Solar‐to‐chemical energy conversion is perceived as one of the most potential solutions to the current energy and environmental crisis,yet requires major scientific endeavors on the development of efficient and sust...Solar‐to‐chemical energy conversion is perceived as one of the most potential solutions to the current energy and environmental crisis,yet requires major scientific endeavors on the development of efficient and sustainable photocatalysts.Remolding the composition and morphology of a semiconductor jointly for the purpose of improving photocatalysis efficiency remains challenging.Herein,we rationally fabricated Cu‐doped ZnS nanoframes via a simple conjunct strategy of substitutional doping,chemical acidic etching,and sulfidation,aiming at enhancing the light utilization and charge separation/transfer efficiency for solar‐light‐driven hydrogen generation.Cu‐doped zeolitic imidazolate framework‐8(ZIF‐8)rhombic dodecahedrons are transformed to hollow Cu‐ZIF‐8 nanoframes converted to Cu‐ZnS nanoframes with three‐dimensional photocatalytic active surfaces via anisotropic chemical etching,which is further converted to Cu‐ZnS nanoframes.By combining the merits of optimal heteroatom doping and frame‐like open architecture,the obtained 1%Cu‐doped ZnS nanoframe exhibits high photocatalytic activity under solar light irradiation with improved hydrogen production rate up to 8.30 mmol h^(–1) g^(–1) and excellent stability in the absence of cocatalysts,which is significantly improved in comparison with those of the bare ZnS and Cu‐ZnS with different morphologies.This work inspired by merging the merits of metal doping and anisotropic chemical etching may shed light on the rational design and fabrication of advanced photocatalysts.展开更多
文摘Solar‐to‐chemical energy conversion is perceived as one of the most potential solutions to the current energy and environmental crisis,yet requires major scientific endeavors on the development of efficient and sustainable photocatalysts.Remolding the composition and morphology of a semiconductor jointly for the purpose of improving photocatalysis efficiency remains challenging.Herein,we rationally fabricated Cu‐doped ZnS nanoframes via a simple conjunct strategy of substitutional doping,chemical acidic etching,and sulfidation,aiming at enhancing the light utilization and charge separation/transfer efficiency for solar‐light‐driven hydrogen generation.Cu‐doped zeolitic imidazolate framework‐8(ZIF‐8)rhombic dodecahedrons are transformed to hollow Cu‐ZIF‐8 nanoframes converted to Cu‐ZnS nanoframes with three‐dimensional photocatalytic active surfaces via anisotropic chemical etching,which is further converted to Cu‐ZnS nanoframes.By combining the merits of optimal heteroatom doping and frame‐like open architecture,the obtained 1%Cu‐doped ZnS nanoframe exhibits high photocatalytic activity under solar light irradiation with improved hydrogen production rate up to 8.30 mmol h^(–1) g^(–1) and excellent stability in the absence of cocatalysts,which is significantly improved in comparison with those of the bare ZnS and Cu‐ZnS with different morphologies.This work inspired by merging the merits of metal doping and anisotropic chemical etching may shed light on the rational design and fabrication of advanced photocatalysts.