Ptnc-FeOx界面作用提升Pt团簇催化CO氧化性能

TL9%TQ426.8%O357.4; 金属-氧化物界面作用对于调节金属催化剂的电子结构、提升催化剂的催化活性和稳定性起到重要影响,在纳米催化研究领域受到广泛关注.利用尿素沉积沉淀法合成了与FeOx形成界面作用的负载型Pt团簇(Ptnc,尺寸为(1.4±0.2)nm),它表现出相对单金属Ptnc催化剂显著提升的CO催化氧化活性.与具有类似Pt负载量的Pt/SiO2相比,Ptnc-FeOx/SiO2催化剂在同等条件下催化CO氧化的完全转化温度从180°C大幅降低至90°C,表观活化能从60 kJ·mol?1降低到19 kJ·mol?1,并具有高出20倍的转换频率(Turnover Frequen...

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Published in核技术 Vol. 44; no. 1; pp. 25 - 34
Main Authors 刘成勇, 黄莉, 宋雪洋, 贺文雪, 王思宇, 龙志鑫, 孙治湖, 韦世强
Format Journal Article
LanguageChinese
Published 中国科学技术大学国家同步辐射实验室 合肥 230029 15.01.2021
Subjects
金属-氧化物界面
漫反射傅里叶变换红外光谱
Ptnc-FeOx催化剂
同步辐射X射线吸收精细结构
CO催化氧化
Online AccessGet full text
ISSN0253-3219
DOI10.11889/j.0253-3219.2021.hjs.44.010103

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Abstract TL9%TQ426.8%O357.4; 金属-氧化物界面作用对于调节金属催化剂的电子结构、提升催化剂的催化活性和稳定性起到重要影响,在纳米催化研究领域受到广泛关注.利用尿素沉积沉淀法合成了与FeOx形成界面作用的负载型Pt团簇(Ptnc,尺寸为(1.4±0.2)nm),它表现出相对单金属Ptnc催化剂显著提升的CO催化氧化活性.与具有类似Pt负载量的Pt/SiO2相比,Ptnc-FeOx/SiO2催化剂在同等条件下催化CO氧化的完全转化温度从180°C大幅降低至90°C,表观活化能从60 kJ·mol?1降低到19 kJ·mol?1,并具有高出20倍的转换频率(Turnover Frequency,TOF).采用同步辐射X射线吸收谱学技术、原位漫反射傅里叶变换红外光谱、球差电镜等多种表征手段,对Ptnc-FeOx之间的界面相互作用进行了探讨.结果表明:Ptnc与FeOx之间通过形成的Pt-Fe金属键发生了从Fe向Pt的电荷转移,从而降低了Ptnc的d带中心位置,减弱了CO在Ptnc表面的吸附强度,有助于实现催化活性和反应动力学速率的提升.
AbstractList TL9%TQ426.8%O357.4; 金属-氧化物界面作用对于调节金属催化剂的电子结构、提升催化剂的催化活性和稳定性起到重要影响,在纳米催化研究领域受到广泛关注.利用尿素沉积沉淀法合成了与FeOx形成界面作用的负载型Pt团簇(Ptnc,尺寸为(1.4±0.2)nm),它表现出相对单金属Ptnc催化剂显著提升的CO催化氧化活性.与具有类似Pt负载量的Pt/SiO2相比,Ptnc-FeOx/SiO2催化剂在同等条件下催化CO氧化的完全转化温度从180°C大幅降低至90°C,表观活化能从60 kJ·mol?1降低到19 kJ·mol?1,并具有高出20倍的转换频率(Turnover Frequency,TOF).采用同步辐射X射线吸收谱学技术、原位漫反射傅里叶变换红外光谱、球差电镜等多种表征手段,对Ptnc-FeOx之间的界面相互作用进行了探讨.结果表明:Ptnc与FeOx之间通过形成的Pt-Fe金属键发生了从Fe向Pt的电荷转移,从而降低了Ptnc的d带中心位置,减弱了CO在Ptnc表面的吸附强度,有助于实现催化活性和反应动力学速率的提升.
Author 孙治湖
贺文雪
黄莉
宋雪洋
王思宇
龙志鑫
韦世强
刘成勇
AuthorAffiliation 中国科学技术大学国家同步辐射实验室 合肥 230029
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WEI Shiqiang
LONG Zhixin
WANG Siyu
HE Wenxue
LIU Chengyong
HUANG Li
SUN Zhihu
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DocumentTitle_FL Role of Ptnc-FeOx metal-oxide interface in enhancing the catalytic activity for CO oxidation
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Keywords 金属-氧化物界面
漫反射傅里叶变换红外光谱
Ptnc-FeOx催化剂
同步辐射X射线吸收精细结构
CO催化氧化
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Title Ptnc-FeOx界面作用提升Pt团簇催化CO氧化性能
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