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The Biomimetic Photoelectrocatalyst of Co-porphyrin Combined g-C3N4 Nanosheet Based on π-π Supramolecular Interaction for High-efficiency CO2 Reduction in Water Medium

Abstract

Aiming at high-efficiency biomimetic CO2 photoelectrochemical conversion, a photoelectrocatalyst with excellent CO2 catalytic activity was designed and prepared by immobilizing CoTPP (cobalt meso-tetraphenylporphyrin) onto g-C3N4 conveniently via self-assembly based on π-π supramolecular interaction. The quasi 3-D structure of CoTPP showed a suitable hole with the size of 3.8 Å x 9.6 Å which was in favour of CO2 adsorption. The pores formed by π-π stacking of CoTPP and g-C3N4 also provided additional space for CO2 adsorption, which was confirmed by the appearance of desorption peak at 250 oC in temperature programmed desorption measurement for CoTPP/g-C3N4. As a normal efficient homogeneous catalyst in organic medium, CoTPP commendably maintained the outstanding CO2 photoelectrocatalytic activity in heterogeneous aqueous solution, even at low overpotential of -0.6 V (vs. normal hydrogen electrode, NHE). Under 8 h PEC CO2 reduction, the formic acid generation on CoTPP/g-C3N4 reached 154.4 μmol with the TON of 137 and high selectivity of nearly 100% in liquid products. The formation of CoTPP-COO- and CoTPP-COOH intermediates by Co(II) active site and CO2 was investigated by the in-situ UV-vis and Raman spectra. Moreover, the isotopic labelling experiment indicated that the water supplied abundant protons for the production of formic acid.

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Publication details

The article was received on 31 Aug 2017, accepted on 03 Nov 2017 and first published on 06 Nov 2017


Article type: Paper
DOI: 10.1039/C7GC02657A
Citation: Green Chem., 2017, Accepted Manuscript
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    The Biomimetic Photoelectrocatalyst of Co-porphyrin Combined g-C3N4 Nanosheet Based on π-π Supramolecular Interaction for High-efficiency CO2 Reduction in Water Medium

    J. Liu, H. Shi, Q. Shen, C. Guo and G. Zhao, Green Chem., 2017, Accepted Manuscript , DOI: 10.1039/C7GC02657A

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