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作 者:常淑玲 孙婷婷 贾镕婧 张立红[1] 徐彦红 CHANG Shuling;SUN Tingting;JIA Rongjing;ZHANG Lihong;XU Yanhong(School of Chemical Engineering and Technology,Tianjin University,Tianjin 300350,China;School of Chemical and Environmental Engineering,Pingdingshan University,Pingdingshan 467000,China)
机构地区:[1]天津大学化工学院,天津300350 [2]平顶山学院化学与环境工程学院,河南平顶山467000
出 处:《燃料化学学报(中英文)》2025年第4期452-461,共10页Journal of Fuel Chemistry and Technology
摘 要:利用电化学方法将惰性CO_(2)选择性和高效地转化为增值化学品是缓解环境和能源危机的重要途径之一。非贵金属Zn因储量丰富、价格低廉且稳定无毒常用于电催化CO_(2)还原(CO_(2)RR)制CO过程。本研究采用水热法制备了ZnOHF粉体并通过热处理对其进行活化。分别采用XRD、SEM、EDS和XPS表征方法对热处理前后ZnOHF的结构、形貌和元素分布进行研究。相比未经过热处理的ZnOHF样品,热处理后的ZnOHF样品在电催化还原CO_(2)合成CO的反应中表现出更高的CO_(2)还原活性和对CO的选择性,其CO的法拉第效率(FE)达到77.4%,这是由于热处理可使ZnOHF表面获得适宜数量的羟基,减小颗粒粒度,增加粗糙度和电化学比表面积(ECSA),从而暴露更多的活性位点,促进CO_(2)在表面的吸附活化以及CO脱附。The selective and efficient conversion of inert CO_(2)into value-added chemicals by electrochemical methods is one of the important ways to alleviate the environmental and energy crisis.Non-precious metal Zn is often used in the electrocatalytic reduction reaction of CO_(2)(CO_(2)RR)to CO due to its abundant reserves,low price,good stability and non-toxic.However,it is still necessary to improve the catalytic performance of traditional Zn-based catalysts for CO_(2)RR.In order to optimize the performance of Zn-based catalysts,pure ZnOHF sample was synthesized by hydrothermal method.The effect of heat treatment on the structure,texture and electrocatalytic CO_(2)RR performance of the samples was investigated.The electrocatalytic evaluation results revealed that the heat-treated ZnOHF sample showed better activity and CO selectivity compared with untreated sample.The Faraday efficiency of CO(FECO)reached 77.4%at-1.15V vs.RHE.Even at potential of-1.05 V vs.RHE,the current density and FECO could be stabilized at-6.17 mA/cm^(2)and 72%in 5 h.This was because heat treatment optimized the amount of surface hydroxyl of ZnOHF.The microcrystalline particles became uniform and fine.The roughness and electrochemical surface area(ECSA)also increased,thus exposing more active sites and promoting the adsorption and activation of CO_(2)as well as the desorption of CO.This study provides experimental basis and theoretical guidance for the design and development of Zn-based catalysts for electrocatalytic CO_(2)RR.
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