Heterojunction construction,especially S-scheme heterojunction,represents an efficient universal strategy to achieve high-performance photocatalytic materials.For further performance stimulation of these well-designed...Heterojunction construction,especially S-scheme heterojunction,represents an efficient universal strategy to achieve high-performance photocatalytic materials.For further performance stimulation of these well-designed heterojunctions,modulating the interfacial internal electric field(IEF)to steer dynamic charge transfer represents a promising approach.Herein,we realized the precise regulation of Fermi level(E_(F))of the oxidation semiconductor(mesoporous WO_(3-x))by tailoring the concentration of oxygen vacancies(V_(O)),maximizing the IEF intensity in Cs_(2)CuBr_(4)@WO_(3-x)(CCB@WO_(3-x))S-scheme heterojunction.The augmented IEF affords a robust driving force for directional electron delivery,leading to boosted charge separation.Hence,the developed CCB@WO_(3-x)S-scheme heterojunction demonstrated outstanding photocatalytic CO_(2)reduction performance,with the electron consumption rate(Relectron)up to 390.34μmol g^(-1)h^(-1),which is 3.28 folds higher than that of pure CCB.An in-depth analysis of the S-scheme electron transfer mode was presented via theoretical investigations,electron spin resonance(ESR),photo-irradiated Kelvin probe force microscopy(KPFM),and in-situ X-ray photoelectron spectroscopy(XPS).Finally,the CO_(2)photoconversion route was explored in detail using in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and DFT theoretical calculations.展开更多
采用原位水热法,将WO_(3)纳米棒负载在层状的g-C_(3)N_(4)上制备具有高吸附性和光催化活性的Z型g-C_(3)N_(4)/WO_(3)复合光催化剂。通过XRD、XPS和SEM对复合材料的形貌和结构进行了表征,并测试其光致发光光谱、光电流和紫外可见漫反射光...采用原位水热法,将WO_(3)纳米棒负载在层状的g-C_(3)N_(4)上制备具有高吸附性和光催化活性的Z型g-C_(3)N_(4)/WO_(3)复合光催化剂。通过XRD、XPS和SEM对复合材料的形貌和结构进行了表征,并测试其光致发光光谱、光电流和紫外可见漫反射光谱;考察了在可见光下g-C_(3)N_(4)/WO_(3)复合材料对土霉素的降解效果及复合材料的可重复利用性能,并结合自由基淬灭实验初步推测了g-C_(3)N_(4)/WO_(3)的光催化机理。结果表明,WO_(3)纳米棒负载到g-C_(3)N_(4)纳米片上并形成异质结;g-C_(3)N_(4)/WO_(3)异质结增强了可见光响应且降低了光生载流子复合率;添加0.6 g g-C_(3)N_(4)的g-C_(3)N_(4)/WO_(3)复合光催化剂具有最佳的光催化活性,在可见光照射下120 min对土霉素的降解率达到86%,优于单组分的g-C_(3)N_(4)和WO_(3),且稳定性较好;在g-C_(3)N_(4)/WO_(3)降解土霉素过程中,空穴(h+)为主要活性物质。展开更多
The efficient utilization of photocatalytic technology is essential for clean energy.Bismuth-based multimetal oxides(Bi_(2)WO_(6),Bi_(2)MoO_(6),BiVO_(4)and Bi_(4)Ti_(3)O_(12))have aroused widespread attention as a vis...The efficient utilization of photocatalytic technology is essential for clean energy.Bismuth-based multimetal oxides(Bi_(2)WO_(6),Bi_(2)MoO_(6),BiVO_(4)and Bi_(4)Ti_(3)O_(12))have aroused widespread attention as a visible light responsive photocatalyst for hydrogen evolution due to their low cost,nontoxicity,modifiable morphology,and outstanding optical and chemical properties.Nevertheless,the photocatalytic activities of pure materials are unsatisfactory because of their relative small specific surface area,poor quantum yield,and the rapid recombination of photogenerated carriers.Therefore,some modification strategies,including morphological control,semiconductor combination,doping,and defect engineering,have been systematically studied to enhance photocatalytic H_(2)evolution activity in the past few years.Herein,we summarize the recent research progress on bismuth-based photocatalysts,pointing out the prospects,opportunities and challenges of bismuth-based photocatalysts.Eventually,we aims to put forward valuable suggestions for designing of bismuth-based photocatalysts applied in hydrogen production on the premise of consolidating the existing theoretical basis of photocatalysis.展开更多
基金This work was financially supported by the National Natural Science Foundation of China(51972213)Natural Science Foundation of Shanghai(22ZR1460700).
