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
This article presents our experimental studies to unravel the dynamic photovoltaic processes occurring at donor:acceptor(D:A)and electrode:active layer(E:A)interfaces under device-operating conditions by using two uni...This article presents our experimental studies to unravel the dynamic photovoltaic processes occurring at donor:acceptor(D:A)and electrode:active layer(E:A)interfaces under device-operating conditions by using two unique magneto-optical measurements,namely photo-induced capacitance and magnetic field effect measurement.First,we have found that a higher surface polarization of dielectric thin film can decrease the surface charge accumulation at E:A interface.The photo-induced capacitance results indicate that dielectric thin film plays a crucial role in the charge collection in generating photocurrent in organic solar cells.Second,our experimental results from magnetic field effect show that the binding energies of charge transfer(CT)states at D:A interface can be evaluated by using the critical bias required to completely dissociate the CT states.This is the first experimental demonstration that the binding energies of CT states can be measured under deviceoperating conditions.Furthermore,we use our measurement of magnetic field effect to investigate the most popular organic photovoltaic solar cells,organometal halide perovskite photovoltaic devices.The results of magneto-photoluminescence show that the photogenerated electrons and holes are inevitably recombined into electron–hole pairs through a spin-dependent process in the perovskites.Therefore,using spin polarizations can present a new design to control the photovoltaic loss in perovskites-based photovoltaic devices.Also,we found that introducing D:A interface can largely affect the bulk charge dissociation and recombination in perovskite solar cells.This indicates that the interfacial and bulk photovoltaic processes are internally coupled in developing photovoltaic actions in perovskite devices.Clearly,these magneto-optical measurements show a great potential to unravel the deeper photovoltaic processes occurring at D:A and E:A interfaces in both organic bulk-heterojunction and perovskite solar cells under device-operating conditions.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.
基金supported by the National Science Foundation of the United States(ECCS-1102011,ECCS-0644945,and CBET-1438181)the support from Sustainable Energy Education and Research Center and Center for Materials Processing at the University of Tennessee+1 种基金This research was partially conducted at the Center for Nanophase Materials Sciences based on user project(CNMS2012-106,CNMS2012-107,CNMS-2012-108),which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities,U.S.Department of Energythe University of Tennessee also acknowledge the project support from the National Natural Science Foundation of China(21161160445,61077020)
文摘This article presents our experimental studies to unravel the dynamic photovoltaic processes occurring at donor:acceptor(D:A)and electrode:active layer(E:A)interfaces under device-operating conditions by using two unique magneto-optical measurements,namely photo-induced capacitance and magnetic field effect measurement.First,we have found that a higher surface polarization of dielectric thin film can decrease the surface charge accumulation at E:A interface.The photo-induced capacitance results indicate that dielectric thin film plays a crucial role in the charge collection in generating photocurrent in organic solar cells.Second,our experimental results from magnetic field effect show that the binding energies of charge transfer(CT)states at D:A interface can be evaluated by using the critical bias required to completely dissociate the CT states.This is the first experimental demonstration that the binding energies of CT states can be measured under deviceoperating conditions.Furthermore,we use our measurement of magnetic field effect to investigate the most popular organic photovoltaic solar cells,organometal halide perovskite photovoltaic devices.The results of magneto-photoluminescence show that the photogenerated electrons and holes are inevitably recombined into electron–hole pairs through a spin-dependent process in the perovskites.Therefore,using spin polarizations can present a new design to control the photovoltaic loss in perovskites-based photovoltaic devices.Also,we found that introducing D:A interface can largely affect the bulk charge dissociation and recombination in perovskite solar cells.This indicates that the interfacial and bulk photovoltaic processes are internally coupled in developing photovoltaic actions in perovskite devices.Clearly,these magneto-optical measurements show a great potential to unravel the deeper photovoltaic processes occurring at D:A and E:A interfaces in both organic bulk-heterojunction and perovskite solar cells under device-operating conditions.