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Title: Selective CO 2 Reduction Catalyzed by Single Cobalt Sites on Carbon Nitride under Visible-Light Irradiation

Abstract

Framework nitrogen atoms of carbon nitride (C 3N 4) can coordinate with and activate metal sites for catalysis. In this study, C 3N 4 was employed to harvest visible light and activate Co 2+ sites, without the use of additional ligands, in photochemical CO 2 reduction. Photocatalysts containing single Co 2+ sites on C 3N 4 were prepared by a simple deposition method and demonstrated excellent activity and product selectivity toward CO formation. A turnover number of more than 200 was obtained for CO production using the synthesized photocatalyst under visible-light irradiation. Inactive cobalt oxides formed at relatively high cobalt loadings but did not alter product selectivity. Further studies with X-ray absorption spectroscopy confirmed the presence of single Co 2+ sites on C 3N 4 and their important role in achieving selective CO 2 reduction.

Authors:
 [1];  [2];  [1];  [3];  [1]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Univ. of New Hampshire, Durham, NH (United States). Dept. of Chemistry
  2. Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering
  3. Worcester Polytechnic Inst., Worcester, MA (United States). Dept. of Chemistry & Biochemistry
  4. Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering, and Division of Chemistry
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1488847
Report Number(s):
BNL-210812-2018-JAAM
Journal ID: ISSN 0002-7863
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 47; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY

Citation Formats

Huang, Peipei, Huang, Jiahao, Pantovich, Sebastian A., Carl, Alexander D., Fenton, Thomas G., Caputo, Christine A., Grimm, Ronald L., Frenkel, Anatoly I., and Li, Gonghu. Selective CO2 Reduction Catalyzed by Single Cobalt Sites on Carbon Nitride under Visible-Light Irradiation. United States: N. p., 2018. Web. doi:10.1021/jacs.8b10380.
Huang, Peipei, Huang, Jiahao, Pantovich, Sebastian A., Carl, Alexander D., Fenton, Thomas G., Caputo, Christine A., Grimm, Ronald L., Frenkel, Anatoly I., & Li, Gonghu. Selective CO2 Reduction Catalyzed by Single Cobalt Sites on Carbon Nitride under Visible-Light Irradiation. United States. doi:10.1021/jacs.8b10380.
Huang, Peipei, Huang, Jiahao, Pantovich, Sebastian A., Carl, Alexander D., Fenton, Thomas G., Caputo, Christine A., Grimm, Ronald L., Frenkel, Anatoly I., and Li, Gonghu. Sat . "Selective CO2 Reduction Catalyzed by Single Cobalt Sites on Carbon Nitride under Visible-Light Irradiation". United States. doi:10.1021/jacs.8b10380.
@article{osti_1488847,
title = {Selective CO2 Reduction Catalyzed by Single Cobalt Sites on Carbon Nitride under Visible-Light Irradiation},
author = {Huang, Peipei and Huang, Jiahao and Pantovich, Sebastian A. and Carl, Alexander D. and Fenton, Thomas G. and Caputo, Christine A. and Grimm, Ronald L. and Frenkel, Anatoly I. and Li, Gonghu},
abstractNote = {Framework nitrogen atoms of carbon nitride (C3N4) can coordinate with and activate metal sites for catalysis. In this study, C3N4 was employed to harvest visible light and activate Co2+ sites, without the use of additional ligands, in photochemical CO2 reduction. Photocatalysts containing single Co2+ sites on C3N4 were prepared by a simple deposition method and demonstrated excellent activity and product selectivity toward CO formation. A turnover number of more than 200 was obtained for CO production using the synthesized photocatalyst under visible-light irradiation. Inactive cobalt oxides formed at relatively high cobalt loadings but did not alter product selectivity. Further studies with X-ray absorption spectroscopy confirmed the presence of single Co2+ sites on C3N4 and their important role in achieving selective CO2 reduction.},
doi = {10.1021/jacs.8b10380},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 47,
volume = 140,
place = {United States},
year = {2018},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on November 10, 2019
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