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Issue 17, 2019
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Facile formation of CoN4 active sites onto a SiO2 support to achieve robust CO2 and proton reduction in a noble-metal-free photocatalytic system

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Abstract

The conversion of CO2 and protons to solar fuels (CO and H2) is the basis of artificial photosynthesis. To date, most of the reported cobalt-based molecular catalysts or single-atom catalysts (SAC) feature a CoN4 core structure. However, the preparation of these metal complex catalysts or SACs requires either a complicated organic ligand synthesis method or harsh material fabrication conditions. In this study, the facile formation of an active CoN4 structure onto a SiO2 support was achieved via self-coordination of Co2+ ions with aminated SiO2 nanoparticles. The formation of the CoN4 structure was identified by synchrotron-based X-ray absorption spectroscopy. The CoN4-SiO2 catalyst exhibited exceptional bifunctional activity of mediating the CO2-to-CO and 2H+-to-H2 conversions in a photochemical system containing g-C3N4 as a photosensitizer. The system robustly produced syngas (CO + H2, CO/H2 = 1 : 1–1 : 2) with a high activity (5053 μmol g−1 and 36 μmol g−1 h−1 based on the catalyst) and remarkable stability (durability > 120 h). Mechanistic studies reveal that the Co(I)-species is the active species generated via a photoinduced electron transfer from g-C3N4 to CoN4-SiO2. The dissociation of Co2+ from the aminated SiO2 support and the decomposition of g-C3N4 under irradiation are the main reasons for the inactivation of the system after long-time photocatalysis.

Graphical abstract: Facile formation of CoN4 active sites onto a SiO2 support to achieve robust CO2 and proton reduction in a noble-metal-free photocatalytic system

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Publication details

The article was received on 25 Jan 2019, accepted on 26 Mar 2019 and first published on 26 Mar 2019


Article type: Paper
DOI: 10.1039/C9TA00949C
Citation: J. Mater. Chem. A, 2019,7, 10475-10482

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    Facile formation of CoN4 active sites onto a SiO2 support to achieve robust CO2 and proton reduction in a noble-metal-free photocatalytic system

    J. Hu, M. Gui, W. Xia, J. Wu, Y. Zhou, N. Feng, J. Xiao, H. Liu, C. Tung, L. Wu and F. Wang, J. Mater. Chem. A, 2019, 7, 10475
    DOI: 10.1039/C9TA00949C

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