Increasing combustion of a large amount of fossil fuels cause excessive emission and accumulation of carbon dioxide (CO2). These activities bring environmental concerns and hinder the sustainable development of future energy. Photocatalytic CO2reduction is one of the efficient approaches to mitigate the issues. Among various semiconductor photocatalysts, cuprous oxide (Cu2O) is one of the most attractive materials for CO2photoreduction due to its suitable bandgap. In our research, we developed interface-specific ultrafast electronic spectroscopy including time-resolved sum-frequency generation spectroscopy (TR-ESFG) and time-resolved electronic second-harmonic generation spectroscopy (TR-ESHG), in conjunction with bulk transient absorption spectroscopy to investigate reaction mechanisms in the photocatalytic CO2of Cu2O. The ultrafast interfacial measurements show that interfacial carriers exhibit different rates of formation and recombination than bulk carriers. We further investigate photocatalytic CO2properties of Cu2O with interfacial carrier dynamics. In particular, with the electrodeposition of polyaniline onto Cu2O, the carrier recombination has been greatly slowed down and the production efficiency and stability have been significantly improved. This work will help us design new materials for photocatalytic CO2reduction.

Interfacial carrier dynamics of photoelectrodes/solution for photocatalytic CO2reduction

ACS Fall 2020 Virtual Meeting

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