Issue 24, 2017

A biomimetic photoelectrocatalyst of Co–porphyrin combined with a 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 a size of 3.8 Å × 9.6 Å which favoured CO2 adsorption. The pores formed by the π–π stacking of CoTPP and g-C3N4 also provided additional space for CO2 adsorption, which was confirmed by the appearance of a desorption peak at 250 °C in the temperature programmed desorption measurement for CoTPP/g-C3N4. As a normal efficient homogeneous catalyst in organic media, CoTPP commendably maintained outstanding CO2 photoelectrocatalytic activity in heterogeneous aqueous solution, even at a low overpotential of −0.6 V (vs. normal hydrogen electrode, NHE). Under 8 h PEC CO2 reduction, formic acid generation on CoTPP/g-C3N4 reached 154.4 μmol with a TON of 137 and high selectivity of nearly 100% in liquid products. The formation of CoTPP–COO and CoTPP–COOH intermediates by the Co(II) active site and CO2 was investigated by in situ UV-vis and Raman spectra. Moreover, an isotopic labelling experiment indicated that water supplied abundant protons for the production of formic acid.

Graphical abstract: A biomimetic photoelectrocatalyst of Co–porphyrin combined with a g-C3N4 nanosheet based on π–π supramolecular interaction for high-efficiency CO2 reduction in water medium

Supplementary files

Article information

Article type
Paper
Submitted
09 ذو الحجة 1438
Accepted
14 صفر 1439
First published
17 صفر 1439

Green Chem., 2017,19, 5900-5910

A biomimetic photoelectrocatalyst of Co–porphyrin combined with a 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, 19, 5900 DOI: 10.1039/C7GC02657A

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