We demonstrated an efficient solar photovoltaic-powered electrochemical CO_(2) reduction device with a high-pressure CO_(2)-captured liquid feed.In an“air-to-barrel”picture,this device holds promise to avoid both hi...We demonstrated an efficient solar photovoltaic-powered electrochemical CO_(2) reduction device with a high-pressure CO_(2)-captured liquid feed.In an“air-to-barrel”picture,this device holds promise to avoid both high-temperature gaseous CO_(2) regeneration and high energy-cost gas product separation steps,while these steps are necessary for devices with a gaseous CO_(2) feed.To date,solar fuel production with a CO_(2)-saturated liquid feed suffers from high over-potential to suppress the hydrogen evolution reaction and consequently,low solar-to-chemical(STC)energy conversion efficiency.Here,we presented a distinct high-pressure operando strategy,i.e.,we took extra advantage of the high pressure in catalyst synthesis besides in the period of the CO_(2) reduction reaction(CO_(2)RR).The power of this strategy was demonstrated by a proof-of-concept device in which a representative copper catalyst was first synthesized in operando in a high-pressure(50 bar)CO_(2)-saturated KHCO3 solution,and then this high-pressure CO_(2)-captured liquid was converted to solar fuel using the operando synthesized Cu catalyst.This Cu catalyst achieved 95%CO_(2)RR selectivity at the recorded low potential of−0.3 V vs.RHE enabled by the combination of operando facet engineering and oxide derivation.Furthermore,this device achieved a record-high STC efficiency of 21.6%under outdoor illumination,superior to other CO_(2)-saturated liquid-fed devices,and compared favorably to gaseous CO_(2)-fed devices.展开更多
基金supported by the National Natural Science Foundation of China(51888103,52006103,51976090,and 52006101)Scientific and Technological Innovation Project of Carbon Emission Peak and Carbon Neutrality of Jiangsu Province(BE2022024)+1 种基金Natural Science Foundation of Jiangsu Province(BK20200072,BK20200491,and BK20200500)China Postdoctoral Science Foundation(2020M681603)。
文摘We demonstrated an efficient solar photovoltaic-powered electrochemical CO_(2) reduction device with a high-pressure CO_(2)-captured liquid feed.In an“air-to-barrel”picture,this device holds promise to avoid both high-temperature gaseous CO_(2) regeneration and high energy-cost gas product separation steps,while these steps are necessary for devices with a gaseous CO_(2) feed.To date,solar fuel production with a CO_(2)-saturated liquid feed suffers from high over-potential to suppress the hydrogen evolution reaction and consequently,low solar-to-chemical(STC)energy conversion efficiency.Here,we presented a distinct high-pressure operando strategy,i.e.,we took extra advantage of the high pressure in catalyst synthesis besides in the period of the CO_(2) reduction reaction(CO_(2)RR).The power of this strategy was demonstrated by a proof-of-concept device in which a representative copper catalyst was first synthesized in operando in a high-pressure(50 bar)CO_(2)-saturated KHCO3 solution,and then this high-pressure CO_(2)-captured liquid was converted to solar fuel using the operando synthesized Cu catalyst.This Cu catalyst achieved 95%CO_(2)RR selectivity at the recorded low potential of−0.3 V vs.RHE enabled by the combination of operando facet engineering and oxide derivation.Furthermore,this device achieved a record-high STC efficiency of 21.6%under outdoor illumination,superior to other CO_(2)-saturated liquid-fed devices,and compared favorably to gaseous CO_(2)-fed devices.
