A catalyst of ferroelectric-BaTiO_(3)@photoelectric-TiO_(2) nanohybrids(BaTiO_(3)@TiO_(2))with enhanced photocatalytic activity was synthesized via a hydrolysis precipitation combined with a hydrothermal approach.Comp...A catalyst of ferroelectric-BaTiO_(3)@photoelectric-TiO_(2) nanohybrids(BaTiO_(3)@TiO_(2))with enhanced photocatalytic activity was synthesized via a hydrolysis precipitation combined with a hydrothermal approach.Compared to pure TiO_(2),pure BaTiO_(3) and BaTiO_(3)/TiO_(2) physical mixture,the heterostructured BaTiO_(3)@TiO_(2) exhibits significantly improved photocatalytic activity and cycling stability in decomposing Rhodamine B(RhB)and the degradation efficiency is 1.7 times higher than pure TiO_(2) and 7.2 times higher than pure BaTiO_(3).These results are mainly attributed to the synergy effect of photoelectric TiO_(2),ferroelectric-BaTiO_(3) and the rationally designed interfacial structure.The mesoporous microstructure of TiO_(2) is of a high specific area and enables excellent photocatalytic activity.The ferroelectric polarization induced built-in electric field in BaTiO_(3) nanoparticles,and the intimate interfacial interactions at the interface of BaTiO_(3) and TiO_(2) are effective in driving the separation and transport of photogenerated charge carriers.This strategy will stimulate the design of heterostructured photocatalysts with outstanding photocatalytic performance via interface engineering.展开更多
Thanks to the excellent optoelectronic properties,lead halide perovskites(LHPs)have been widely employed in highperformance optoelectronic devices such as solar cells and lightemitting diodes.However,overcoming their ...Thanks to the excellent optoelectronic properties,lead halide perovskites(LHPs)have been widely employed in highperformance optoelectronic devices such as solar cells and lightemitting diodes.However,overcoming their poor stability against water has been one of the biggest challenges for most applications.Herein,we report a novel hot-injection method in a Pb-poor environment combined with a well-designed purification process to synthesize water-dispersible CsPbBr_(3) nanocrystals(NCs).The as-prepared NCs sustain their superior photoluminescence(91%quantum yield in water)for more than 200 days in an aqueous environment,which is attributed to a passivation effect induced by excess CsBr salts.Thanks to the ultra-stability of these LHP NCs,for the first time,we report a new application of LHP NCs,in which they are applied to electrocatalysis of CO_(2) reduction reaction.Noticeably,they show significant electrocatalytic activity(faradaic yield:32%for CH4,40%for CO)and operation stability(>350 h).展开更多
AgCl/Ti_(3)C_(2)@TiO_(2)ternary composites were prepared to form a heterojunction structure between AgCl and TiO_(2)and introduce Ti3C2 as a cocatalyst.The as-prepared AgCl/Ti_(3)C_(2)@TiO_(2)composites showed higher ...AgCl/Ti_(3)C_(2)@TiO_(2)ternary composites were prepared to form a heterojunction structure between AgCl and TiO_(2)and introduce Ti3C2 as a cocatalyst.The as-prepared AgCl/Ti_(3)C_(2)@TiO_(2)composites showed higher photocatalytic activity than pure AgCl and Ti_(3)C_(2)@TiO_(2)for photooxidation of a 1,4-dihydropyridine derivative(1,4-DHP)and tetracycline hydrochloride(TCH)under visible light irradiation(λ>400 nm).The photocatalytic activity of AgCl/Ti_(3)C_(2)@TiO_(2)composites depended on Ti_(3)C_(2)@TiO_(2)content,and the catalytic activity of the optimized samples were 6.9 times higher than that of pure AgCl for 1,4-DHP photodehydrogenation and 7.3 times higher than that of Ti_(3)C_(2)@TiO_(2)for TCH photooxidation.The increased photocatalytic activity was due to the formation of a heterojunction structure between AgCl and TiO_(2)and the introduction of Ti3C2 as a cocatalyst,which lowered the internal resistance,sped up the charge transfer,and increased the separation efficiency of photogenerated carries.Photogenerated holes and superoxide radical anions were the major active species in the photocatalytic process.展开更多
