Lead halide perovskite (LHP) nanocrystals have been intensely studied as photocatalysts for artificial photosynthesis in recent years.However,the toxicity of lead in LHP seriously limits their potential for widespread...Lead halide perovskite (LHP) nanocrystals have been intensely studied as photocatalysts for artificial photosynthesis in recent years.However,the toxicity of lead in LHP seriously limits their potential for widespread applications.Herein,we first present the synthesis of 2D lead-free halide perovskite (Cs_(3)Bi_(2)I_(9)) nanosheets with self-template-oriented method,in which BiOI/Bi_(2)O_(2) nanosheets were used as the template and Bi ion source simultaneously.Through facile electrostatic self-assembly strategy,a Z-scheme heterojunction composed of Cs_(3)Bi_(2)I_(9)nanosheets and CeO_(2) nanosheets (Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1) was constructed as photocatalyst for the photo-reduction of CO_(2) coupled with the oxidation of H_(2)O.Due to the matching energy levels and the close interfacial contact between Cs_(3)Bi_(2)I_(9)and CeO_(2) nanosheets,the separation efficiency of the photogenerated carriers in Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1 composite was significantly improved.Consequently,the environment-friendly halide perovskite heterojunction Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1presents impressive photocatalytic activity for the reduction of CO_(2)to CH_(4)and CO with an electron consumption yield of 877.04μmol g^(-1),which is over 7 and 15 times higher than those of pristine Cs_(3)Bi_(2)I_(9)and CeO_(2)nanosheets,exceeding the yield of other reported bismuth-based perovskite for photocatalytic CO_(2)reduction.展开更多
Defect and charge transfer efficiency of nano-photocatalysts are important factors which influence their photocatalytic performance.In this work,oxygen vacancies are successfully introduced in the synthesis process of...Defect and charge transfer efficiency of nano-photocatalysts are important factors which influence their photocatalytic performance.In this work,oxygen vacancies are successfully introduced in the synthesis process of Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterojunctions through one-step in situ selfcombustion method.High-resolution transmission electron microscopy (HRTEM),UV-Vis diffuse reflectance spectra (UV-Vis DRS),and electron spin resonance (ESR) measurements confirm the existence of oxygen vacancies.In addition,by controlling the ratio of reactants of Bi(NO_(3))_(3)to Al(NO_(3))_(3),the ratio of Bi_(2)Al_(4)O_(9)and β-Bi_(2)O_(3)in the heterojunction can be easily adjusted.Photocurrent responses and surface photovoltage spectroscopy (SPV) indicate that the construction of the Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterostructure improves the separation efficiency of the photo-generated electrons and holes.CO_(2)-TPD results imply that the amounts and stability of heterojunctions are enhanced compared with their counterparts.The Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterojunction with 14 mol%Bi_(2)Al_(4)O_(9)shows the highest photocatalytic ability for reduction of CO_(2)into CO.The enhanced photoreduction of CO_(2)performance can be ascribed to the synergistic effects of the heterojunction for electron separation and oxygen vacancies for CO_(2)activation.展开更多
A self-powered solar-blind ultraviolet(UV)photodetector(PD)was successfully constructed on a Ga_(2)O_(3)/Bi_(2)WO_(6)heterojunction,which was fabricated by spin-coating the hydrothermally grown Bi_(2)WO_(6)onto MOCVD-...A self-powered solar-blind ultraviolet(UV)photodetector(PD)was successfully constructed on a Ga_(2)O_(3)/Bi_(2)WO_(6)heterojunction,which was fabricated by spin-coating the hydrothermally grown Bi_(2)WO_(6)onto MOCVD-grown Ga_(2)O_(3)film.The results show that a typical type-I heterojunction is formed at the interface of the Ga_(2)O_(3)film and clustered Bi_(2)WO_(6),which demonstrates a distinct photovoltaic effect with an open-circuit voltage of 0.18 V under the irradiation of 254 nm UV light.Moreover,the Ga_(2)O_(3)/Bi_(2)WO_(6)PD displays excellent photodetection performance with an ultra-low dark current of~6 fA,and a high light-to-dark current ratio(PDCR)of 3.5 x 10^(4)in self-powered mode(0 V),as well as a best responsivity result of 2.21 mA/W in power supply mode(5 V).Furthermore,the PD possesses a stable and fast response speed under different light intensities and voltages.At zero voltage,the PD exhibits a fast rise time of 132 ms and 162 ms,as well as a quick decay time of 69 ms and 522 ms,respectively.In general,the newly attempted Ga_(2)O_(3)/Bi_(2)WO_(6)heterojunction may become a potential candidate for the realization of self-powered and high-performance UV photodetectors.展开更多
The development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(...The development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In_(2.77)S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2) production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In_(2.77)S_(4)/respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In_(2.77)S_(4) according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2) production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2) around the active centers,the energy barriers of O_(2) protonation and H_(2)O_(2) desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2) photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.展开更多
