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
相关论文
共 50 条
  • [1] Research on Effects of Solvents on Propylene Epoxidation with the TS-1 Catalyst
    Wang, Lina
    PROCEEDINGS OF THE 2017 5TH INTERNATIONAL CONFERENCE ON MACHINERY, MATERIALS AND COMPUTING TECHNOLOGY (ICMMCT 2017), 2017, 126 : 1231 - 1235
  • [2] Propylene oxide inhibits propylene epoxidation over Au/TS-1
    Harris, James W.
    Arvay, Jeremy
    Mitchell, Garrett
    Delgass, W. Nicholas
    Ribeiro, Fabio H.
    JOURNAL OF CATALYSIS, 2018, 365 : 105 - 114
  • [3] Propylene epoxidation over Au/TS-1 modified by ammonium salt: Enhancement of the attractiveness of gold precursors and supports
    Dong, Tao
    Huang, Qian
    Chen, Lu
    Peng, Jiahui
    Hu, Hui
    Huang, Qingming
    Chen, Xiaohui
    CHEMICAL PHYSICS LETTERS, 2022, 804
  • [4] Effect of solvent on the propylene epoxidation over TS-1 catalyst
    Liu, XW
    Wang, XS
    Guo, XW
    Li, G
    CATALYSIS TODAY, 2004, 93-5 : 505 - 509
  • [5] Kinetics of Propylene Epoxidation over Extracrystalline Gold Active Sites on AU/TS-1 Catalysts
    Arvay, Jeremy W.
    Hong, Wei
    Li, Christina
    Delgass, W. Nicholas
    Ribeiro, Fabio H.
    Harris, James W.
    ACS CATALYSIS, 2022, 12 (16) : 10147 - 10160
  • [6] Gold supported on nitrogen-incorporated TS-1 for gas-phase epoxidation of propylene
    Liu Yiwu
    Zhang Xiaoming
    Suo Jishuan
    CHINESE JOURNAL OF CATALYSIS, 2013, 34 (02) : 336 - 340
  • [7] The Influence of Active Biomolecules in Plant Extracts on the Performance of Au/TS-1 Catalysts in Propylene Epoxidation
    Lian, Ting
    Zeng, Wei
    Liu, Hai
    Yu, Jing
    Huang, Jiale
    Wang, Haitao
    Sun, Daohua
    EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2019, 2019 (23) : 2853 - 2859
  • [8] Kinetic insights into reaction pathways of acrolein formation in propylene epoxidation by H 2 and O 2 over Au/TS-1 catalyst
    Du, Wei
    Zhang, Zhihua
    Wang, Jundi
    Song, Nan
    Duan, Xuezhi
    Zhou, Xinggui
    CHEMICAL ENGINEERING JOURNAL, 2024, 487
  • [9] Au/TS-1 catalyst for propylene epoxidation with H2 and O2: Effect of surface property and morphology of TS-1 zeolite
    Xu, Jialun
    Zhang, Zhihua
    Yu, Daiyi
    Du, Wei
    Song, Nan
    Duan, Xuezhi
    Zhou, Xinggui
    NANO RESEARCH, 2023, 16 (05) : 6278 - 6289
  • [10] Gas-phase epoxidation of propylene over small gold ensembles on TS-1
    Taylor, B
    Lauterbach, J
    Delgass, WN
    APPLIED CATALYSIS A-GENERAL, 2005, 291 (1-2) : 188 - 198