The construction of stable and efficient materials that emit blue and green light remains a challenge.Among the blue light materials reported,metal-organic framework(MOF)materials are rarely reported as blue phosphors...The construction of stable and efficient materials that emit blue and green light remains a challenge.Among the blue light materials reported,metal-organic framework(MOF)materials are rarely reported as blue phosphors due to their weak luminescence intensity.Based on the construction of CsPbBr_(3)@MOF(CPB@MOF),an innovative idea was proposed to simultaneously enhance the green luminescence of CPB and the blue luminescence of MOF through the interaction between CPB and MOF for the first time.As expected,the blue luminescence from CPB:7%SCN−@0.5%MOF:Eu as well as the green luminescence from 5%CPB:7%SCN−@MOF:Eu was sufficient to construct high-performance light-emitting diode(LED)devices and further excite solar cells to generate stable photoelectric signals.The white LED(WLED)device with excellent color quality(color rendering index(CRI)=96.2)and correlated color temperature(CCT=9688 K)can be constructed by using the obtained blue-emitting CPB:7%SCN-@0.5%MOF:Eu,green-emitting 5%CPB:7%SCN−@MOF:Eu,and red-emitting PPB:30%Mn^(2+).The density functional theory(DFT)theoretical calculation results indicate that the p orbital of Pb plays the major role in the conduction band,and the p orbital of Br plays the major role in the valance band of CPB and CPB:SCN−.While the p orbital of O plays the major role in both the conduction band and valance band of MOF.The heat capacity of CPB and CPB:SCN−separately reaches the Dulong–Petit limit at 200 and 400 K,indicating that the thermal stability of CsPbBr_(3)increases after SCN−doping.展开更多
Halide perovskite nanocrystals are potential catalysts for CO_(2) photoreduction,while,the strong radiative recombination and insufficient stability limit their catalytic performance and application.Herein,we report t...Halide perovskite nanocrystals are potential catalysts for CO_(2) photoreduction,while,the strong radiative recombination and insufficient stability limit their catalytic performance and application.Herein,we report that layered double hydroxide nanosheets activate CsPbBr_(3) nanocrystals(CLDH)for enhanced photocatalytic CO_(2) reduction.These CLDH heterojunctions show the remarkably enhanced CO_(2) photoreduction performance;without cocatalyst and sacrificial agent,the average electron consumption rate of CLDH(49.16μmol·g^(−1)·h^(−1))is approximately 3.7 times higher than that of pristine CsPbBr_(3).Also,CLDH catalyst exhibits a robust stability after ten cycles over 30 h.展开更多
Tuning the photoresponse of monolayer MoS_(2) could extend its potential application in many fields,however,it is still a challenge.In this study,CsPbBr_(3) nanoparticles were prepared and spin-coated on the surface o...Tuning the photoresponse of monolayer MoS_(2) could extend its potential application in many fields,however,it is still a challenge.In this study,CsPbBr_(3) nanoparticles were prepared and spin-coated on the surface of monolayer MoS_(2) to fabricate hybrid CsPbBr_(3)/MoS_(2) photodetectors.By combing the photoelectrical property of the CsPbBr_(3),the synergistic effect has been systematically studied from its carrier mobility,photoresponse and detectivity.It was found that nanofilm-coating of CsPbBr_(3)would impede the photoelectric performance due to the electron-hole recombination facilitated by the defects at the interface of C PbBr_(3) and MoS_(2) films.While the nanoparticles decorating was observed to significantly improve the conductivity of the monolayer Mo S_(2),which also increased the on/off ratio of the MoS_(2) transistor from 8.2×10~3 to 4.4×10^(4),and enhanced the carrier mobility from 0.090 cm^(2)V^(-1)s^(-1)to 0.202 cm^(2)V^(-1)s^(-1),ascribing to a mixed electron recombination-injection process.Furthermore,the CsPbBr_(3) nanofilm would decrease the responsivity to 136 and 178 A/W under the light wavelength of 400 and 500 nm,respectively,while decorating CsPbBr_(3) nanoparticles improve the photoresponse to 948 and 883 A/W with the detectivity at the level of 10^(11)Jones.This work may provide an easy and cost-efficient way to tune the photoresponse of MoS_(2) photodetectors.展开更多
