Converting solar energy into valuable hydrogen and hydrocarbon fuels through photoelectrocatalytic water splitting and CO2 reduction is highly promising in addressing the growing demand for renewable and clean energy ...Converting solar energy into valuable hydrogen and hydrocarbon fuels through photoelectrocatalytic water splitting and CO2 reduction is highly promising in addressing the growing demand for renewable and clean energy resources. However, the solar-to-fuel conversion efficiency is still very low due to limited light absorption and rapid bulk recombination of charge carriers. In this work, we present chlorophyll (Chl) and its derivative sodium copper chlorophyllin (ChlCuNa), as dye sensitizers, modified BiVO4 to improve the photoelectrochemical (PEC) performance. The photocurrent of BiVO4 is surprisingly decreased after a direct sensitization of Chl while the sensitization of ChlCuNa obviously enhances photocurrent of BiV04 electrodes by improved surface hydrophilicity and extended light absorption. ChlCuNa-sensitized BiVO4 achieves an improved H2 evolution rate of 5.43/~molh l cm 2 in water splitting and an enhanced HCOOH production rate 0f2.15 p^mol h 1 cm 2 in CO2 PEC reduction, which are 1.9 times and 2.4 times higher than pristine BiV04, respectively. It is suggested that the derivative ChlCuNa is a more effective sensitizer for solar-to-fuel energy conversion and CO2 utilization than Chl.展开更多
基金financial support from Ministry of Science and Technology of the People’s Republic of China(No.2016YFE0112200)the National Natural Science Foundation of China(Nos.21507011,21677037,21607027)
文摘Converting solar energy into valuable hydrogen and hydrocarbon fuels through photoelectrocatalytic water splitting and CO2 reduction is highly promising in addressing the growing demand for renewable and clean energy resources. However, the solar-to-fuel conversion efficiency is still very low due to limited light absorption and rapid bulk recombination of charge carriers. In this work, we present chlorophyll (Chl) and its derivative sodium copper chlorophyllin (ChlCuNa), as dye sensitizers, modified BiVO4 to improve the photoelectrochemical (PEC) performance. The photocurrent of BiVO4 is surprisingly decreased after a direct sensitization of Chl while the sensitization of ChlCuNa obviously enhances photocurrent of BiV04 electrodes by improved surface hydrophilicity and extended light absorption. ChlCuNa-sensitized BiVO4 achieves an improved H2 evolution rate of 5.43/~molh l cm 2 in water splitting and an enhanced HCOOH production rate 0f2.15 p^mol h 1 cm 2 in CO2 PEC reduction, which are 1.9 times and 2.4 times higher than pristine BiV04, respectively. It is suggested that the derivative ChlCuNa is a more effective sensitizer for solar-to-fuel energy conversion and CO2 utilization than Chl.