Abstract
Abstract
Graphene and many 2D carbon allotropes are good support materials for single-atom catalysts (SACs) and have been successfully applied to many catalytic reactions. Herein, based on the egg tray graphene (ETG), a carbon allotrope constructed in our previous report, we designed ETG and three N-doped ETG supported Pd SACs, Pd@ETG-N
x
(x= 0–3), for dehydrogenation of formic acid (HCOOH) by density functional theory. Our calculations show that ETG is easier for N doping than graphene, and Pd single atom can be stably adsorbed on the ETG with different N doping concentrations. Major pathways of formic acid dehydrogenation and dehydration were identified. We found that HCOOH dehydrogenation proceeds along the COOH-mediated pathway on each catalyst. With the increased N content in the substrate, the activity and H2 selectivity of Pd SACs are greatly improved. Especially, among these four SACs, Pd@ETG-N3 shows the best catalytic performance, which is even better than Pd(111). Furthermore, electronic analysis was made to reveal the metal-support interactions and the origin of the activity trend of Pd@ETG-N
x
. Our study reveals the unique potential of carbon allotropes in catalyst design, and provides theoretical insights for rational design of efficient catalysts by adjusting the support and the coordination environment.
Funder
Research and Development Program of China
National Natural Science Foundation of China
Subject
Mechanical Engineering,Mechanics of Materials,Condensed Matter Physics,General Materials Science,General Chemistry
Cited by
1 articles.
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