Biomass-assisted approach for large-scale construction of multi-functional isolated single-atom site catalysts
Tao Wu, Sha Li, Shoujie Liu, Weng‐Chon Cheong, Cheng Peng, Kai Yao, Yingping Li, Jieyue Wang, Binbin Jiang, Zheng Chen, Zhiming Chen, Xianwen Wei, Konglin Wu
Abstract
In recent years, the isolated single-atom site (ISAS) catalysts have attracted much attention as they are cost-effective, can achieve 100% atom-utilization efficiency, and often display superior catalytic performance. Here, we developed a biomass-assisted pyrolysis-etching-activation (PEA) strategy to construct ISAS metal decorated on N and B co-doped porous carbon (ISAS M/NBPC, M = Co, Fe, or Ni) catalysts. This PEA strategy can be applied in the universal and large-scale preparation of ISAS catalysts. Interestingly, the ISAS M/NBPC (M = Co, Fe, or Ni) catalysts show multi-functional features and excellent catalytic activities. They can be used to conduct different types of catalytic reactions, such as O-silylation (OSI), oxidative dehydrogenation (ODH), and transfer hydrogenation (THG). In addition, we used the transfer hydrogenation of nitrobenzene as a typical reaction and revealed the difference between ISAS Co/NBPC and ISAS Co/NPC (N-doped porous carbon) catalysts by density functional theory (DFT) calculations, and which showed that the decreased barrier of the ratedetermining step and the low-lying potential energy diagram indicate that the catalytic activity is higher when ISAS Co/NBPC is used than that when ISAS Co/NPC is used. These results demonstrate that the catalytic performance can be effectively improved by adjusting the coordination environment around the ISAS.