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Enhancing hydrogen evolution and oxidation kinetics through oxygen insertion into nickel lattice

Journal of Energy Chemistry 2024年第8期95卷 529-539页

作者： Wanli Liang Xiyu Gong Jinchang Xu Zixuan Dan Fanyan Xie Hulei Yu Hao-Fan Wang Yanshuo Jin Hongjuan Wang Yonghai Cao Hui Meng Hao Yu School of Chemistry and Chemical Engineering South China University of Technology Siyuan Laboratory Guangzhou Key Laboratory of Vacuum Coating Technologies and New Energy Materials Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy Materials Guangdong Provincial Key Laboratory of Optical Fiber Sensing and Communications Department of Physics Jinan University GBA Branch of Aerospace Information Research Institute Chinese Academy of Sciences Instrumental Analysis & Research Center Sun Yat-sen University School of Materials Science and Engineering South China University of Technology

Nickel-based materials,including metallic Ni and Ni oxide,have been widely studied in the exploration of non-precious-metal hydrogen electrocatalysts,but neither pure Ni nor NiO is ideal for the hydrogen evolution reaction（HER） and hydrogen oxidation reaction（HOR）.In this paper,an oxygen insertion strategy was applied on nickel to regulate its hydrogen electrocatalytic performance,and the oxygen-inserted nickel catalyst was successfully obtained with the assistance of tungsten dioxide support（denoted as O-Ni/WO2）.The partial insertion of oxygen in Ni maintains the face-centered cubic arrangement of Ni atoms,simultaneously expanding the lattice and increasing the lattice spacing.Consequently,the adsorption strength of*H and*OH on Ni is optimized,thus resulting in superior electrocatalytic performance of0-Ni/WO2in alkaline HER/HOR.The Tafel slope of O-Ni/WO2@NF for HER is 56 mV dec-1,and the kinetic current density of O-Ni/WO2for HOR reaches 4.85 mA cm-2,which is ahead of most currently reported catalysts.Our proposed strategy of inserting an appropriate amount of anions into the metal lattice could provide more possibilities for the design of high-performance catalysts.

关键词： Adsorption free energy hydrogen evolution hydrogen oxidation Nickel Oxygen insertion

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Delicate surface vacancies engineering of Ru doped MOF-derived Ni-NiO@C hollow microsphere superstructure to achieve outstanding hydrogen oxidation performance

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Journal of Energy Chemistry 2022年第9期31卷 395-404,I0011页

作者： Yuting Yang Yi Huang Shuqing Zhou Yi Liu Luyan Shi Tayirjan Taylor Isimjan Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004GuangxiChina Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST) Thuwal 23955-6900Saudi Arabia

Surface vacancy defects,as the bridge between theoretical structural study and the design of heterogenous catalysts,have captured much attention.This work develops a metal-organic framework-engaged replacement-pyrolysis approach to obtain highly dispersed Ru nanoparticles immobilized on the vacancy-rich Ni-NiO@C hollow microsphere(Ru/Ni-NiO@C).Fine annealing at 400°C introduces nickel and oxygen vacancies on Ru/Ni-NiO@C surface,resulting in an improved electrical conductivity and rapid mass-charge transfer efficiency.Ru/Ni-NiO@C with a hollow micro/nanostructure and interconnected meso-porosity favors the maximal exposure of abundant active sites and elevation of hydrogen oxidation reaction(HOR)activity.Experimental results and density functional theory(DFT)calculations reveal that an electronic effect between Ru and Ni-NiO@C,in conjunction with nickel/oxygen vacancies in the NiO species could synergistically optimize hydrogen binding energy(HBE)and hydroxide binding energy(OHBE).The HBE and OHBE optimizations thus created confer Ru/Ni-NiO@C with a mass activity over 7.75 times higher than commercial Pt/C.Our work may provide a constructive route to make a breakthrough in elevating the hydrogen electrocatalytic performance.