基金financially supported by the Natural Science Foundation of Tianjin City (17JCJQJC43800, 19JCQNJC05500)the National Key R&D Program of China (2017YFA0700104)+1 种基金NSFC (21931007)the 111 Project of China (D17003)。
文摘Lead halide perovskite (LHP) nanocrystals have been intensely studied as photocatalysts for artificial photosynthesis in recent years.However,the toxicity of lead in LHP seriously limits their potential for widespread applications.Herein,we first present the synthesis of 2D lead-free halide perovskite (Cs_(3)Bi_(2)I_(9)) nanosheets with self-template-oriented method,in which BiOI/Bi_(2)O_(2) nanosheets were used as the template and Bi ion source simultaneously.Through facile electrostatic self-assembly strategy,a Z-scheme heterojunction composed of Cs_(3)Bi_(2)I_(9)nanosheets and CeO_(2) nanosheets (Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1) was constructed as photocatalyst for the photo-reduction of CO_(2) coupled with the oxidation of H_(2)O.Due to the matching energy levels and the close interfacial contact between Cs_(3)Bi_(2)I_(9)and CeO_(2) nanosheets,the separation efficiency of the photogenerated carriers in Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1 composite was significantly improved.Consequently,the environment-friendly halide perovskite heterojunction Cs_(3)Bi_(2)I_(9)/CeO_(2)-3:1presents impressive photocatalytic activity for the reduction of CO_(2)to CH_(4)and CO with an electron consumption yield of 877.04μmol g^(-1),which is over 7 and 15 times higher than those of pristine Cs_(3)Bi_(2)I_(9)and CeO_(2)nanosheets,exceeding the yield of other reported bismuth-based perovskite for photocatalytic CO_(2)reduction.
基金financial support from the National Natural Science Foundation of China(21776059,21376061)the Natural Science Foundation for Distinguished Young Scholars of Hebei Province(B2015208010)the Research Foundation of Hebei Province Education Department(No.ZC2016007)。
文摘Defect and charge transfer efficiency of nano-photocatalysts are important factors which influence their photocatalytic performance.In this work,oxygen vacancies are successfully introduced in the synthesis process of Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterojunctions through one-step in situ selfcombustion method.High-resolution transmission electron microscopy (HRTEM),UV-Vis diffuse reflectance spectra (UV-Vis DRS),and electron spin resonance (ESR) measurements confirm the existence of oxygen vacancies.In addition,by controlling the ratio of reactants of Bi(NO_(3))_(3)to Al(NO_(3))_(3),the ratio of Bi_(2)Al_(4)O_(9)and β-Bi_(2)O_(3)in the heterojunction can be easily adjusted.Photocurrent responses and surface photovoltage spectroscopy (SPV) indicate that the construction of the Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterostructure improves the separation efficiency of the photo-generated electrons and holes.CO_(2)-TPD results imply that the amounts and stability of heterojunctions are enhanced compared with their counterparts.The Bi_(2)Al_(4)O_(9)/β-Bi_(2)O_(3)heterojunction with 14 mol%Bi_(2)Al_(4)O_(9)shows the highest photocatalytic ability for reduction of CO_(2)into CO.The enhanced photoreduction of CO_(2)performance can be ascribed to the synergistic effects of the heterojunction for electron separation and oxygen vacancies for CO_(2)activation.
基金Project supported by the National Key Research and Development Program of China(Grant No.2022YFB3605404)Natural Science Research Start up Foundation of Recruiting Talents of Nanjing University of Posts and Telecommunications(Grant Nos.XK1060921119,XK1060921115,and XK1060921002)+1 种基金National Natural Science Foundation of China(Grant No.62204125)China Postdoctoral Science Foundation(Grant No.2022M721689)。
文摘A self-powered solar-blind ultraviolet(UV)photodetector(PD)was successfully constructed on a Ga_(2)O_(3)/Bi_(2)WO_(6)heterojunction,which was fabricated by spin-coating the hydrothermally grown Bi_(2)WO_(6)onto MOCVD-grown Ga_(2)O_(3)film.The results show that a typical type-I heterojunction is formed at the interface of the Ga_(2)O_(3)film and clustered Bi_(2)WO_(6),which demonstrates a distinct photovoltaic effect with an open-circuit voltage of 0.18 V under the irradiation of 254 nm UV light.Moreover,the Ga_(2)O_(3)/Bi_(2)WO_(6)PD displays excellent photodetection performance with an ultra-low dark current of~6 fA,and a high light-to-dark current ratio(PDCR)of 3.5 x 10^(4)in self-powered mode(0 V),as well as a best responsivity result of 2.21 mA/W in power supply mode(5 V).Furthermore,the PD possesses a stable and fast response speed under different light intensities and voltages.At zero voltage,the PD exhibits a fast rise time of 132 ms and 162 ms,as well as a quick decay time of 69 ms and 522 ms,respectively.In general,the newly attempted Ga_(2)O_(3)/Bi_(2)WO_(6)heterojunction may become a potential candidate for the realization of self-powered and high-performance UV photodetectors.
文摘The development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In_(2.77)S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2) production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In_(2.77)S_(4)/respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In_(2.77)S_(4) according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2) production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2) around the active centers,the energy barriers of O_(2) protonation and H_(2)O_(2) desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2) photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.
