To overcome the serious technological issues affecting lithium-sulfur(Li-S) batteries,such as sluggish sulfur redox kinetics and the detrimental shuttle effect,heterostructure engineering has been investigated as a st...To overcome the serious technological issues affecting lithium-sulfur(Li-S) batteries,such as sluggish sulfur redox kinetics and the detrimental shuttle effect,heterostructure engineering has been investigated as a strategy to effectively capture soluble lithium polysulfide intermediates and promote their conversion reaction by integrating highly polar metal oxides with catalytically active metals sulfides.However,to fully exploit the outstanding properties of heterostructure-based composites,their detailed structure and interfacial contacts should be designed rationally.Herein,optimally arranged TiO_(2)and MoS_(2)-based heterostructures(TiO_(2)@MoS_(2)) are fabricated on carbon cloth as a multifunctional interlayer to efficiently trap polysulfide intermediates and accelerate their redox kinetics.Owing to the synergistic effects between TiO_(2)and MoS_(2)and the uniform heterointerface distribution that induces the ideally oriented built-in electric field,Li-S batteries with TiO_(2)@MoS_(2)interlayers exhibit high rate capability(601 mA h g^(-1)at 5 C),good cycling stability(capacity-fade rate of 0.067% per cycle over 500 cycles at2 C),and satisfactory areal capacity(5.2 mA h cm^(-2)) under an increased sulfur loading of 5.2 mg cm^(-2).Moreover,by comparing with a MoS_(2)@TiO_(2)interlayer composed of reversely arranged heterostructures,the effect of the built-in electric field’s direction on the electrocatalytic reactions of polysulfide intermediates is thoroughly investigated for the first time.The superior electrocatalytic activities of the rationally arranged TiO_(2)@MoS_(2)interlayer demonstrate the importance of optimizing the built-in electric field of heterostructures for producing high-performance Li-S batteries.展开更多
Oxygen evolution reaction(OER)as a half-anodic reaction of water splitting hinders the overall reaction efficiency owing to its thermodynamic and kinetic limitations.Iodide oxidation reaction(IOR)with low thermodynami...Oxygen evolution reaction(OER)as a half-anodic reaction of water splitting hinders the overall reaction efficiency owing to its thermodynamic and kinetic limitations.Iodide oxidation reaction(IOR)with low thermodynamic barrier and rapid reaction kinetics is a promising alternative to the OER.Herein,we present a molybdenum disulfide(MoS_(2))electrocatalyst for a high-efficiency and remarkably durable anode enabling IOR.MoS_(2)nanosheets deposited on a porous carbon paper via atomic layer deposition show an IOR current density of 10 mA cm^(–2)at an anodic potential of 0.63 V with respect to the reversible hydrogen electrode owing to the porous substrate as well as the intrinsic iodide oxidation capability of MoS_(2)as confirmed by theoretical calculations.The lower positive potential applied to the MoS_(2)-based heterostructure during IOR electrocatalysis prevents deterioration of the active sites on MoS_(2),resulting in exceptional durability of 200 h.Subsequently,we fabricate a two-electrode system comprising a MoS_(2)anode for IOR combined with a commercial Pt@C catalyst cathode for hydrogen evolution reaction.Moreover,the photovoltaic–electrochemical hydrogen production device comprising this electrolyzer and a single perovskite photovoltaic cell shows a record-high current density of 21 mA cm^(–2)at 1 sun under unbiased conditions.展开更多
Perovskite light-emitting diodes(PeLEDs)are considered as promising candidates for nextgeneration solution-processed full-color displays.However,the external quantum efficiencies(EQEs)and operational stabilities of de...Perovskite light-emitting diodes(PeLEDs)are considered as promising candidates for nextgeneration solution-processed full-color displays.However,the external quantum efficiencies(EQEs)and operational stabilities of deep-blue(<460 nm)PeLEDs still lag far behind their red and green counterparts.Herein,a rapid crystallization method based on hot-antisolvent bathing is proposed for realization of deep-blue PeLEDs.By promoting immediate removal of the precursor solvent from the wet perovskite films,development of the quasi-two-dimensional(2D)Ruddlesden–Popper perovskite(2D-RPP)crystals with n values>3 is hampered completely,so that phase-pure 2D-RPP films with bandgaps suitable for deep-blue PeLEDs can be obtained successfully.The uniquely developed rapid crystallization method also enables formation of randomly oriented 2D-RPP crystals,thereby improving the transfer and transport kinetics of the charge carriers.Thus,high-performance deep-blue PeLEDs emitting at 437 nm with a peak EQE of 0.63%are successfully demonstrated.The color coordinates are confirmed to be(0.165,0.044),which match well with the Rec.2020 standard blue gamut and have excellent spectral stability.展开更多
