A systematic theoretical study of hydrogen activation, spillover and desorption in single-atom alloys
| Autor: | Guo-Chen Zhao, Chun-Guang Liu, Yong-Qing Qiu |
|---|---|
| Rok vydání: | 2021 |
| Předmět: |
Hydrogen
010405 organic chemistry Chemistry Process Chemistry and Technology chemistry.chemical_element Electronic structure 010402 general chemistry 01 natural sciences Catalysis Dissociation (chemistry) 0104 chemical sciences Metal Spillover effect Chemical physics visual_art Desorption visual_art.visual_art_medium Density functional theory |
| Zdroj: | Applied Catalysis A: General. 610:117948 |
| ISSN: | 0926-860X |
| Popis: | Towards the computational design of single-atom alloys (SAAs) catalysts, we systematically studied the hydrogen activation, spillover and desorption by density functional theory (DFT) and first-principles calculations. Herein, we designed a model with 27 individual isolated metals in Cu(111) slab and described the scaling relationships and meticulous electronic structures. The results show that CuPd, CuMn, CuPt SAAs possess appropriate H atom binding ability and lower H2 dissociation barrier superior to pure metal Cu. There have been many reports about the design of hydrogenation catalysts before, but most of them are about CuPd and CuPt SAAs. Here we found that CuMn SAAs exhibits excellent catalytic performance, even comparable to CuPd and CuPt SAAs. Based on exhaustive electronic structure analysis, we discovered a rare electronic structure on CuMn SAAs, where Mn has no obvious electronic interaction with the host metal Cu, even like a free atom. The incredible phenomenon promotes CuMn SAAs to possess extraordinary hydrogenation catalytic activity. This paper seeks to provide deep insights into chemistry, catalysis, and interfaces for people to design new catalysts. |
| Databáze: | OpenAIRE |
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