Mononuclear gold species anchored on TS-1 framework as catalyst precursor for selective epoxidation of propylene

被引:21
|
作者
Ayvali, Tugce [1 ]
Ye, Lin [1 ]
Wu, Simson [1 ]
Lo, Benedict T. W. [1 ]
Huang, Chen [2 ]
Yu, Bin [1 ]
Cibin, Giannantonio [3 ]
Kirkland, Angus I. [2 ]
Tang, Chiu [3 ]
Bagabas, Abdulaziz A. [4 ]
Tsang, S. C. Edman [1 ]
机构
[1] Univ Oxford, Dept Chem, Wolfson Catalysis Ctr, Oxford OX1 3QR, England
[2] Univ Oxford, Dept Mat, 16 Parks Rd, Oxford OX1 3PH, England
[3] Diamond Light Source, Harwell Sci & Innovat Campus, Didcot OX11 ODE, Oxon, England
[4] KACST, MSRI, NPTC, POB 6086, Riyadh 11442, Saudi Arabia
基金
英国工程与自然科学研究理事会;
关键词
Catalysis; Gold; Propylene epoxidation; TS-1; Synchrotron XRD; GAS-PHASE EPOXIDATION; PROPENE EPOXIDATION; ACTIVE-SITES; H-2; O-2; PERFORMANCE; ATOMS; TEMPERATURE; STABILITY; SUPPORTS;
D O I
10.1016/j.jcat.2018.09.002
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
Deposition of gold on supports can produce catalytically active forms of gold as well as spectators, but previous understanding of the nature of active immobilized precursors is poor. By using synchrotron X-ray powder diffraction (SXRD) and X-ray absorption spectroscopy (XAS) techniques, we report a novel synthesis and structural elucidation of atomically dispersed gold species anchored to the internal surface of TS-1 as K+Au(OH)(2)Na+(O-f)(3) ("f" signifies the framework atoms of TS-1 in the formula.). It is found that the choice of alkali ions plays a crucial role in nucleation and stabilization of the atomic precursor. These anchored single Au upon controlled reduction in H-2 can form uniform gold clusters in direct contact with the TS-1 surface containing isolated Ti sites: their interface exhibits excellent specificity and stability towards epoxidation of propylene in H-2/O-2 due to synergetic effect. (C) 2018 Elsevier Inc. All rights reserved.
引用
收藏
页码:229 / 233
页数:5
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