Sublimation-Induced Sulfur Vacancies in MoS2 Catalyst for One-Pot Synthesis of Secondary Amines

被引:56
|
作者
Zhang, Yunrui [1 ]
Gao, Yongjun [1 ]
Yao, Siyu [2 ,3 ,4 ]
Li, Siwei [2 ,3 ,4 ]
Asakura, Hiroyuki [5 ,6 ]
Teramura, Kentaro [5 ,6 ]
Wang, Haijun [1 ]
Ma, Ding [2 ,3 ,4 ]
机构
[1] Hebei Univ, Coll Chem & Environm Sci, Key Lab Analyt Sci & Technol Hebei Prov, Baoding 071002, Peoples R China
[2] Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
[3] Peking Univ, Coll Engn, Beijing 100871, Peoples R China
[4] Peking Univ, BIC ESAT, Beijing 100871, Peoples R China
[5] Kyoto Univ, Grad Sch Engn, Dept Mol Engn, Nishikyo Ku, Kyoto 6158510, Japan
[6] Kyoto Univ, Elements Strategy Initiat Catalysts & Batteries, Nishikyo Ku, 1-30 Goryo Ohara, Kyoto 6158245, Japan
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
reductive amination; sulfur vacancies; one-pot strategy; cascade reaction; molybdenum sulfide; TRANSFER HYDROGENATION; REDUCTIVE AMINATION; CARBONYL-COMPOUNDS; NITRO-COMPOUNDS; ACTIVE-SITES; NITROARENES; SURFACE;
D O I
10.1021/acscatal.9b01429
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
MoS2 catalysts with abundant S and Mo defects have been developed for the one-pot reductive amination of nitro compounds with aldehydes to synthesize secondary amines. The combination of multiple structural characterizations demonstrates that the density of S vacancies can be tuned by changing the thermal sublimation temperature. The experimental results and DFT calculations demonstrate that S vacancies on the surface of MoS2 are the active sites for the hydrogenation of the intermediate imines to the final products secondary amines.
引用
收藏
页码:7967 / 7975
页数:17
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