Photoelectrochemical (PEC) CO2 reduction reaction (CRR) in aqueous medium is among the most promising methods to produce renewable fuel with solar and water as the energy and electron source. But the high negative bias remains a prerequisite to achieve an appreciable conversion at present due to the large overpotential of CO2 reduction. This communication describes PEC CRR with low onset potential on an amorphous silicon (a-Si) photocathode decoracted with grain-boundary-rich gold catalysts. Syngas, with high throughput and desirable CO/H2 ratios such as 1:2 and 1:1, was produced in a wide PEC range from the equilibrium potential E0(CO2/CO) of -0.1 V vs. reversible hydrogen electrode (VRHE) to as positive as 0.4 VRHE, leading to a half-cell conversion efficiency of 0.42%. This performance stands for the highest half-cell efficiency and lowest onset potential for CO2 reduction ever reported among aqueous PEC cathodes under 1 sun. The a-Si/TiO2/Au photocathodes exhibit an excellent stability in a wide potential range, with a high CO mass activity up to 180 ampere per gram of gold at -0.1 VRHE. The control of grain boundary manifests powerful potential to adjust product selectivity in PEC CO2 reduction.
Read more in our recent publication:
Energy Environ. Sci. 2018, in press.