期刊
ACS CATALYSIS
卷 8, 期 9, 页码 7799-7808出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b01324
关键词
propene epoxidation; Au-Ag bimetallic catalysts; TS-1-B; DFT; synergy
资金
- National Science Foundation of China [21606254]
- Key Research and Development Plan of Shandong Province [2017GSF17126]
- Natural Science Foundation of Shandong Province [ZR2016BB16]
- Independent Innovation Foundation of Qingdao [17-1-1-18-jch]
- Fundamental Research Funds for the Central Universities [18CX02014A]
Gradually emerging environmental concerns have triggered the development of highly efficient catalysts for propene epoxidation with H-2 and O-2. Unfortunately, intensifying the activity and stability is still a challenging task. Herein, Au-Ag bimetallic catalysts were deposited on titanium silicate-1 with blocked pores (TS-1-B). Via density functional theory calculations together with multiple types of characterization (e.g., high-angle annular dark-field scanning transmission electron microscopy, ultraviolet-visible, and X-ray photoelectron spectrometry), we found that the synergy between Au and Ag significantly improved the catalytic performance via not only the decrease in the Au nanoparticle size but also the enhanced oxygen adsorption and electron transfer ability from Au to O-2. Furthermore, a volcano-shaped relationship between the Au/Ag ratio and catalytic performance was also established, and the Au-10-Ag-1/TS-1-B catalyst showed an excellent stable PO formation rate (174-233 g(PO) h(-1) g(Au)(-1)) and a H-2 efficiency of 44%, higher than those of the reported stable catalysts. The insights and methodology reported here may pave the way for maximizing Au utilization efficiency and unraveling the intrinsic structure-performance relationship of bimetallic catalysts for propene epoxidation.
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