Ligand Stabilized Ni1 Catalyst for Efficient CO Oxidation

Supported single transition metal (TM1) catalysts have attracted broad attention in academia recently. Still, their corresponding reactivity and stability under reaction conditions are critical but have not well explored at the fundamental level. Herein, we use density functional theory calculation...

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Published in:Chemphyschem Vol. 21; no. 21; pp. 2417 - 2425
Main Authors: Jian, Minzhen, Zhao, Chuanlin, Li, Wei‐Xue
Format: Journal Article
Language:English
Published: Weinheim Wiley Subscription Services, Inc 03-11-2020
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Summary:Supported single transition metal (TM1) catalysts have attracted broad attention in academia recently. Still, their corresponding reactivity and stability under reaction conditions are critical but have not well explored at the fundamental level. Herein, we use density functional theory calculation and ab initio molecular dynamics simulation to investigate the role of reactants and ligands on the reactivity and stability of graphitic carbon nitride (g‐C3N4) supported Ni1 for CO oxidation. We find out that supported bare Ni1 atoms are only metastable on the surface and tend to diffuse into the interlayer of g‐C3N4. Though Ni1 is catalytically active at moderate temperatures, CO adsorption induced dimerization deactivates the catalyst. Hydroxyl groups not only are able to stabilize the supported Ni1 atom, but also increase the reactivity by participating directly in the reaction. Our results provide valuable insights on improving the chemical stability of TM1 by ligands without sacrificing the reactivity, which are helpful for the rational design of highly loaded atomically dispersed supported metal catalysts. Helpful ligands: Supported bare Ni1 atoms are metastable on the surface, poisoned by CO at low temperature, aggregated by adsorbed CO at moderate temperature, and catalyze the CO oxidation at high temperature. Hydroxyl groups are promising ligands to stabilize the Ni1 atom and at same time increase the reactivity by participating directly in the reaction. The distinct role of reactants and ligands on reactivity and stability provide valuable insights for the rational design of single atoms catalysts.
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ISSN:1439-4235
1439-7641
DOI:10.1002/cphc.202000730