文摘Heterojunction construction,especially S-scheme heterojunction,represents an efficient universal strategy to achieve high-performance photocatalytic materials.For further performance stimulation of these well-designed heterojunctions,modulating the interfacial internal electric field(IEF)to steer dynamic charge transfer represents a promising approach.Herein,we realized the precise regulation of Fermi level(E_(F))of the oxidation semiconductor(mesoporous WO_(3-x))by tailoring the concentration of oxygen vacancies(V_(O)),maximizing the IEF intensity in Cs_(2)CuBr_(4)@WO_(3-x)(CCB@WO_(3-x))S-scheme heterojunction.The augmented IEF affords a robust driving force for directional electron delivery,leading to boosted charge separation.Hence,the developed CCB@WO_(3-x)S-scheme heterojunction demonstrated outstanding photocatalytic CO_(2)reduction performance,with the electron consumption rate(Relectron)up to 390.34μmol g^(-1)h^(-1),which is 3.28 folds higher than that of pure CCB.An in-depth analysis of the S-scheme electron transfer mode was presented via theoretical investigations,electron spin resonance(ESR),photo-irradiated Kelvin probe force microscopy(KPFM),and in-situ X-ray photoelectron spectroscopy(XPS).Finally,the CO_(2)photoconversion route was explored in detail using in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and DFT theoretical calculations.
文摘采用原位水热法,将WO_(3)纳米棒负载在层状的g-C_(3)N_(4)上制备具有高吸附性和光催化活性的Z型g-C_(3)N_(4)/WO_(3)复合光催化剂。通过XRD、XPS和SEM对复合材料的形貌和结构进行了表征,并测试其光致发光光谱、光电流和紫外可见漫反射光谱;考察了在可见光下g-C_(3)N_(4)/WO_(3)复合材料对土霉素的降解效果及复合材料的可重复利用性能,并结合自由基淬灭实验初步推测了g-C_(3)N_(4)/WO_(3)的光催化机理。结果表明,WO_(3)纳米棒负载到g-C_(3)N_(4)纳米片上并形成异质结;g-C_(3)N_(4)/WO_(3)异质结增强了可见光响应且降低了光生载流子复合率;添加0.6 g g-C_(3)N_(4)的g-C_(3)N_(4)/WO_(3)复合光催化剂具有最佳的光催化活性,在可见光照射下120 min对土霉素的降解率达到86%,优于单组分的g-C_(3)N_(4)和WO_(3),且稳定性较好;在g-C_(3)N_(4)/WO_(3)降解土霉素过程中,空穴(h+)为主要活性物质。
基金This research was supported by National Natural Science Foundation of China(21706132 and 21976093)Jiangsu Provincial Specially Appointed Professors Foundation,The Startup Foundation for Introducing Talent of NUIST.
文摘The efficient utilization of photocatalytic technology is essential for clean energy.Bismuth-based multimetal oxides(Bi_(2)WO_(6),Bi_(2)MoO_(6),BiVO_(4)and Bi_(4)Ti_(3)O_(12))have aroused widespread attention as a visible light responsive photocatalyst for hydrogen evolution due to their low cost,nontoxicity,modifiable morphology,and outstanding optical and chemical properties.Nevertheless,the photocatalytic activities of pure materials are unsatisfactory because of their relative small specific surface area,poor quantum yield,and the rapid recombination of photogenerated carriers.Therefore,some modification strategies,including morphological control,semiconductor combination,doping,and defect engineering,have been systematically studied to enhance photocatalytic H_(2)evolution activity in the past few years.Herein,we summarize the recent research progress on bismuth-based photocatalysts,pointing out the prospects,opportunities and challenges of bismuth-based photocatalysts.Eventually,we aims to put forward valuable suggestions for designing of bismuth-based photocatalysts applied in hydrogen production on the premise of consolidating the existing theoretical basis of photocatalysis.
