adsorption of Cl−.RuTiO_(2)/MXene@CC could achieve a high current density of 1000 mA·cm^(−2)at a small overpotential of 220 mV,superior to commercial dimensionally stable anodes(DSA).This study provides a new strategy for constructing efficient CER catalysts at high current density.

关键词： chlorine evolution reaction high current density MXene TiO_(2) RuO_(2)

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Amorphous porous sulfides nanosheets with hydrophilic/aerophobic surface for high-current-density water splitting

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Chinese Chemical Letters 2023年第7期34卷 230-235页

作者： Xiaoli Wu Sheng Zhao Lijie Yin Luqi Wang Linlin Li Feng Hu Shengjie Peng Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies College of Materials Science and TechnologyNanjing University of Aeronautics and AstronauticsNanjing 210016China

The rational construction of electrocatalysts with desired features is significant but challenging for superior water splitting at high current density. Herein, amorphous Co Ni S nanosheets are synthesized on nickel foam(NF) through a facile structure evolution strategy and present advanced performance at high current densities in water splitting. The high catalytic activity can be attributed to the sufficient active sites exposed by the flexible amorphous configuration. Moreover, the hydrophilicity and aerophobicity of a-CoNiS/NF promote surface wettability of the self-supporting electrode and avoid the aggregation of bubbles, which expedites the diffusion of electrolyte and facilitates the mass transfer. As a result, the optimized electrode demonstrates low overpotentials of 289 and 434 m V at 500 m A/cm^(2) under alkaline conditions for hydrogen evolution reaction(HER) and oxygen evolution reaction(OER), respectively. Impressively, an electrolytic water splitting cell assembled by bifunctional a-Co Ni S/NF operates with a low cell voltage of 1.46 V@10 mA/cm^(2) and reaches 1.79 V at 500 mA/cm^(2). The strategy sheds light on a competitive platform for the reasonable design of non-precious-metal electrocatalysts under high current density.

关键词： Electrocatalysts Metal-organic frameworks Amorphous high current density Overall water splitting

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Regulation of hydrogen evolution performance of titanium oxide-carbon composites at high current density with a Ti-O hybrid orbital

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Carbon Energy 2022年第3期4卷 480-490页

作者： Meichen Liu Zhiping Lei Qingping Ke Peixin Cui Jiancheng Wang Jingchong Yan Zhanku Li Hengfu Shui Shibiao Ren Zhicai Wang Ying Kong Shigang Kang Anhui Province Key Laboratory of Coal Clean Conversion and high Valued Utilization Institute of Material Science&EngineeringSchool of Chemistry&Chemical EngineeringAnhui University of TechnologyMa'anshanChina Key Laboratory of Soil Environment and Pollution Remediation Institute of Soil ScienceThe Chinese Academy of SciencesNanjingChina Key Laboratory of Coal Science and Technology Ministry of Education and Shanxi ProvinceTaiyuan University of TechnologyTaiyuanChina

Rational design and controllable synthesis of practical electrodes with high sta bility and activity at high current density for a hydrogen evolution reaction(HER)are critical for renewable and sustainable energy conversion.However,high-performance TiO_(2)-based electrocatalysts for HER are quite limited,and the cat alytic active centers still remain elusive.Herein,a simple strategy is demonstrated for the synthesis of TiO_(2)-carbon composite(TiO_(2)/C)with high HER performance and stability.The remarkable HER performance of TiO_(2)/C can be ascribed to the doping of carbon atoms,which leads to stronger hybridization of Ti 3d and O 2p orbitals,thus substantially improving the electrocatalytic efficiency.This study elucidates that the hydrogen evolution activity of oxide electrocatalysts can be largely improved by regulating their electronic structures by doping carbon atoms and also provides an effective strategy for designing heterostructured electro catalysts with high catalytic activity and stability at high current density for HER.

关键词： C doping HER high current density Ti-O hybridization TiO_(2)/C

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Synergized oxygen vacancies with Mn_(2)O_(3)@CeO_(2)heterojunction as high current density catalysts for Li-O_(2)batteries

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Chinese Journal of Structural Chemistry 2023年第11期42卷 40-49页

作者： Renshu Huang Jinli Chen Xingfa Chen Tianqi Yu Huyi Yu Kaien Li Bin Li Shibin Yin Guangxi Key Laboratory of Electrochemical Energy Materials School of Chemistry and Chemical EngineeringGuangxi University100 Daxue RoadNanning530004China

The application of Li-O_(2)batteries(LOBs)with ultra-high theoretical energy density is limited due to the slow redox kinetics and serious side reactions,especially in high-rate cycles.Herein,CeO_(2)is constructed on the surface of Mn_(2)O_(3)through an interface engineering strategy,and Mn_(2)O_(3)@CeO_(2)heterojunction with good activity and stability at high current density is prepared.The interfacial properties of catalyst and formation mechanism of Li_(2)O_(2)are deeply studied by density functional theory(DFT)and experiments,revealing the charge-discharge reaction mechanism of LOBs.The results show that the strong electron coupling between Mn_(2)O_(3)and CeO_(2)can promote the formation of oxygen vacancies.Heterojunction combined with oxygen vacancy can improve the affinity for O_(2)and LiO_(2)reaction intermediates,inducing the formation of thin-film Li_(2)O_(2)with low potential and easy decomposition,thus improving the cycle stability at high current density.Consequently,it achieved a high specific capacity of 12545 at 1000 mA g^(-1)and good cyclability of 120 cycles at 4000 mA g^(-1).This work thus sheds light on designing efficient and stable catalysts for LOBs under high current density.