关键词： Ru/Ni-NiO@C Vacancy defects Electrocatalysis Metal-organic framework hydrogen oxidation

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Activity and Stability of Rare Earth-Based Hydride Alloys as Catalysts of hydrogen Absorption-oxidation Reactions

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Journal of Rare Earths 2004年第6期22卷 871-874页

作者：应桃开高学平胡伟康 Noréus Dag College of Biology and Chemistry Zhejiang Normal University Jinhua 321004China Institute of New Energy Material Chemistry Nankai University Tianjin 300071China Department of Structural Chemistry Arrhenius Laboratory Stockholm University S-106 91 Stockholm Sweden

Rare earth-based AB(5)-type hydrogen storage alloys as catalysts of hydrogen-diffusion electrodes for hydrogen absorption and oxidation reactions in alkaline fuel cells were investigated. It is demonstrated that the metahydride hydrogen-diffusion electrodes could be charged by hydrogen gas and electrochemically discharged, at the same time to retain a stable oxidation potential for a long period. The catalytic activities and stability are almost comparable with a Pt catalyst on the active carbon. Further improvement of performances is expected via reduction of catalyst size into nanometers.

关键词： inorganic chemistry electrocatalyst alkaline fuel cell hydrogen oxidation rare earths

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Remarkably Enhanced hydrogen oxidation Reaction Activity of Carbon-supported Pt by Facile Nickel Modification

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Chemical Research in Chinese Universities 2020年第1期36卷 105-109页

作者： HUANG Xuewei LONG Chang HAN Jianyu ZHANG Jing QIU Xueying TANG Zhiyong College of Chemistry Zhengzhou UniversityZhengzhou 450001P.R.China CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190P.R.China School of Materials Science and Engineering Harbin Institute of TechnologyHarbin 150080P.R.China Institute of Applied Chemistry Shanxi UniversityTaiyuan 030006P.R.China

Developing high activity catalysts for hydrogen oxidation reaction(HOR)under alkaline condition remains a challenge in the exchange membrane fuel cell(AEMFC).Herein,we report that the activity of carbon-supported platinum(Pt/C)towards the hydrogen oxidation reaction(HOR)in alkaline media can be remarkably enhanced by simple immersion of Pt/C in nickel chloride solution.The adsorption of hydrogen on the catalyst surface is weakened by modification of nickel.The HOR activity on the Pt/C after immersion possesses an excellent mass current density of 33.4 A/gmetal,which is 18%higher than that(28.3 A/gmetal)on Pt/C.

关键词： Electrocatalyst hydrogen oxidation Pt/C Modified nickel

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Mathematical Modeling of the Process for Coupled Propane Dehydrogenation and hydrogen oxidation

Mathematical Modeling of the Process for Coupled Propane Deh...

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作者： Md Sayeed Reza 华东理工大学

学位级别：硕士

The growing consumption of propylene derivatives has profoundly increased the propylene demand in recent years.Propane dehydrogenation is believed to have a great potential as a propene booster in the future.In contrast to conventional catalytic dehydrogenation,alternative approach for obtaining higher-than-equilibrium olefin yields and for making the overall process thermal neutral or exothermic is a combination process of catalytic dehydrogenation and selective hydrogen oxidation.But,the process becomes complex due to coupling of dehydrogenation and selective hydrogen oxidation.This research is focused on designing a mathematical model for the coupled process of propane dehydrogenation and hydrogen oxidation in order to achieve better propane conversion and high selectivity based on the kinetics of Pt-Sn/Al2O3 catalyst.A mathematical model has been designed with recycle stream.In this model,an adiabatic CSTR has been designed as a propane dehydrogenation reactor and an adiabatic fixed bed reactor has been designed for hydrogen oxidation.The principal idea of this coupled process is to supply heat for propane dehydrogenation by selective combustion of the hydrogen molecules formed in the dehydrogenation process,which can make the overall process heat-balanced or slightly exothermic and propane conversion also increases.Another benefit is that the resultant steam can prevent coke formation and therefore inhibit the deactivation of catalyst in fixed bed reactor and the catalyst activity in CSTR can be controlled by controlling the continuous regeneration of catalyst in regeneration reactor.

关键词： propane dehydrogenation hydrogen oxidation selective hydrogen combustion recycle stream

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