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Efficient bifunctional catalysts of CoSe/N-doped carbon nanospheres supported Pt nanoparticles for methanol electrolysis of hydrogen generation

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Nano Research 2022年第10期15卷 8936-8945页

作者： Yang Zhou Qiaowei Wang Xinlong Tian Ligang Feng School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikou 570228China

methanol electrolysis is significant but challenging as an energy-saving technique for electrochemical hydrogen production.Herein,we demonstrated a novel and efficient bifunctional catalyst of CoSe/N-doped carbon nanospheres supported Pt nanoparticles for hydrogen generation via methanol electrolysis;high catalytic performance for both methanol oxidation(MOR)and hydrogen evolution(HER)was observed benefitting from the effective interaction of metal and support effect as well as the oxophilic characteristics of cobalt selenide.Theoretical calculation disclosed the increased charge density of Pt induced by the CoSe/NC support has a bifunctional ability for optimizing the H*adsorption energy for hydrogen evolution reaction and weakening the CO adsorption energy of methanol oxidation reaction.Specifically,the largely improved CO-tolerance ability was observed in the CO-stripping technique,where about 90 mV less of the peak potential for CO oxidation than that of Pt/C catalyst was observed,resulting from a strong electronic effect as indicated by the spectroscopic analysis.The peak current density of 84.2 mA·cm^(–2) was found for MOR,which was about 3.1 times higher than that of Pt/C;and a low overpotential of 32 mV was required to reach 10 mA·cm^(–2) for HER in 0.5 mol·L^(–1) H_(2)SO_(4) with 1.0 mol·L^(–1) CH3OH.When serviced as both anode and cathode catalyst in a methanol electrolyzer,a low cell potential of 0.67 V to offer 10 mA cm^(-2) was obtained,about 170 mV less than that of Pt/C catalyst;moreover,it was 1.1 V lower than that of water-splitting(1.77 V),indicating a promising energy-saving technique for hydrogen generation.They also showed very good catalytic stability and anti-poisoning ability during the catalysis process.This work would help understand the metal-support interaction for hydrogen generation vis methanol electrolysis.

关键词： bifunctional electrocatalyst methanol electrolysis hydrogen evolution reaction Pt-based catalysts metal-organic frameworks

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Low carbon alcohol fuel electrolysis of hydrogen generation catalyzed by a novel and effective Pt–CoTe/C bifunctional catalyst system

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Green Energy & Environment 2024年第4期9卷 758-770页

作者： Yang Zhou Lice Yu Jinfa Chang Ligang Feng Jiujun Zhang School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou225002JiangsuChina NanoScience Technology Center University of Central FloridaOrlandoFL32826USA College of Sciences&Institute for Sustainable Energy Shanghai UniversityShanghai200444China

Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts for membrane electrode fabrication are required to drive the electrolysis reactions.Herein,the efficient catalytic promotion effect of a novel catalyst promoter,CoTe,on Pt is demonstrated for low carbon alcohol fuels of methanol and ethanol electrolysis for hydrogen generation.Experimental and density functional theory calculation results indicate that the optimized electronic structure of Pt–CoTe/C resulting from the synergetic effect between Pt and CoTe further regulates the adsorption energies of CO and H*that enhances the catalytic ability for methanol and ethanol electrolysis.Moreover,the good water activation ability of CoTe and the strong electronic effect of Pt and CoTe increased the tolerance ability to the poisoning species as demonstrated by the CO-stripping technique.The high catalytic kinetics and stability,as well as the promotion effect,were also carefully discussed.Specifically,71.9%and 75.5%of the initial peak current density was maintained after 1000 CV cycles in acid electrolyte for methanol and ethanol oxidation;and a low overpotential of 30 and 35 mV was required to drive the hydrogen evolution reaction in methanol and ethanol solution at the current density of 10 mA cm^(-2).In the two-electrode system for alcohol fuels electrolysis,using the optimal Pt–CoTe/C catalyst as bi-functional catalysts,the cell potential of 0.66 V(0.67 V)was required to achieve 10 mA cm^(-2) for methanol(ethanol)electrolysis,much smaller than that of water electrolysis(1.76 V).The current study offers a novel platform for hydrogen generation via low carbon alcohol fuel electrolysis,and the result is helpful to the catalysis mechanism understanding of Pt assisted by the novel promoter.

关键词： methanol electrolysis Ethanol electrolysis Cobalt telluride Pt-based electrocatalyst Hydrogen evolution reaction

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