Chinese Journal of Catalysis ›› 2016, Vol. 37 ›› Issue (9): 1569-1578.DOI: 10.1016/S1872-2067(16)62504-4

• Articles • Previous Articles    

Chemoselective transfer hydrogenation to nitroarenes mediated by oxygen-implanted MoS2

Chaofeng Zhang, Xu Wang, Mingrun Li, Zhixin Zhang, Yehong Wang, Rui Si, Feng Wang   

  1. a. State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
    b. University of Chinese Academy of Sciences, Beijing 100049, China;
    c. Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China
  • Received:2016-06-03 Revised:2016-07-11 Online:2016-09-21 Published:2016-09-21
  • Contact: Feng Wang
  • Supported by:

    This work was supported by the National Natural Science Foundation of China(21422308, 21403216, 21273231) and Dalian Excellent Youth Foundation(2014J11JH126).

Abstract:

We present an efficient approach for the chemoselective synthesis of arylamines from nitroarenes and formate over an oxygen-implanted MoS2 catalyst(O-MoS2). O-MoS2 was prepared by incomplete sulfiidation and reduction of an ammonium molybdate precursor. A number of Mo-O bonds were implanted in the as-synthesized ultrathin O-MoS2 nanosheets. As a consequence of the different coordination geometries of O(MoO2) and S(MoS2), and lengths of the Mo-O and Mo-S bonds, the implanted Mo-O bonds induced obvious defects and more coordinatively unsaturated(CUS) Mo sites in O-MoS2, as confirmed by X-ray diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy, high resolution transmission electron microscopy, and extended X-ray absorption fine structure characterization of various MoS2-based materials. O-MoS2 with abundant CUS Mo sites was found to efficiently catalyze the chemoselective reduction of nitroarenes to arylamines.

Key words: MoS2, Coordinative unsaturated Mo, Nitroarene, Transfer hydrogenation, Formate, Heterogeneous catalysis