CdS photocatalysts have broad application prospects in environmental purification,energy conversion,and organic synthesis.However,their practical use is often hindered by the rapid recombination of photo-generated ele...CdS photocatalysts have broad application prospects in environmental purification,energy conversion,and organic synthesis.However,their practical use is often hindered by the rapid recombination of photo-generated electron-hole pairs,which limits their efficiency on various reactions.Controlling morphological structures and crystal facets engineering are effective methods to enhance the photocatalytic performance of CdS.In this work,two different forms of CdS photocatalysts were synthesized by a hydrothermal method,namely nanoflower-shaped (CdS-NF) and nanorod-shaped (CdS-NR) for hydrogen peroxide (H_(2)O_(2)) production.The exposed crystal planes of CdS-NF are mainly (0 0 2) planes,while the accesible crystal planes of CdS-NR are notablly (1 0 1) planes.Notably,the photocatalytic hydrogen peroxide production yield of CdS-NR was high at 1225.13 μmol·h^(−1)·g^(−1),which is 1.78 times higher than the H_(2)O_(2) generation rate of CdS-NF.Moreover,through free radical capture experiments and DFT calculations,the reaction pathway was further explored.Both different configurations of cadmium sulfide based photocatalysts conform to the reaction mechanism of oxygen reduction as the main and water oxidation as the auxiliary.展开更多
The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor ...The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.展开更多
在强光照射下,CdS量子点易发生光腐蚀现象,通过金属掺杂和复合的方式可以提高CdS的光催化性能和光稳定性。采用水热法合成了Zn掺杂CdS/g-C_(3)N_(4)复合纳米材料(Zn-CdS/g-C_(3)N_(4))。利用扫描电子显微镜(SEM)、透射电子显微镜(TEM)、...在强光照射下,CdS量子点易发生光腐蚀现象,通过金属掺杂和复合的方式可以提高CdS的光催化性能和光稳定性。采用水热法合成了Zn掺杂CdS/g-C_(3)N_(4)复合纳米材料(Zn-CdS/g-C_(3)N_(4))。利用扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)、X射线光电子能谱(XPS)和傅里叶变换红外光谱(FT-IR)等手段对Zn-CdS/g-C_(3)N_(4)复合材料的形貌、结构和组成等进行了表征。结果表明,Zn-CdS纳米颗粒附着在g-C_(3)N_(4)表面上,从而形成Zn-CdS/g-C_(3)N_(4)复合材料,且复合后材料带隙减小,光生电子-空穴复合率降低。在500 W Xe灯照射下,研究了Zn-CdS/g-C_(3)N_(4)对罗丹明B(RhB)的光催化降解性能。在最优条件下,光照40 min后,所制备的Zn-CdS/g-C_(3)N_(4)对RhB的光催化降解效率达99%。此外,所合成的Zn-CdS/g-C_(3)N_(4)复合材料光稳定性较高、可再生性好。这归因于Zn和Cd的协同作用以及与g-C_(3)N_(4)的复合,促进了光生载流子的分离和转移。展开更多
基金support from Natural Science Foundation of Shandong Province(ZR2022MB049,ZR2021MB104)the National Natural Science Foundation of China(22078174).
文摘CdS photocatalysts have broad application prospects in environmental purification,energy conversion,and organic synthesis.However,their practical use is often hindered by the rapid recombination of photo-generated electron-hole pairs,which limits their efficiency on various reactions.Controlling morphological structures and crystal facets engineering are effective methods to enhance the photocatalytic performance of CdS.In this work,two different forms of CdS photocatalysts were synthesized by a hydrothermal method,namely nanoflower-shaped (CdS-NF) and nanorod-shaped (CdS-NR) for hydrogen peroxide (H_(2)O_(2)) production.The exposed crystal planes of CdS-NF are mainly (0 0 2) planes,while the accesible crystal planes of CdS-NR are notablly (1 0 1) planes.Notably,the photocatalytic hydrogen peroxide production yield of CdS-NR was high at 1225.13 μmol·h^(−1)·g^(−1),which is 1.78 times higher than the H_(2)O_(2) generation rate of CdS-NF.Moreover,through free radical capture experiments and DFT calculations,the reaction pathway was further explored.Both different configurations of cadmium sulfide based photocatalysts conform to the reaction mechanism of oxygen reduction as the main and water oxidation as the auxiliary.
文摘The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.
文摘在强光照射下,CdS量子点易发生光腐蚀现象,通过金属掺杂和复合的方式可以提高CdS的光催化性能和光稳定性。采用水热法合成了Zn掺杂CdS/g-C_(3)N_(4)复合纳米材料(Zn-CdS/g-C_(3)N_(4))。利用扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)、X射线光电子能谱(XPS)和傅里叶变换红外光谱(FT-IR)等手段对Zn-CdS/g-C_(3)N_(4)复合材料的形貌、结构和组成等进行了表征。结果表明,Zn-CdS纳米颗粒附着在g-C_(3)N_(4)表面上,从而形成Zn-CdS/g-C_(3)N_(4)复合材料,且复合后材料带隙减小,光生电子-空穴复合率降低。在500 W Xe灯照射下,研究了Zn-CdS/g-C_(3)N_(4)对罗丹明B(RhB)的光催化降解性能。在最优条件下,光照40 min后,所制备的Zn-CdS/g-C_(3)N_(4)对RhB的光催化降解效率达99%。此外,所合成的Zn-CdS/g-C_(3)N_(4)复合材料光稳定性较高、可再生性好。这归因于Zn和Cd的协同作用以及与g-C_(3)N_(4)的复合,促进了光生载流子的分离和转移。
