催化作用
活动站点
材料科学
分子
电子转移
小分子
组合化学
化学物理
机制(生物学)
纳米技术
光化学
化学
有机化学
物理
生物化学
量子力学
作者
Jieyuan Li,Shi Yin,Fan Dong,Wanglai Cen,Ying‐Hao Chu
标识
DOI:10.1021/acsami.7b04026
摘要
Because of the limited characterization methods of the structures and morphology of N-doped carbocatalysts that are available at the atomic level, the detailed promotion mechanism of the catalytic efficiency is unspecific and the particular active sites introduced by the N atoms require further evaluation. Herein, this challenging issue is tackled by extensive theoretical simulation. It is first proposed that the active sites, wherein O2 molecules become adsorbed and activated, be tailored by synergistic graphitic and pyridinic N atoms (GrN and PyN, respectively), which remarkably accelerate the generation of highly chemically reactive O-containing species. The boosted catalytic efficiency is essentially contributed by the electron donor and acceptor of the two active sites, which are induced by PyN and GrN, respectively. These active sites steer the electron transfer between O2 molecules, and the reaction centers in a one-way transmission manner along the PyN → O1 → O2 → C → GrN path. This work provides a feasible protocol for the modification of generally practical carbocatalysts and sheds new light on the understanding of the catalysis mechanism.
科研通智能强力驱动
Strongly Powered by AbleSci AI