The development of photocatalysts with wide spectral absorption and high charge separation efficiency has always been a pursued objective for photocatalytic solar energy conversion.Herein,we reported a wide-range visi...The development of photocatalysts with wide spectral absorption and high charge separation efficiency has always been a pursued objective for photocatalytic solar energy conversion.Herein,we reported a wide-range visible-light-active Bi_(4)TaO_(8)Cl(BTOC)single crystal nanoplate with dominating{110}and{001}facets for enhancing the intrinsic charge separation efficiency.Insitu selective photodeposition of metals and metal oxides provides evidences of photogenerated electrons and holes spatially separated on{110}and{001}coexposed facets of BTOC,respectively.The intrinsic charge separation efficiency was demonstrated to be closely dependent on the crystal facets,which can be modulated by tuning the coexposed crystal facet ratio.Further surface modification of BTOC with suitable dual cocatalyst Ag and RuOx enables remarkable improvement of charge separation efficiency and photocatalytic water oxidation performance.Investigation by comparison between well-defined BTOC nanoplate and BTOC nanoparticles confirmed the significance of coexposed crystal facets for efficient spatial charge separation and the blocking of reverse reaction from Fe^(2+)to Fe^(3+)ions during water oxidation reaction,indicating that rational modulation of exposed crystal facets is significant for controlling the intrinsic charge separation efficiency on Bi_(4)TaO_(8)Cl photocatalyst for efficient photocatalytic water splitting.展开更多
基金The work was supported by the National Key Research and Development Program of China(2021YFA1502300)conducted by the Fundamental Research Center of Artificial Photosynthesis(FReCAP),and financially supported by the National Natural Science Foundation of China(22088102)+1 种基金R.L.thanks the support from the National Natural Science Foundation of China(22090033)the Youth Innovation Promotion Association of the Chinese Academy of Sciences.A.A.gratefully acknowledges the CAS-TWAS Presidential fellowship.
文摘The development of photocatalysts with wide spectral absorption and high charge separation efficiency has always been a pursued objective for photocatalytic solar energy conversion.Herein,we reported a wide-range visible-light-active Bi_(4)TaO_(8)Cl(BTOC)single crystal nanoplate with dominating{110}and{001}facets for enhancing the intrinsic charge separation efficiency.Insitu selective photodeposition of metals and metal oxides provides evidences of photogenerated electrons and holes spatially separated on{110}and{001}coexposed facets of BTOC,respectively.The intrinsic charge separation efficiency was demonstrated to be closely dependent on the crystal facets,which can be modulated by tuning the coexposed crystal facet ratio.Further surface modification of BTOC with suitable dual cocatalyst Ag and RuOx enables remarkable improvement of charge separation efficiency and photocatalytic water oxidation performance.Investigation by comparison between well-defined BTOC nanoplate and BTOC nanoparticles confirmed the significance of coexposed crystal facets for efficient spatial charge separation and the blocking of reverse reaction from Fe^(2+)to Fe^(3+)ions during water oxidation reaction,indicating that rational modulation of exposed crystal facets is significant for controlling the intrinsic charge separation efficiency on Bi_(4)TaO_(8)Cl photocatalyst for efficient photocatalytic water splitting.
