TY - JOUR
T1 - A facile sulfur-assisted method to synthesize porous alveolate Fe/g-C3N4 catalysts with ultra-small cluster and atomically dispersed Fe sites
AU - An, Sufeng
AU - Zhang, Guanghui
AU - Liu, Jiaqiang
AU - Li, Keyan
AU - Wan, Gang
AU - Liang, Yan
AU - Ji, Donghui
AU - Miller, Jeffrey T.
AU - Song, Chunshan
AU - Liu, Wei
AU - Liu, Zhongmin
AU - Guo, Xinwen
N1 - Funding Information:
Materials Research Collaborative Access Team (MRCAT, Sector 10-BM) operations are supported by the Department of Energy and the MRCAT member institutions. Sector 20 operations are supported by the US Department of Energy and the Canadian Light Source.
Funding Information:
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).
Publisher Copyright:
© 2020 Dalian Institute of Chemical Physics, the Chinese Academy of Sciences
PY - 2020/8
Y1 - 2020/8
N2 - 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.
AB - 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.
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U2 - 10.1016/S1872-2067(20)63529-X
DO - 10.1016/S1872-2067(20)63529-X
M3 - Article
AN - SCOPUS:85081280493
VL - 41
SP - 1198
EP - 1207
JO - Chinese Journal of Catalysis
JF - Chinese Journal of Catalysis
SN - 0253-9837
IS - 8
ER -