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Customizing the microenvironment of CO_(2) electrocatalysis via three‐phase interface engineering

SmartMat 2022年第1期3卷 111-129页

作者： Xianlong Zhou Hao Liu Bao Yu Xia Kostya(Ken)Ostrikov Yao Zheng Shi‐Zhang Qiao School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSouth AustraliaAustralia Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureWuhanChina National Laboratory for Optoelectronics School of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)China School of Chemistry and Physics and Centre for Materials Science Queensland University of Technology(QUT)BrisbaneAustralia

Converting CO_(2) into high‐value fuels and chemicals by renewable‐electricitypowered electrochemical CO_(2) reduction reaction(CRR)is a viable approach toward carbon‐emissions‐neutral *** the thermocatalytic hydrogenation of CO_(2) at the solid‐gas interface,the CRR takes place at the three‐phase gas/solid/liquid interface near the electrode surface in aqueous solution,which leads to major challenges including the limited mass diffusion of CO_(2) reactant,competitive hydrogen evolution reaction,and poor product *** we critically examine the various methods of surface and interface engineering of the electrocatalysts to optimize the microenvironment for CRR,which can address the above *** effective modification strategies for the gas transport,electrolyte composition,controlling intermediate states,and catalyst engineering are *** key emphasis is made on the diverse atomic‐precision modifications to increase the local CO_(2) concentration,lower the energy barriers for CO_(2) activation,decrease the H2O coverage,and stabilize intermediates to effectively control the catalytic activity and *** perspectives on the challenges and outlook for the future applications of three‐phase interface engineering for CRR and other gasinvolving electrocatalytic reactions conclude the article.

关键词： catalytic selectivity electrochemical CO_(2)reduction intermediates microenvironment three‐phase interface

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Conversion of Catalytically Inert 2D Bismuth Oxide Nanosheets for Effective Electrochemical Hydrogen Evolution Reaction Catalysis via Oxygen Vacancy Concentration Modulation

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Nano-Micro Letters 2022年第6期14卷 48-64页

作者： Ziyang Wu Ting Liao Sen Wang Janith Adikaram Mudiyanselage Aaron SMicallef Wei Li Anthony PO’Mullane Jianping Yang Wei Luo Kostya Ostrikov Yuantong Gu Ziqi Sun School of Mechanical Medical and Process EngineeringQueensland University of Technology2 George StreetBrisbaneQLD 4000Australia Centre for Materials Science Queensland University of Technology2 George StreetBrisbaneQLD 4000Australia School of Earth and Atmospheric Sciences Queensland University of Technology2 George StreetBrisbaneQLD 4000Australia School of Chemistry and Physics Queensland University of Technology2 George StreetBrisbaneQLD 4000Australia Central Analytical Research Facility Queensland University of Technology2 George StreetBrisbaneQLD 4000Australia State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620People’s Republic of China

Oxygen vacancies(Vo)in electrocatalysts are closely correlated with the hydrogen evo-lution reaction(HER)*** role of vacancy defects and the effect of their concentration,how-ever,yet remains ***,Bi2O3,an unfavorable electrocata-lyst for the HER due to a less than ideal hydrogen adsorption Gibbs free energy(ΔGH*),is utilized as a perfect model to explore the func-tion of Vo on HER *** a facile plasma irradia-tion strategy,Bi2O3 nanosheets with different Vo concentrations are fabricated to evaluate the influence of defects on the HER ***,while the generated oxygen vacancies contribute to the enhanced HER performance,higher Vo concentrations beyond a saturation value result in a significant drop in HER *** tunning the Vo concentration in the Bi_(2)O_(3)nanosheets via adjusting the treatment time,the Bi2O3 catalyst with an optimized oxygen vacancy concentration and detectable charge carrier concentration of 1.52×10^(24)cm^(−3)demonstrates enhanced HER performance with an overpotential of 174.2 mV to reach 10 mA cm^(−2),a Tafel slope of 80 mV dec−1,and an exchange current density of 316 mA cm−2 in an alkaline solution,which approaches the top-tier activity among Bi-based HER ***-functional theory calculations confirm the preferred adsorption of H*onto Bi2O3 as a function of oxygen chemical potential(ΔμO)and oxygen partial potential(PO2)and reveal that high Vo concentrations result in excessive stability of adsorbed hydrogen and hence the inferior HER *** study reveals the oxygen vacancy concentration-HER catalytic activity relationship and provides insights into activating catalytically inert materials into highly efficient electrocatalysts.

关键词： Alkaline hydrogen evolution reaction Bismuth oxide Plasma irradiation 2D materials Oxygen vacancy

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