Citation: Shunlin Li, Lili Wang, Mengmeng Wu, Yafei Sun, Xiaojuan Zhu, Ying Wan. Measurable surface d charge of Pd as a descriptor for the selective hydrogenation activity of quinoline[J]. Chinese Journal of Catalysis, ;2020, 41(9): 1337-1347. doi: 10.1016/S1872-2067(20)63580-X shu

Measurable surface d charge of Pd as a descriptor for the selective hydrogenation activity of quinoline

The Education Ministry Key Laboratory of Resource Chemistry, Shanghai Key Laboratory of Rare Earth Functional Materials, and Department of Chemistry, Shanghai Normal University, Shanghai 200234, China

Received Date: 15 January 2020
Revised Date: 21 February 2020

Fund Project: This work was supported by the National Natural Science Foundation of China (21773156), the Ministry of Education of China (PCSIRT_IRT_16R49), the International Joint Laboratory on Resource Chemistry of China (IJLRC), the Shanghai Sci. & Tech. and Edu. Committee (17JC1404200, 19070502700), and the Shanghai Gaofeng & Gaoyuan Project for University Academic Program Development.

AuPd nanoalloys with tunable Pd concentrations have been synthesized and used as model catalysts. They have been directly imaged by high-angle annular dark-field scanning transmission electron microscopy and investigated by thorough analyses of their extended X-ray absorption fine structure, X-ray absorption near-edge structure, X-ray diffraction and X-ray photoelectron spectroscopy measurements. The bimetallic nanoparticles are embedded in a carbonaceous matrix and have almost an identical structure at the atomic level and the same electronic properties as AuPd bulk alloys with the same compositions. The d-electron increase at surface Pd sites is determined by the Pd concentration of the alloy. Similarly, their activation entropy and catalytic activity for the hydrogenation of quinoline is related to the Pd concentration, with Au₅₀Pd₅₀ the most active of the alloys investigated. An almost 11 times higher activity was achieved compared to a pure Pd catalyst. The experimentally measurable surface d charge at the Pd sites in the AuPd was found to linearly correlate with the activation entropy and catalytic activity for the hydrogenation of quinoline. The alloy structure is stable, showing negligible metal segregation, dissolution-redeposition and aggregation during the hydrogenation process which involves strong adsorption.
- Surface d charge,
- AuPd alloy,
- Activation entropy,
- Quinoline,
- Hydrogenation
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