期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 15, 期 8, 页码 2809-2820出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c2cp42907a
关键词
-
资金
- Ministry of Education, Culture, Sports, Science and Technology, Japan (MEXT)
- MEXT
- JSPS
- Grants-in-Aid for Scientific Research [22550001] Funding Source: KAKEN
The catalytic activity for the oxygen reduction reaction (ORR) of both the pristine and defect-possessing hexagonal boron nitride (h-BN) monolayer and H-terminated nanoribbon have been studied theoretically using density functional theory. It is demonstrated that an inert h-BN monolayer can be functionalized and become catalytically active by nitrogen doping. It is shown that the energetics of adsorption of O-2, O, OH, OOH, and H2O on N atom impurities in the h-BN monolayer (N-B@h-BN) is quite similar to that known for a Pt(111) surface. The specific mechanism of destructive and cooperative adsorption of ORR intermediates on the surface point defects is discussed. It is demonstrated that accounting for entropy and zero-point energy (ZPE) corrections results in destabilization of the ORR intermediates adsorbed on N-B@h-BN, while solvent effects lead to their stabilization. Therefore, entropy, ZPE and solvent effects partly cancel each other and have to be taken into account simultaneously. Analysis of the free energy changes along the ORR pathway allows us to suggest that a N-doped h-BN monolayer can demonstrate catalytic properties for the ORR under the condition that electron transport to the catalytically active center is provided.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据