Pt-表层限域的表面FeOx结构用于低温CO氧化反应

doi:10.1016/S1872-2067(12)60673-1

催化学报 ›› 2013, Vol. 34 ›› Issue (11): 2029-2035.DOI: 10.1016/S1872-2067(12)60673-1

Pt-表层限域的表面FeO_x结构用于低温CO氧化反应

徐红, 傅强, 包信和

中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连116023

收稿日期:2013-06-06 修回日期:2013-07-24 出版日期:2013-10-18 发布日期:2013-10-18
通讯作者: Qiang Fu
基金资助:
国家自然科学基金(21222305,11079005,20923001);国家重点基础研究发展计划(973计划,2013CB834603,2011CBA00503,2013CB933100).

Nanosized FeO_x overlayers on Pt-skin surfaces for low temperature CO oxidation

Hong Xu, Qiang Fu, Xinhe Bao

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2013-06-06 Revised:2013-07-24 Online:2013-10-18 Published:2013-10-18
Contact: Qiang Fu
Supported by:
This work was supported by the National Natural Science Foundation of China (21222305, 11079005, 20923001) and the National Basic Research Program of China (973 Program, 2013CB834603, 2011CBA00503, 2013CB933100).

摘要/Abstract

摘要：

通过简单的浸渍-还原并随后在酸性溶液中处理制备了Pt-Cu双金属催化剂. 利用电感耦合等离子体发射光谱、X射线衍射和X射线光电子能谱对不同处理条件下的Pt-Cu纳米粒子的结构和组成进行了表征. 研究发现, Pt-Cu催化剂在高温H₂中还原形成了PtCu₃合金结构, 酸洗处理后形成了包含Pt-骨架(Pt-skeleton)的表面结构和PtCu₃合金核的纳米粒子. 而Pt-骨架结构又可通过在H₂中退火转变为规整的Pt-表层(Pt-skin)结构. Pt-表层表面修饰Fe氧化物后在CO选择氧化反应中表现出较好的催化性能. 通过此方法制备的三金属Pt-Cu-Fe催化剂可达到与Pt-Fe相近的高活性, 并且催化剂中Pt的用量大大降低.

关键词: 一氧化碳氧化, 铂-表层, 铁氧化物, 界面催化

Abstract:

Pt-Cu/carbon black catalysts were prepared by an impregnation-reduction method followed by acid leaching. The structure and composition of Pt-Cu nanoparticles treated under different conditions were investigated by inductively coupled plasma atomic emission spectrometry, X-ray diffraction, and X-ray photoelectron spectroscopy. PtCu₃ alloy formed upon annealing Pt-Cu/carbon black catalysts in H₂. Acid leaching produced Pt-Cu nanoparticles consisting of Pt-skeleton surface structure and PtCu₃ alloy core. The Pt-skeleton could be transformed to well-defined Pt-skin structure through further annealing the leached Pt-Cu nanoparticles in H₂. Decorating the Pt-skin surfaces with Fe oxide nanopatches resulted in enhanced reactivity in the preferential oxidation of CO in excess H₂. The tri-component Pt-Cu-Fe catalysts exhibited comparable activity to the bi-component Pt-Fe catalysts but used much less Pt.

Key words: CO oxidation, Pt-skin, Fe oxide, Interface catalysis

徐红, 傅强, 包信和. Pt-表层限域的表面FeO_x结构用于低温CO氧化反应[J]. 催化学报, 2013, 34(11): 2029-2035.

Hong Xu, Qiang Fu, Xinhe Bao. Nanosized FeO_x overlayers on Pt-skin surfaces for low temperature CO oxidation[J]. Chinese Journal of Catalysis, 2013, 34(11): 2029-2035.

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Pt-表层限域的表面FeO_x结构用于低温CO氧化反应

Nanosized FeO_x overlayers on Pt-skin surfaces for low temperature CO oxidation

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Pt-表层限域的表面FeOx结构用于低温CO氧化反应

Nanosized FeOx overlayers on Pt-skin surfaces for low temperature CO oxidation

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Pt-表层限域的表面FeO_x结构用于低温CO氧化反应

Nanosized FeO_x overlayers on Pt-skin surfaces for low temperature CO oxidation