Photocatalytic ammonia(NH_(3))decomposition is a key strategy for green hydrogen production and renewable energy conversion.Although conventional plasmonic metal/TiO_(2) composites exhibit some activity,their applicat...Photocatalytic ammonia(NH_(3))decomposition is a key strategy for green hydrogen production and renewable energy conversion.Although conventional plasmonic metal/TiO_(2) composites exhibit some activity,their applications are constrained by high carrier recombination rates and narrow light harvesting ranges.To address these challenges,this study innovatively introduces the plasmonic semiconductor MoO_(3-x),which is characterized by broad-spectrum absorption and abundant oxygen vacancies,to construct a Cu-MoO_(3-x)/TiO_(2) plasmon resonance coupling nanostructure.The construction of the Cu-MoO_(3-x) composite stabilizes Cu via MoO_(3-x) coating and facilitates electron transfer from Cu to MoO_(3-x),generating more oxygen vacancies for NH_(3) activation.The visible localized surface plasmon resonance(LSPR)response of Cu,coupled with the visible to near-infrared LSPR resonance of MoO_(3-x),broadens the spectral response and optimizes carrier dynamics,thereby reducing the recombination of photogenerated carriers.The use of hot carriers and plasmonic photothermal effects synergistically accelerate surface reaction kinetics and enhance photocatalytic efficiency.In particular,the optimal Cu-MoO_(3-x)/TiO_(2) catalyst results in an enhanced NH_(3) decomposition rate of 103.2 mmol·g^(-1)·h^(-1) under fullspectrum light irradiation,representing 29-fold and 94-fold enhancements over those of Cu/TiO_(2) and MoO_(3-x)/TiO_(2),respectively.This innovative design strategy transcends traditional plasmonic metal/semiconductor catalyst designs and opens new avenues for developing efficient solar-driven plasmon resonance coupling catalysts.展开更多
基金financially supported in part by the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0450401)the National Natural Science Foundation of China(U23A2091,22122506,22479140,22479139,22232003,22075267,22109152)+3 种基金Anhui Provincial Natural Science Foundation(2408085JX001)Youth Innovation Promotion Association of CAS(Y2023129)Fundamental Research Funds for the Central Universities(20720220007,WK2060000039,KY2140000031)West Light Foundation of the Chinese Academy of Sciences(xbzg-zdsys-202209).
文摘Photocatalytic ammonia(NH_(3))decomposition is a key strategy for green hydrogen production and renewable energy conversion.Although conventional plasmonic metal/TiO_(2) composites exhibit some activity,their applications are constrained by high carrier recombination rates and narrow light harvesting ranges.To address these challenges,this study innovatively introduces the plasmonic semiconductor MoO_(3-x),which is characterized by broad-spectrum absorption and abundant oxygen vacancies,to construct a Cu-MoO_(3-x)/TiO_(2) plasmon resonance coupling nanostructure.The construction of the Cu-MoO_(3-x) composite stabilizes Cu via MoO_(3-x) coating and facilitates electron transfer from Cu to MoO_(3-x),generating more oxygen vacancies for NH_(3) activation.The visible localized surface plasmon resonance(LSPR)response of Cu,coupled with the visible to near-infrared LSPR resonance of MoO_(3-x),broadens the spectral response and optimizes carrier dynamics,thereby reducing the recombination of photogenerated carriers.The use of hot carriers and plasmonic photothermal effects synergistically accelerate surface reaction kinetics and enhance photocatalytic efficiency.In particular,the optimal Cu-MoO_(3-x)/TiO_(2) catalyst results in an enhanced NH_(3) decomposition rate of 103.2 mmol·g^(-1)·h^(-1) under fullspectrum light irradiation,representing 29-fold and 94-fold enhancements over those of Cu/TiO_(2) and MoO_(3-x)/TiO_(2),respectively.This innovative design strategy transcends traditional plasmonic metal/semiconductor catalyst designs and opens new avenues for developing efficient solar-driven plasmon resonance coupling catalysts.
