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Room-Temperature Synthesis of Single Iron Site by Electrofiltration for Photoreduction of CO2 into Tunable Syngas.

Authors
  • Wang, Zhiyuan1, 2
  • Yang, Jia1
  • Cao, Junbo3
  • Chen, Wenxing4
  • Wang, Gang3
  • Liao, Fan1
  • Zhou, Xiao1
  • Zhou, Fangyao1
  • Li, Ruilong1
  • Yu, Zhen-Qiang2
  • Zhang, Guoqing1
  • Duan, Xuezhi3
  • Wu, Yuen1
  • 1 School of Chemistry and Materials Science, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China. , (China)
  • 2 School of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, China. , (China)
  • 3 State Key Laboratory of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China. , (China)
  • 4 Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China. , (China)
Type
Published Article
Journal
ACS Nano
Publisher
American Chemical Society
Publication Date
May 11, 2020
Identifiers
DOI: 10.1021/acsnano.0c02162
PMID: 32379422
Source
Medline
Keywords
Language
English
License
Unknown

Abstract

Developing a convenient and effective method to prepare single-atom catalysts at mild synthetic conditions remains a challenging task. Herein, a voltage-gauged electrofiltration method was demonstrated to synthesize single-atom site catalysts at room temperature. Under regulation of the graphene oxide membrane, a bulk Fe plate was directly converted into Fe single atoms, and the diffusion rate of Fe ions was greatly reduced, resulting in an ultralow concentration of Fe2+ around the working electrode, which successfully prevented the growing of nuclei and aggregating of metal atoms. Monatomic Fe atoms are homogeneously anchored on the as-prepared nitrogen-doped carbon. Owing to the fast photoelectron injection from photosensitizers to atomically dispersed Fe sites through the highly conductive supported N-C, the Fe-SAs/N-C exhibits an outstanding photocatalytic activity toward CO2 aqueous reduction into syngas with a tunable CO/H2 ratio under visible light irradiation. The gas evolution rates for CO and H2 are 4500 and 4950 μmol g-1 h-1, respectively, and the tunable CO/H2 ratio is from 0.3 to 8.8. This article presents an efficient strategy to develop the single-atom site catalysts and bridges the gap between heterogeneous and homogeneous catalysts toward photocatalytic CO2 aqueous reduction into syngas.

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