Electronic Modification by Transitional Metal Dopants to Tune the Oxidation Activity of Pt-CeO2-Based Catalysts

Jianghao Zhang; Ruoting Shan; Hongfei Xiao

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Electronic Modification by Transitional Metal Dopants to Tune the Oxidation Activity of Pt-CeO2-Based Catalysts

机译：Electronic Modification by Transitional Metal Dopants to Tune the Oxidation Activity of Pt-CeO2-Based Catalysts

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While utilization of transitional metals as a promoter has been extensively studied to enhance the activity of Pt-based catalysts for the oxidation of formaldehyde(HCHO),there is still a lack of well elucidated property-function relationship for the rational selection of a promoter in catalyst design.Herein,we modified a Pt/CeO2 catalyst with two transitional metal dopants(i.e.,Mn and Cu)that showed negligible influence on the physical structure of the Pt-CeO2 matrix but distinct effects on the activity of the catalyst.Complementary characterizations combined with density functional theory modeling revealed that the transitional metal dopants significantly modified the electronic structure of the catalyst and shifted the d-band of Pt to higher energy with different extents,which may tune the bonding strength of HCHO/intermediates with the Pt-CeO2 interface domain.The catalyst with moderate bonding strength(i.e.,Pt-Mn/CeO2)displayed the highest reactivity under the ambient condition,while Pt-Cu/CeO2 with the highest bonding strength showed a dramatically decreased activity.No correlation was observed between the abundancy of the active oxygen and catalytic activity,likely due to the oxygen supply having a much higher rate than the rate-determining step.This work contributes to the elucidation about the property-function relationship of a transitional metal dopant in Pt-based catalysts for the oxidation of HCHO.

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《Environmental Science & Technology: ES&T》 |2022年第23期|17331-17340|共10页
作者
Jianghao Zhang; Ruoting Shan; Hongfei Xiao;
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作者单位

State Key Joint Laboratory of Environment Simulation and Pollution Control,Research Center for Eco-environmental Sciences,Chinese Academy of Sciences,Beijing 100085,China;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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正文语种英语
中图分类环境科学、安全科学;
关键词
Pt-CeO2; based catalysts; electronic modification; HCHO abatement; bonding strength to HCHO; catalytic oxidation; mechanistic study;

Electronic Modification by Transitional Metal Dopants to Tune the Oxidation Activity of Pt-CeO2-Based Catalysts

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