The synthesis of renewable chemical fuels from CO_(2) and H_(2)O via photoelectrochemical(PEC)route reprensents a promising room-temperature approach for transforming greenhouse gas into value-added chemicals(e.g.,syn...The synthesis of renewable chemical fuels from CO_(2) and H_(2)O via photoelectrochemical(PEC)route reprensents a promising room-temperature approach for transforming greenhouse gas into value-added chemicals(e.g.,syngas),but to date it has been hampered by the lack of efficient photocathode for CO_(2) reduction.Herein,we report efficient PEC CO_(2) reduction into syngas by photocathode engineering.The photocathode is consisting of a planar p-n Si junction for strong light harvesting,GaN nanowires for efficient electron extraction and transfer,and Au/TiO_(2)for rapid electrocatalytic syngas production.The photocathode yields a record-high solar energy conversion efficiency of 2.3%.Furthermore,desirable syngas compositions with CO/H_(2)ratios such as 1:2 and 1:1 can be produced by simply varying the size of Au nanoparticle.Theoretical calculations reveal that the active sites for CO and H_(2)generation are the facet and undercoordinated sites of Au particles,respectively.展开更多
基金supported by the National Natural Science Foundation of China(22005048,51822604,51906040)the Natural Science Foundation of Jiangsu Province(Grants No BK20200399)+2 种基金Emissions Reduction Alberta(ERA)McGill Engineering Doctoral AwardNational Sciences and Engineering Research Council(NSERC)Discovery grant(grant#RGPIN2017-05187)support from“Zhishan Young Scholar”Program of Southeast University。
文摘The synthesis of renewable chemical fuels from CO_(2) and H_(2)O via photoelectrochemical(PEC)route reprensents a promising room-temperature approach for transforming greenhouse gas into value-added chemicals(e.g.,syngas),but to date it has been hampered by the lack of efficient photocathode for CO_(2) reduction.Herein,we report efficient PEC CO_(2) reduction into syngas by photocathode engineering.The photocathode is consisting of a planar p-n Si junction for strong light harvesting,GaN nanowires for efficient electron extraction and transfer,and Au/TiO_(2)for rapid electrocatalytic syngas production.The photocathode yields a record-high solar energy conversion efficiency of 2.3%.Furthermore,desirable syngas compositions with CO/H_(2)ratios such as 1:2 and 1:1 can be produced by simply varying the size of Au nanoparticle.Theoretical calculations reveal that the active sites for CO and H_(2)generation are the facet and undercoordinated sites of Au particles,respectively.
