A facile sulfur-assisted method to synthesize porous alveolate Fe/g-C3N4 catalysts with ultra-small cluster and atomically dispersed Fe sites

doi:10.1016/S1872-2067(20)63529-X

Chinese Journal of Catalysis ›› 2020, Vol. 41 ›› Issue (8): 1198-1207.DOI: 10.1016/S1872-2067(20)63529-X

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A facile sulfur-assisted method to synthesize porous alveolate Fe/g-C₃N₄ catalysts with ultra-small cluster and atomically dispersed Fe sites

Sufeng An^a, Guanghui Zhang^a, Jiaqiang Liu^a, Keyan Li^a, Gang Wan^b, Yan Liang^a, Donghui Ji^a, Jeffrey T. Miller^c, Chunshan Song^d, Wei Liu^e, Zhongmin Liu^e, Xinwen Guo^a

a State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China;
b Stanford Synchrotron Radiation Light Source, SLAC National Accelerator Laboratory and Stanford University, Menlo Park, CA 94025, USA;
c Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, USA;
d EMS Energy Institute, PSU-DUT Joint Center for Energy Research and Department of Energy & Mineral Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, USA;
e Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2019-11-02 Revised:2019-11-27 Online:2020-08-18 Published:2020-08-08
Supported by:
This work was supported by the National Natural Science Foundation of China (21401017, 21236008), the Fundamental Research Funds for the Central Universities (DUT19LK17, DUT18RC(3)057), G. Z. and J. T. M. were supported in part by the National Science Foundation under Cooperative Agreement (EEC-1647722). Use of the Advanced Photon Source is supported by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences (DE-AC02-06CH11357).

Abstract

Abstract: Heterogeneous catalysts with ultra-small clusters and atomically dispersed (USCAD) active sites have gained increasing attention in recent years. However, developing USCAD catalysts with high-density metal sites anchored in porous nanomaterials is still challenging. Here, through the template-free S-assisted pyrolysis of low-cost Fe-salts with melamine (MA), porous alveolate Fe/g-C₃N₄ catalysts with high-density (Fe loading up to 17.7 wt%) and increased USCAD Fe sites were synthesized. The presence of a certain amount of S species in the Fe-salts/MA system plays an important role in the formation of USCAD S-Fe-salt/CN catalysts; the S species act as a "sacrificial carrier" to increase the dispersion of Fe species through Fe-S coordination and generate porous alveolate structure by escaping in the form of SO₂ during pyrolysis. The S-Fe-salt/CN catalysts exhibit greatly promoted activity and reusability for degrading various organic pollutants in advanced oxidation processes compared to the corresponding Fe-salt/CN catalysts, due to the promoted accessibility of USCAD Fe sites by the porous alveolate structure. This S-assisted method exhibits good feasibility in a large variety of S species (thiourea, S powder, and NH₄SCN) and Fe salts, providing a new avenue for the low-cost and large-scale synthesis of high-density USCAD metal/g-C₃N₄ catalysts.

Key words: Sulfur-assisted synthesis, Porous alveolate structure, Ultra-small cluster and atomically, dispersed active sites, Fe/g-C₃N₄, Advanced oxidation processes

Sufeng An, Guanghui Zhang, Jiaqiang Liu, Keyan Li, Gang Wan, Yan Liang, Donghui Ji, Jeffrey T. Miller, Chunshan Song, Wei Liu, Zhongmin Liu, Xinwen Guo. A facile sulfur-assisted method to synthesize porous alveolate Fe/g-C₃N₄ catalysts with ultra-small cluster and atomically dispersed Fe sites[J]. Chinese Journal of Catalysis, 2020, 41(8): 1198-1207.

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A facile sulfur-assisted method to synthesize porous alveolate Fe/g-C₃N₄ catalysts with ultra-small cluster and atomically dispersed Fe sites

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