A facile sulfur-assisted method to synthesize porous alveolate Fe/g-C3N4 catalysts with ultra-small cluster and atomically dispersed Fe sites
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. In this work, 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.
- Authors:
-
- Dalian Univ. of Technology, Liaoning (China)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- Purdue Univ., West Lafayette, IN (United States)
- Pennsylvania State Univ., University Park, PA (United States)
- Chinese Academy of Sciences (CAS), Liaoning (China)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF)
- OSTI Identifier:
- 1646793
- Grant/Contract Number:
- AC02-76SF00515; 21401017; 21236008; DUT19LK17; DUT18RC(3)057); EEC-1647722; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chinese Journal of Catalysis
- Additional Journal Information:
- Journal Volume: 41; Journal Issue: 8; Journal ID: ISSN 1872-2067
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; sulfur-assisted synthesis; porous alveolate structure; ultra-small cluster and atomically dispersed active sites; Fe/g-C3N4; advanced oxidation processes
Citation Formats
An, Sufeng, Zhang, Guanghui, Liu, Jiaqiang, Li, Keyan, Wan, Gang, Liang, Yan, Ji, Donghui, Miller, Jeffrey T., Song, Chunshan, Liu, Wei, Liu, Zhongmin, and Guo, Xinwen. A facile sulfur-assisted method to synthesize porous alveolate Fe/g-C3N4 catalysts with ultra-small cluster and atomically dispersed Fe sites. United States: N. p., 2020.
Web. doi:10.1016/s1872-2067(20)63529-x.
An, Sufeng, Zhang, Guanghui, Liu, Jiaqiang, Li, Keyan, Wan, Gang, Liang, Yan, Ji, Donghui, Miller, Jeffrey T., Song, Chunshan, Liu, Wei, Liu, Zhongmin, & Guo, Xinwen. A facile sulfur-assisted method to synthesize porous alveolate Fe/g-C3N4 catalysts with ultra-small cluster and atomically dispersed Fe sites. United States. https://doi.org/10.1016/s1872-2067(20)63529-x
An, Sufeng, Zhang, Guanghui, Liu, Jiaqiang, Li, Keyan, Wan, Gang, Liang, Yan, Ji, Donghui, Miller, Jeffrey T., Song, Chunshan, Liu, Wei, Liu, Zhongmin, and Guo, Xinwen. Thu .
"A facile sulfur-assisted method to synthesize porous alveolate Fe/g-C3N4 catalysts with ultra-small cluster and atomically dispersed Fe sites". United States. https://doi.org/10.1016/s1872-2067(20)63529-x. https://www.osti.gov/servlets/purl/1646793.
@article{osti_1646793,
title = {A facile sulfur-assisted method to synthesize porous alveolate Fe/g-C3N4 catalysts with ultra-small cluster and atomically dispersed Fe sites},
author = {An, Sufeng and Zhang, Guanghui and Liu, Jiaqiang and Li, Keyan and Wan, Gang and Liang, Yan and Ji, Donghui and Miller, Jeffrey T. and Song, Chunshan and Liu, Wei and Liu, Zhongmin and Guo, Xinwen},
abstractNote = {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. In this work, 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.},
doi = {10.1016/s1872-2067(20)63529-x},
journal = {Chinese Journal of Catalysis},
number = 8,
volume = 41,
place = {United States},
year = {Thu Mar 12 00:00:00 EDT 2020},
month = {Thu Mar 12 00:00:00 EDT 2020}
}
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