Chongqing Key Laboratory of Catalysis and New Environmental Materials, College of Environment and Resources, Chongqing Technology and Business University , Chongqing 400067, P. R. China.
ACS Appl Mater Interfaces. 2017 Jun 14;9(23):19861-19869. doi: 10.1021/acsami.7b04026. Epub 2017 May 31.
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 O 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 O molecules, and the reaction centers in a one-way transmission manner along the PyN → O → O → 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.
由于目前在原子水平上可用的掺杂氮的碳催化剂的结构和形态的有限描述方法，催化效率的详细促进机制不明确，并且氮原子引入的特殊活性位需要进一步评估。在此，通过广泛的理论模拟来解决这个具有挑战性的问题。本文首先提出通过协同的石墨和吡啶氮原子（GrN 和 PyN）来调整活性位，从而吸附和激活 O 分子，这显著加速了高化学活性含氧物种的生成。两种活性位的电子供体和受体分别诱导产生的增强的催化效率，其中 PyN 和 GrN 分别作为电子供体和受体。这些活性位引导 O 分子之间的电子转移，并且反应中心沿着 PyN→O→O→C→GrN 路径以单向传输的方式进行。这项工作为一般实用的碳催化剂的改性提供了可行的方案，并为理解催化机制提供了新的思路。
