Ultrasmall gold nanoparticles confined in zeolite Y: Preparation and activity in CO oxidation

被引:43
作者
Chen, Yi-Hsiu [1 ]
Mou, Chung-Yuan [2 ]
Wan, Ben-Zu [1 ]
机构
[1] Natl Taiwan Univ, Dept Chem Engn, Taipei 106, Taiwan
[2] Natl Taiwan Univ, Dept Chem, Taipei 106, Taiwan
关键词
Proton-type zeolite Y (HY); Surface charge; Surface modification; Gold catalyst; CO oxidation; SUPPORTED AU CATALYSTS; SELECTIVE OXIDATION; MESOPOROUS SILICA; OXIDE SUPPORTS; NANOCLUSTERS; CLUSTERS; STABILITY; AL-SBA-15; CHLORIDE; SIO2;
D O I
10.1016/j.apcatb.2017.06.083
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In this study, proton-type zeolites Y (HY) with Al/Si ratio of 0.36 were used as a support for deposition of HAuCl4 (in pH 6 solution) to prepare Au/Y catalysts for CO oxidation at 25 degrees C. The low isoelectric point of HY (similar to pH = 2) made this support inappropriate for loading negatively charged gold complexes, and caused the generation of large gold particles with low catalytic activity. We found that through a Na+ pretreatment of HY to form H(Na)Y, the surface charge can be reversed to positive, thus favoring the deposition. The resulting Au/H(Na)Y, without any high temperature treatment, gave excellent activity in CO oxidation comparable to Au/TiO2. The CO oxidation rate of 0.21 mol CO/mol Au.s remained stable at 25 degrees C. HRTEM images of the catalyst show highly dispersed gold nanoparticles similar to 1 nm confined in the nanocage of H(Na)Y. XPS spectra show high proportion of Au(III) associated with Au-O. The weak Au-O in Au/H(Na)Y is found responsible for the easy reduction in TPR. For comparison, the other alternative procedures of gold deposition were also tried to reverse the surface charge of HY by decreasing the pH of solution. However, high contents of residual Cl in the nano-gold catalyst lead to almost no activity in CO oxidation. (C) 2017 Elsevier B.V. All rights reserved.
引用
收藏
页码:506 / 514
页数:9
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