Owing to their outstanding optoelectronic properties,all-inorganic CsPbBr_(3) perovskite nanocrystals(NCs)are regarded as excellent materials for various optoelectronic applications.Unfortunately,their practical appli...Owing to their outstanding optoelectronic properties,all-inorganic CsPbBr_(3) perovskite nanocrystals(NCs)are regarded as excellent materials for various optoelectronic applications.Unfortunately,their practical applications are limited by poor stability against water,heat,and polar solvents.Here,we propose a facile synthesis strategy for CsPbBr_(3)@Cs_(4)PbBr_(6) NCs via tetraoctylammonium bromide ligand induction at room temperature.The resulting CsPbBr_(3)@Cs_(4)PbBr_(6) NCs show a high photoluminescence quantum yield of 94%.In order to prevent Cs4PbBr6 from being converted back to CsPbBr_(3) NCs when exposed to water,a second coating layer of SiO2 is formed on the surface of the CsPbBr_(3)@Cs_(4)PbBr_(6) NCs by the facile hydrolysis of tetramethoxysilane.The resulting CsPbBr_(3)@Cs_(4)PbBr_(6)/SiO_(2) NCs with their double coating structure have outstanding stability against not only a polar solvent(ethanol)but also water and heat.The as-prepared CsPbBr_(3)@Cs_(4)PbBr_(6)/SiO_(2) NCs serve as green emitters in efficient white light-emitting diodes(WLEDs)with a high color rendering index(CRI)of 91 and a high power efficiency 59.87 lm W−1.Furthermore,the use of these WLEDs in visible light communication(VLC)results in a maximum rate of 44.53 Mbps,suggesting the great potential of the reported methods and materials for solid-state illumination and VLC.展开更多
文摘通过CdBr_(2)对全无机CsPbBr_(3)钙钛矿薄膜进行钝化处理,研究不同浓度CdBr_(2)的异丙醇溶液对全无机CsPbBr_(3)钙钛矿太阳能电池光电性能的影响.结果表明:CdBr_(2)钝化CsPbBr_(3)钙钛矿表面后,降低了钙钛矿表面的Br空位缺陷密度,抑制了非辐射复合,促进了光生电子和空穴的抽取和传输,因此降低了界面光电子复合损失,使全无机钙钛矿太阳能电池器件的光电转换效率从6.58%提高到8.19%,开路电压从1.368 V提高到1.531 V.
基金Project(cstc2020jcyj-msxm X0930) supported by the Natural Science Foundation of Chongqing,ChinaProject(KJQN201901522) supported by Technological Research Program of Chongqing Municipal Education Commission,ChinaProject(cx2020068) supported by the Venture&Innovation Support Program for Chongqing Overseas Returnees,China。
文摘A catalyst of ferroelectric-BaTiO_(3)@photoelectric-TiO_(2) nanohybrids(BaTiO_(3)@TiO_(2))with enhanced photocatalytic activity was synthesized via a hydrolysis precipitation combined with a hydrothermal approach.Compared to pure TiO_(2),pure BaTiO_(3) and BaTiO_(3)/TiO_(2) physical mixture,the heterostructured BaTiO_(3)@TiO_(2) exhibits significantly improved photocatalytic activity and cycling stability in decomposing Rhodamine B(RhB)and the degradation efficiency is 1.7 times higher than pure TiO_(2) and 7.2 times higher than pure BaTiO_(3).These results are mainly attributed to the synergy effect of photoelectric TiO_(2),ferroelectric-BaTiO_(3) and the rationally designed interfacial structure.The mesoporous microstructure of TiO_(2) is of a high specific area and enables excellent photocatalytic activity.The ferroelectric polarization induced built-in electric field in BaTiO_(3) nanoparticles,and the intimate interfacial interactions at the interface of BaTiO_(3) and TiO_(2) are effective in driving the separation and transport of photogenerated charge carriers.This strategy will stimulate the design of heterostructured photocatalysts with outstanding photocatalytic performance via interface engineering.
