Ordered Porous Nitrogen-Doped Carbon Matrix with Atomically Dispersed Cobalt Sites as an Efficient Catalyst for Dehydrogenation and Transfer Hydrogenation of N-Heterocycles

Yunhu Han, Ziyun Wang, Ruirui Xu, Wei Zhang, Wenxing Chen, Lirong Zheng, Jian Zhang, Jun Luo, Konglin Wu, Youqi Zhu, Chen Chen, Qing Peng, qiang Liu, Peijun Hu, Dingsheng Wang, Yadong Li

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58 Citations (Scopus)

Abstract

Single-atom catalysts (SACs) have been explored widely as potential substitutes for homogeneous catalysts. Isolated cobalt single-atom sites were stabilized on an ordered porous nitrogen-doped carbon matrix (ISAS-Co/OPNC). ISAS-Co/OPNC is a highly efficient catalyst for acceptorless dehydrogenation of N-heterocycles to release H 2 . ISAS-Co/OPNC also exhibits excellent catalytic activity for the reverse transfer hydrogenation (or hydrogenation) of N-heterocycles to store H 2 , using formic acid or external hydrogen as a hydrogen source. The catalytic performance of ISAS-Co/OPNC in both reactions surpasses previously reported homogeneous and heterogeneous precious-metal catalysts. The reaction mechanisms are systematically investigated using first-principles calculations and it is suggested that the Eley–Rideal mechanism is dominant. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
Original languageEnglish
Pages (from-to)11262-11266
JournalAngewandte Chemie International Edition
Volume57
Issue number35
Early online date06 Jul 2018
DOIs
Publication statusPublished - 21 Aug 2018

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