Journal
ACS NANO
Volume 16, Issue 10, Pages 16869-16879Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.2c06834
Keywords
surface alloy; hydrogenation; PdBi; X-ray absorption spectroscopy; interdiffusion
Categories
Funding
- National Natural Science Foundation of China [51901147, 21903058, 22173066]
- Natural Science and Engineering Council of Canada (NSERC), Canada Foundation for Innovation (CFI), Canada Research Chair (CRC)
- Ontario Research Foundation (ORF)
- University of Western Ontario
- U.S. DOE [DE-AC02-06CH11357]
- Canadian Light Source
- CFI
- NSERC
- National Research Council (NRC)
- Canadian Institute for Health Research (CIHR)
- University of Saskatchewan
- CLS Graduate Student Travel Support Program
- Suzhou Key Laboratory of Functional Nano & Soft Materials, Collaborative Innovation Center of Suzhou Nano Science Technology
- 111 Project
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By modulating the surface alloy structure of PdBi, the electronic structure of Pd can be continuously adjusted, leading to enhanced catalytic performance in the selective hydrogenation of propyne.
Building a reliable relationship between the electronic structure of alloyed metallic catalysts and catalytic performance is important but remains challenging due to the interference from many entangled factors. Herein, a PdBi surface alloy structural model, by tuning the deposition rate of Bi atoms relative to the atomic interdiffusion rate at the interface, realizes a continuous modulation of the electronic structure of Pd. Using advanced X-ray characterization techniques, we provide a precise depiction of the electronic structure of the PdBi surface alloy. As a result, the PdBi catalysts show enhanced propene selectivity compared with the pure Pd catalyst in the selective hydro-genation of propyne. The prevented formation of saturated beta- hydrides in the subsurface layers and weakened propene adsorption on the surface contribute to the high selectivity. Our work provides in-depth understanding of the electronic properties of surface alloy structure and underlies the study of the electronic structure-performance relationship in bimetallic catalysts.
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