1. Base-free catalytic aerobic oxidation of mercaptans over MOF-derived Co/CN catalyst with controllable composition and structure.
- Author
-
Zhang, Canyang, Gao, Hongyi, Hai, Guangtong, Zeng, Yaojun, Wang, Xingqi, Xing, Liwen, Zhao, Jie, Wang, Ge, and Shu, Xingtian
- Subjects
- *
CATALYSTS , *CATALYTIC oxidation , *POROSITY , *ACTIVATION energy , *DENSITY functional theory , *CATALYTIC activity - Abstract
The synergistic effects between Co NPs and pyridinic nitrogen of Co/CN-x catalysts was the key to realize the base-free oxidation of mercaptans to their corresponding disulfides by decreasing the energy barrier for the deprotonation of mercaptans. [Display omitted] The oxidation of mercaptans under mild and base-free conditions is of vital importance in terms of economy and environment for petroleum processing industry. Here, we developed a series of MOF-derived cobalt-based nitrogen-doped (N -doped) carbon (Co/CN-x) catalysts for the base-free catalytic oxidation of mercaptans. The optimal Co/CN-900 showed excellent catalytic activity for the oxidation of mercaptans under base-free conditions, yielding complete conversion of various mercaptans and > 99.0% selectivity of disulfides. The high performance can be contributed to the advantages of hierarchical pore structure for the diffusion and migration of substrates, self-carrying alkalinity for the formation of mercaptide anion, abundant active Co sites for catalytic oxidation of mercaptans as well as the synergistic effects between the Co nanoparticles (NPs) and N -doped carbon supports. Furthermore, a possible mechanism for base-free catalytic oxidation of mercaptans over Co/CN-x catalysts is proposed based on a set of control experiments and density functional theory (DFT) calculations. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF