Ordered Porous Nitrogen-Doped Carbon Matrix with Atomically Dispersed Cobalt Sites as an Efficient Catalyst for Dehydrogenation and Transfer Hydrogenation of N-Heterocycles
作者: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、P. Hu、Dingsheng Wang、Yadong Li
DOI:10.1002/anie.201805467
日期:2018.8.27
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 H2. ISAS‐Co/OPNC also exhibits excellent catalytic activity for the reverse
单原子催化剂(SAC)已被广泛研究作为均相催化剂的潜在替代品。孤立的钴单原子位点稳定在有序的多孔氮掺杂碳基质(ISAS-Co / OPNC)上。ISAS-Co / OPNC是用于N杂环的无受体脱氢以释放H 2的高效催化剂。ISAS-Co / OPNC还具有出色的催化活性,可用于N杂环的反向转移加氢(或加氢)以存储H 2,使用甲酸或外部氢作为氢源。ISAS-Co / OPNC在这两个反应中的催化性能均超过了先前报道的均相和非均相贵金属催化剂。使用第一性原理系统地研究了反应机理,并提出以Eley-Rideal机理为主导。