关键词： Li-O_(2)batteries Oxygen vacancies Catalyst high current density Heterojunction

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N‑Doped Graphene‑Decorated NiCo Alloy Coupled with Mesoporous NiCoMoO Nano‑sheet Heterojunction for Enhanced Water Electrolysis Activity at high current density

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Nano-Micro Letters 2021年第5期13卷 77-89页

作者： Guangfu Qian Jinli Chen Tianqi Yu Lin Luo Shibin Yin College of Chemistry and Chemical Engineering MOE Key Laboratory of New Processing Technology for Nonferrous Metals and MaterialsState Key Laboratory of Processing for Non‑Ferrous Metal and Featured MaterialsGuangxi University100 Daxue RoadNanning 530004P.R.China

Developing highly effective and stable non-noble metalbased bifunctional catalyst working at high current density is an urgent issue for water electrolysis(WE).Herein,we prepare the N-doped graphene-decorated NiCo alloy coupled with mesoporous NiCoMoO nano-sheet grown on 3D nickel foam(NiCo@C-NiCoMoO/NF)for water splitting.NiCo@C-NiCoMoO/NF exhibits outstanding activity with low overpotentials for hydrogen and oxygen evolution reaction(HER:39/266 mV;OER:260/390 mV)at±10 and±1000 mA cm^(−2).More importantly,in 6.0 M KOH solution at 60℃ for WE,it only requires 1.90 V to reach 1000 mA cm−2 and shows excellent stability for 43 h,exhibiting the potential for actual application.The good performance can be assigned to N-doped graphene-decorated NiCo alloy and mesoporous NiCoMoO nano-sheet,which not only increase the intrinsic activity and expose abundant catalytic activity sites,but also enhance its chemical and mechanical stability.This work thus could provide a promising material for industrial hydrogen production.

关键词： N-doped graphene-decorated NiCo alloy Catalyst Mesoporous nano-sheet Water electrolysis high current density

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A theoretical analysis of the electromigration-induced void morphological evolution under high current density

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Acta Mechanica Sinica 2017年第5期33卷 868-878页

作者： Yuexing Wang Yao Yao School of Mechanics and Civil Engineering Northwestern Polytechnical University

In this work, analysis of electromigration-induced void morphological evolution in solder interconnects is performed based on mass diffusion theory. The analysis is conducted for three typical experimentally observed void shapes: circular, ellipse, and cardioid. Void morphological evolution is governed by the competition between the electric field and surface capillary force. In the developed model, both the electric field and capillary force on the void's surface are solved analytically. Based on the mass conversation principle, the normal velocity on the void surface during diffusion is obtained. The void morphological evolution behavior is investigated, and a physical model is developed to predict void collapse to a crack or to split into sub-voids under electric current. It is noted that when the electric current is being applied from the horizontal direction, a circular void may either move stably along the electric current direction or collapse to a finger shape, depending on the relative magnitude of the electric current and surface capillary force. However, the elliptical-shaped void will elongate along the electric current direction and finally collapse to the finger shape. On the other hand, the cardioid-shaped void could bifurcate into two sub-voids when the electric current reaches a critical value. The theoretical predictions agree well with the experimental observations.

关键词： Electromigration Analytical solution Void evolution high current density Mass diffusion

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Fabrication of Large Scale Self-supported WC/Ni(OH)_(2) Electrode for high-current-density Hydrogen Evolution

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Chinese Journal of Structural Chemistry 2021年第10期40卷 1365-1371页

作者： LI Ping-Yu HONG Wen-Ting LIU Wei CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100049China

In the industry, cheap and stable electrocatalysts are eagerly expected for hydrogen evolution reaction(HER) at a high current density. Two-component electrochemical catalysts with integrated multiple interfaces seem to be an expedient strategy to enhance the inherent electronic structure of hybrid electrocatalysts and optimize the catalytic ability. In this work, we report an active tungsten carbide and nickel hydroxide(WC/Ni(OH)_(2)) electrocatalyst seamlessly synthesized on the substrate of W foil. Ni(OH)_(2) trends to adsorb OH_(ad) and WC can effectively adsorb H_(ad). Prompted by the synergistic effect, the ability of the catalyst manifests an effective HER kinetics with an overpotential of 475 m V(vs. RHE) at a high current density of 1000 m A/cm^(2) in 1 M KOH. Moreover, due to its self-supported construction, the catalyst presents reliable long-term stability with no obvious active property loss after 8000 cycles and 50 hours of operation in an alkaline solution.

关键词： hydrogen evolution reaction tungsten carbide nickel hydroxide high current density

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Analysis and Numerical Simulation of Forced Cooling in Induction Coils With high current density

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Journal of Iron and Steel Research(International) 2012年第S2期19卷 758-761页

作者： BRESSAN Fernando FORZAN Michele LUPI Sergio NIKANOROV Aleksandr NACKE Bernard University of Padua Department of Electrical Engineering Institute of Electrotechnology Leibniz Universitat Hannover

A static model of the forced cooling of inductors used for induction heating is proposed in order to achieve better coil design to prolong its lifetime and prevent failures.The main aim is to define for the most common copper tubes and inductor geometries an equivalent convection heat transmission coefficient depending upon temperature and pressure of the cooling fluid,in order to model the very complex physics of forced cooling with a strongly simplified method.The model,called 'Line Region Model',considers only the coil's copper tube and its internal surface(interface copper-water)as boundary where the heat exchange conditions are imposed.

关键词： coefficient of heat transfer by convection forced cooling of inductor high current density

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