CuS is an encouraging photoelectrode candidate that meets the essential requirements for efficient solar-to-hydrogen production,but it has not been thoroughly studied.A CuS light absorber layer is grown by the self-as...CuS is an encouraging photoelectrode candidate that meets the essential requirements for efficient solar-to-hydrogen production,but it has not been thoroughly studied.A CuS light absorber layer is grown by the self-assembly of copper and sulfur precursors on a carbon paper(CP)electrode.Simultaneously,rGO is introduced as a buffer layer to control the optical and electrical properties of the absorber.The well-ordered microstructural arrangement suppresses the recombination loss of electrons and holes owing to enhanced charge-carrier generation,separation,and transport.The potential reaching 10 mA cm^(-2)in 1.0 M KOH solution is significantly lowered to 0.87 V,and the photocurrent density at 1.23 V is 94.7 mA cm^(-2).The computational result reveals that the potential-determining step is sensitive to O^(*)stability;the lower stability of O^(*)in the thin layer of CuS/rGO decreases the free-energy gap between the initial and final states of the potential-determining step,resulting in a lowering of the onset potential.The faradaic efficiency for the photoelectrochemical oxygen evolution reaction in the optimized 2CuS/1rGO/CP photoanode is 98.60%,and the applied bias photon-to-current and the solar-to-hydrogen efficiencies are 11.2%and 15.7%,respectively,and its ultra-high performance is maintained for 250 h.These record-breaking achievement indices may be a trigger for establishing a green hydrogen economy.展开更多
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2022R1A2C2008313)
文摘CuS is an encouraging photoelectrode candidate that meets the essential requirements for efficient solar-to-hydrogen production,but it has not been thoroughly studied.A CuS light absorber layer is grown by the self-assembly of copper and sulfur precursors on a carbon paper(CP)electrode.Simultaneously,rGO is introduced as a buffer layer to control the optical and electrical properties of the absorber.The well-ordered microstructural arrangement suppresses the recombination loss of electrons and holes owing to enhanced charge-carrier generation,separation,and transport.The potential reaching 10 mA cm^(-2)in 1.0 M KOH solution is significantly lowered to 0.87 V,and the photocurrent density at 1.23 V is 94.7 mA cm^(-2).The computational result reveals that the potential-determining step is sensitive to O^(*)stability;the lower stability of O^(*)in the thin layer of CuS/rGO decreases the free-energy gap between the initial and final states of the potential-determining step,resulting in a lowering of the onset potential.The faradaic efficiency for the photoelectrochemical oxygen evolution reaction in the optimized 2CuS/1rGO/CP photoanode is 98.60%,and the applied bias photon-to-current and the solar-to-hydrogen efficiencies are 11.2%and 15.7%,respectively,and its ultra-high performance is maintained for 250 h.These record-breaking achievement indices may be a trigger for establishing a green hydrogen economy.
