Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of nove...Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and Au.The electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and HER.Impressively,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 V.Moreover,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was assembled.Accordingly,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS equipment.The interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.展开更多
Photoelectrochemical devices have been developed to enable the conversion of solar energy.However,their commercial potential is restricted by the limited stability of the materials employed.To enhance the stability of...Photoelectrochemical devices have been developed to enable the conversion of solar energy.However,their commercial potential is restricted by the limited stability of the materials employed.To enhance the stability of photocathode and its solar water splitting performance,a P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt composite photocathode is developed in this work.The novel TiO_(2)/HfO_(2)/MoS_(2) serial nanostructure provides excellent stability of the photocathode,and optimizes the interface energy barrier to further facilitate the transfer process of photogenerated carriers within the photocathode.The best P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt photocathode demonstrates an initial potential of 0.5 V(vs.RHE)and a photocurrent density of-29 mA/cm^(2) at 0 V(vs.RHE).Through intensity modulated photocurrent spectroscopy and photoluminescence test,it is known that the enhanced water splitting performance is attributed to the optimized carrier transfer property.These findings provide a feasible strategy for the stability and photon quantum efficiency enhancement of silicon-based photocathode devices.展开更多
基金supported by the Key projects of intergovernmental international cooperation in the Key R&D programs of the Ministry of Science and Technology of China(No.2021YFE0115800)the National Science Funding Committee of China(No.U20A20250)。
文摘Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and Au.The electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and HER.Impressively,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 V.Moreover,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was assembled.Accordingly,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS equipment.The interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.
基金supported by the Key projects of intergovernmental international cooperation in key R&D programs of the Ministry of science and technology of China(No.2021YFE0115800)the National Science Funding Committee of China(No.U20A20250).
文摘Photoelectrochemical devices have been developed to enable the conversion of solar energy.However,their commercial potential is restricted by the limited stability of the materials employed.To enhance the stability of photocathode and its solar water splitting performance,a P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt composite photocathode is developed in this work.The novel TiO_(2)/HfO_(2)/MoS_(2) serial nanostructure provides excellent stability of the photocathode,and optimizes the interface energy barrier to further facilitate the transfer process of photogenerated carriers within the photocathode.The best P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt photocathode demonstrates an initial potential of 0.5 V(vs.RHE)and a photocurrent density of-29 mA/cm^(2) at 0 V(vs.RHE).Through intensity modulated photocurrent spectroscopy and photoluminescence test,it is known that the enhanced water splitting performance is attributed to the optimized carrier transfer property.These findings provide a feasible strategy for the stability and photon quantum efficiency enhancement of silicon-based photocathode devices.
