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Title: Well-defined surface catalytic sites for solar CO 2 reduction: heterogenized molecular catalysts and single atom catalysts

Abstract

Exciting progress has been made in the area of solar fuel generation by CO2 reduction. New photocatalytic materials containing well-defined surface catalytic sites have emerged in recent years, including heterogenized molecular catalysts and single atom catalysts. This Feature Article summarizes our recent research in this area, together with brief discussions of relevant literature. In our effort to obtain heterogenized molecular catalysts, a diimine-tricarbonyl Re(I) complex and a tetraaza macrocyclic Co(III) compound were covalently attached to different surfaces, and the effects of ligand derivatization and surface characteristics on their structures and photocatalytic activities were investigated. Single atom catalysts combine the advantages of homogeneous and heterogeneous catalysis. A single-site cobalt catalyst was prepared on graphitic carbon nitride, which demonstrated excellent activity in selective CO2 reduction under visible-light irradiation. Doping carbon nitride with carbon was found to have profound effects on the structure and activity of the single-site cobalt catalyst. Our research achievements are presented to emphasize how spectroscopic techniques, including infrared, UV-visible, electron paramagnetic resonance, and X-ray absorption spectroscopies, could be combined with catalyst synthesis and computation modeling to understand the structures and properties of well-defined surface catalytic sites at the molecular level. This article also highlights challenges and opportunities in themore » broad context of solar CO2 reduction.« less

Authors:
 [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Department of Chemistry, University of New Hampshire, Durham NH 03824, USA
Publication Date:
Research Org.:
Univ. of New Hampshire, Durham, NH (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1989534
Alternate Identifier(s):
OSTI ID: 1992772
Grant/Contract Number:  
SC0016417; 1352437; 2102655
Resource Type:
Published Article
Journal Name:
ChemComm
Additional Journal Information:
Journal Name: ChemComm Journal Volume: 59 Journal Issue: 61; Journal ID: ISSN 1359-7345
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
14 SOLAR ENERGY

Citation Formats

Huang, Peipei, Shaaban, Ehab, Ahmad, Esraa, St. John, Allison, Jin, Tianqi, and Li, Gonghu. Well-defined surface catalytic sites for solar CO 2 reduction: heterogenized molecular catalysts and single atom catalysts. United Kingdom: N. p., 2023. Web. doi:10.1039/D3CC01821K.
Huang, Peipei, Shaaban, Ehab, Ahmad, Esraa, St. John, Allison, Jin, Tianqi, & Li, Gonghu. Well-defined surface catalytic sites for solar CO 2 reduction: heterogenized molecular catalysts and single atom catalysts. United Kingdom. https://doi.org/10.1039/D3CC01821K
Huang, Peipei, Shaaban, Ehab, Ahmad, Esraa, St. John, Allison, Jin, Tianqi, and Li, Gonghu. Thu . "Well-defined surface catalytic sites for solar CO 2 reduction: heterogenized molecular catalysts and single atom catalysts". United Kingdom. https://doi.org/10.1039/D3CC01821K.
@article{osti_1989534,
title = {Well-defined surface catalytic sites for solar CO 2 reduction: heterogenized molecular catalysts and single atom catalysts},
author = {Huang, Peipei and Shaaban, Ehab and Ahmad, Esraa and St. John, Allison and Jin, Tianqi and Li, Gonghu},
abstractNote = {Exciting progress has been made in the area of solar fuel generation by CO2 reduction. New photocatalytic materials containing well-defined surface catalytic sites have emerged in recent years, including heterogenized molecular catalysts and single atom catalysts. This Feature Article summarizes our recent research in this area, together with brief discussions of relevant literature. In our effort to obtain heterogenized molecular catalysts, a diimine-tricarbonyl Re(I) complex and a tetraaza macrocyclic Co(III) compound were covalently attached to different surfaces, and the effects of ligand derivatization and surface characteristics on their structures and photocatalytic activities were investigated. Single atom catalysts combine the advantages of homogeneous and heterogeneous catalysis. A single-site cobalt catalyst was prepared on graphitic carbon nitride, which demonstrated excellent activity in selective CO2 reduction under visible-light irradiation. Doping carbon nitride with carbon was found to have profound effects on the structure and activity of the single-site cobalt catalyst. Our research achievements are presented to emphasize how spectroscopic techniques, including infrared, UV-visible, electron paramagnetic resonance, and X-ray absorption spectroscopies, could be combined with catalyst synthesis and computation modeling to understand the structures and properties of well-defined surface catalytic sites at the molecular level. This article also highlights challenges and opportunities in the broad context of solar CO2 reduction.},
doi = {10.1039/D3CC01821K},
journal = {ChemComm},
number = 61,
volume = 59,
place = {United Kingdom},
year = {Thu Jul 27 00:00:00 EDT 2023},
month = {Thu Jul 27 00:00:00 EDT 2023}
}

Journal Article:
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https://doi.org/10.1039/D3CC01821K

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Toward Solar-Driven Photocatalytic CO 2 Reduction Using Water as an Electron Donor
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