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Significance Statement
Reducing carbon dioxide (CO2) to hydrocarbon fuel with solar energy is significant for high-density solar energy storage and carbon balance. As CO2 is an extremely stable and unreactive molecule, the conversion of CO2 to fuels is a scientifically challenging problem that requires appropriate catalysts and high energy input. Using density functional theory calculations, the work [published in J. Amer. Chem. Soc. 138 (2016) 6292] by Aijun Du from Queensland University of Technology in Australia for the first time reported that single atoms of palladium and platinum supported on g-C3N4, i.e. Pd/g-C3N4 and Pt/g-C3N4, respectively, can act as efficient photocatalysts for CO2 reduction.
The supported individual metal atoms function as the active sites, while g-C3N4 provides the source of hydrogen (H*) from the hydrogen evolution reaction. The complete, as-designed photocatalysts exhibit excellent activity in CO2 reduction. HCOOH is the preferred product of CO2 reduction on the Pd/g-C3N4 catalyst with a rate-determining barrier of 0.66 eV, while the Pt/g-C3N4 catalyst prefers to reduce CO2 to CH4 with a rate-determining barrier of 1.16 eV. In addition, deposition of atom catalysts on g-C3N4 also significantly enhances the visible-light absorption, rendering them ideal for visible-light reduction of CO2.
The use of single atom supported on a stable substrate not only minimizes materials usage but also demonstrate fascinating catalytic activity due to their high ratio of low-coordinated metal atoms. This finding opens a new avenue of CO2 reduction for renewable energy supply.
Journal Reference
Am. Chem. Soc.,2016,138 (19), pp 6292–6297.
Guoping Gao1, Yan Jiao2, Eric R. Waclawik1, Aijun Du1
[expand title=”Show Affiliations”]- School of Chemistry, Physics and Mechanical Engineering,Queensland University of Technology, Garden Point Campus, Brisbane, QLD 4001, Australia
- School of Chemical Engineering,University of Adelaide, Adelaide, SA 5005, Australia
Abstract
Reducing carbon dioxide to hydrocarbon fuel with solar energy is significant for high-density solar energy storage and carbon balance. In this work, single atoms of palladium and platinum supported on graphitic carbon nitride (g-C3N4), i.e., Pd/g-C3N4 and Pt/g-C3N4, respectively, acting as photocatalysts for CO2 reduction were investigated by density functional theory calculations for the first time. During CO2 reduction, the individual metal atoms function as the active sites, while g-C3N4 provides the source of hydrogen (H*) from the hydrogen evolution reaction. The complete, as-designed photocatalysts exhibit excellent activity in CO2 reduction. HCOOH is the preferred product of CO2 reduction on the Pd/g-C3N4 catalyst with a rate-determining barrier of 0.66 eV, while the Pt/g-C3N4 catalyst prefers to reduce CO2 to CH4 with a rate-determining barrier of 1.16 eV. In addition, deposition of atom catalysts on g-C3N4 significantly enhances the visible-light absorption, rendering them ideal for visible-light reduction of CO2. Our findings open a new avenue of CO2 reduction for renewable energy supply.
Copyright © 2016 American Chemical Society
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