基金supported by the National R&D Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (2018M3D1A1058793 and 2021R1A3B1068920)supported by the Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (2018M3D1A1058744)the Yonsei Signature Research Cluster Program of 2021 (2021-22-0002)。
文摘To overcome the serious technological issues affecting lithium-sulfur(Li-S) batteries,such as sluggish sulfur redox kinetics and the detrimental shuttle effect,heterostructure engineering has been investigated as a strategy to effectively capture soluble lithium polysulfide intermediates and promote their conversion reaction by integrating highly polar metal oxides with catalytically active metals sulfides.However,to fully exploit the outstanding properties of heterostructure-based composites,their detailed structure and interfacial contacts should be designed rationally.Herein,optimally arranged TiO_(2)and MoS_(2)-based heterostructures(TiO_(2)@MoS_(2)) are fabricated on carbon cloth as a multifunctional interlayer to efficiently trap polysulfide intermediates and accelerate their redox kinetics.Owing to the synergistic effects between TiO_(2)and MoS_(2)and the uniform heterointerface distribution that induces the ideally oriented built-in electric field,Li-S batteries with TiO_(2)@MoS_(2)interlayers exhibit high rate capability(601 mA h g^(-1)at 5 C),good cycling stability(capacity-fade rate of 0.067% per cycle over 500 cycles at2 C),and satisfactory areal capacity(5.2 mA h cm^(-2)) under an increased sulfur loading of 5.2 mg cm^(-2).Moreover,by comparing with a MoS_(2)@TiO_(2)interlayer composed of reversely arranged heterostructures,the effect of the built-in electric field’s direction on the electrocatalytic reactions of polysulfide intermediates is thoroughly investigated for the first time.The superior electrocatalytic activities of the rationally arranged TiO_(2)@MoS_(2)interlayer demonstrate the importance of optimizing the built-in electric field of heterostructures for producing high-performance Li-S batteries.
基金the National R&D Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(Grant Nos.2021R1A3B10689202021M3H4A1A03049662)+1 种基金the Materials and Components Technology Development Program of MOTIE/KEIT(10080527)the Yonsei Signature Research Cluster Program of 2021(2021-22-0002)。
文摘Oxygen evolution reaction(OER)as a half-anodic reaction of water splitting hinders the overall reaction efficiency owing to its thermodynamic and kinetic limitations.Iodide oxidation reaction(IOR)with low thermodynamic barrier and rapid reaction kinetics is a promising alternative to the OER.Herein,we present a molybdenum disulfide(MoS_(2))electrocatalyst for a high-efficiency and remarkably durable anode enabling IOR.MoS_(2)nanosheets deposited on a porous carbon paper via atomic layer deposition show an IOR current density of 10 mA cm^(–2)at an anodic potential of 0.63 V with respect to the reversible hydrogen electrode owing to the porous substrate as well as the intrinsic iodide oxidation capability of MoS_(2)as confirmed by theoretical calculations.The lower positive potential applied to the MoS_(2)-based heterostructure during IOR electrocatalysis prevents deterioration of the active sites on MoS_(2),resulting in exceptional durability of 200 h.Subsequently,we fabricate a two-electrode system comprising a MoS_(2)anode for IOR combined with a commercial Pt@C catalyst cathode for hydrogen evolution reaction.Moreover,the photovoltaic–electrochemical hydrogen production device comprising this electrolyzer and a single perovskite photovoltaic cell shows a record-high current density of 21 mA cm^(–2)at 1 sun under unbiased conditions.
基金National R&D Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(Grant Nos.2018M3D1A1058793 and 2021R1A3B1068920)the Yonsei Signature Research Cluster Program of 2021(Grant No.2021-22-0002).
文摘Perovskite light-emitting diodes(PeLEDs)are considered as promising candidates for nextgeneration solution-processed full-color displays.However,the external quantum efficiencies(EQEs)and operational stabilities of deep-blue(<460 nm)PeLEDs still lag far behind their red and green counterparts.Herein,a rapid crystallization method based on hot-antisolvent bathing is proposed for realization of deep-blue PeLEDs.By promoting immediate removal of the precursor solvent from the wet perovskite films,development of the quasi-two-dimensional(2D)Ruddlesden–Popper perovskite(2D-RPP)crystals with n values>3 is hampered completely,so that phase-pure 2D-RPP films with bandgaps suitable for deep-blue PeLEDs can be obtained successfully.The uniquely developed rapid crystallization method also enables formation of randomly oriented 2D-RPP crystals,thereby improving the transfer and transport kinetics of the charge carriers.Thus,high-performance deep-blue PeLEDs emitting at 437 nm with a peak EQE of 0.63%are successfully demonstrated.The color coordinates are confirmed to be(0.165,0.044),which match well with the Rec.2020 standard blue gamut and have excellent spectral stability.