期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 114, 期 23, 页码 5930-5934出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1701280114
关键词
confined catalysis; two-dimensional materials; density functional theory; oxygen reduction reaction; graphene
资金
- National Natural Science Foundation of China [21373208, 91545204, 21688102, 21621063]
- Ministry of Science and Technology of China [2016YFA0200200, 2013CB834603, 2013CB933100]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17020200]
Confined microenvironments formed in heterogeneous catalysts have recently been recognized as equally important as catalytically active sites. Understanding the fundamentals of confined catalysis has become an important topic in heterogeneous catalysis. Well-defined 2D space between a catalyst surface and a 2D material overlayer provides an ideal microenvironment to explore the confined catalysis experimentally and theoretically. Using density functional theory calculations, we reveal that adsorption of atoms and molecules on a Pt(111) surface always has been weakened under monolayer graphene, which is attributed to the geometric constraint and confinement field in the 2D space between the graphene overlayer and the Pt(111) surface. A similar result has been found on Pt(110) and Pt(100) surfaces covered with graphene. The microenvironment created by coating a catalyst surface with 2D material overlayer can be used to modulate surface reactivity, which has been illustrated by optimizing oxygen reduction reaction activity on Pt(111) covered by various 2D materials. We demonstrate a concept of confined catalysis under 2D cover based on a weak van der Waals interaction between 2D material overlayers and underlying catalyst surfaces.
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