基金This research was supported by the National Natural Science Foundation of China(Nos.11674258,51602305,51702219,61975134,11904250)Guangdong Basic and Applied Basic Research Foundation(2020B1515020051)+2 种基金the Science and Technology Innovation Commission of Shenzhen(JCYJ20180305125345378)Shenzhen Nanshan District Pilotage Team Program(LHTD20170006)Partial support from The Institute For Lasers,Photonics and Biophotonics at The University at Buffalo is also acknowledged.T.Z.and I.Z.were supported by the U.S.DOE,Office of Science BES,Award No.DE-SC0004890.
文摘Thanks to the excellent optoelectronic properties,lead halide perovskites(LHPs)have been widely employed in highperformance optoelectronic devices such as solar cells and lightemitting diodes.However,overcoming their poor stability against water has been one of the biggest challenges for most applications.Herein,we report a novel hot-injection method in a Pb-poor environment combined with a well-designed purification process to synthesize water-dispersible CsPbBr_(3) nanocrystals(NCs).The as-prepared NCs sustain their superior photoluminescence(91%quantum yield in water)for more than 200 days in an aqueous environment,which is attributed to a passivation effect induced by excess CsBr salts.Thanks to the ultra-stability of these LHP NCs,for the first time,we report a new application of LHP NCs,in which they are applied to electrocatalysis of CO_(2) reduction reaction.Noticeably,they show significant electrocatalytic activity(faradaic yield:32%for CH4,40%for CO)and operation stability(>350 h).
基金This work was supported by the Opening Project of the Key Laboratory of Green Chemistry of Sichuan Institutes of Higher Education(LZJ2002)the Open Project of Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province(CSPC2016-3-2).
文摘AgCl/Ti_(3)C_(2)@TiO_(2)ternary composites were prepared to form a heterojunction structure between AgCl and TiO_(2)and introduce Ti3C2 as a cocatalyst.The as-prepared AgCl/Ti_(3)C_(2)@TiO_(2)composites showed higher photocatalytic activity than pure AgCl and Ti_(3)C_(2)@TiO_(2)for photooxidation of a 1,4-dihydropyridine derivative(1,4-DHP)and tetracycline hydrochloride(TCH)under visible light irradiation(λ>400 nm).The photocatalytic activity of AgCl/Ti_(3)C_(2)@TiO_(2)composites depended on Ti_(3)C_(2)@TiO_(2)content,and the catalytic activity of the optimized samples were 6.9 times higher than that of pure AgCl for 1,4-DHP photodehydrogenation and 7.3 times higher than that of Ti_(3)C_(2)@TiO_(2)for TCH photooxidation.The increased photocatalytic activity was due to the formation of a heterojunction structure between AgCl and TiO_(2)and the introduction of Ti3C2 as a cocatalyst,which lowered the internal resistance,sped up the charge transfer,and increased the separation efficiency of photogenerated carries.Photogenerated holes and superoxide radical anions were the major active species in the photocatalytic process.
基金supported by the National Natural Science Foundation of China(No.22271080)the Joint Guidance Project of Heilongjiang Natural Science Foundation(No.LH2023B020).
文摘The construction of stable and efficient materials that emit blue and green light remains a challenge.Among the blue light materials reported,metal-organic framework(MOF)materials are rarely reported as blue phosphors due to their weak luminescence intensity.Based on the construction of CsPbBr_(3)@MOF(CPB@MOF),an innovative idea was proposed to simultaneously enhance the green luminescence of CPB and the blue luminescence of MOF through the interaction between CPB and MOF for the first time.As expected,the blue luminescence from CPB:7%SCN−@0.5%MOF:Eu as well as the green luminescence from 5%CPB:7%SCN−@MOF:Eu was sufficient to construct high-performance light-emitting diode(LED)devices and further excite solar cells to generate stable photoelectric signals.The white LED(WLED)device with excellent color quality(color rendering index(CRI)=96.2)and correlated color temperature(CCT=9688 K)can be constructed by using the obtained blue-emitting CPB:7%SCN-@0.5%MOF:Eu,green-emitting 5%CPB:7%SCN−@MOF:Eu,and red-emitting PPB:30%Mn^(2+).The density functional theory(DFT)theoretical calculation results indicate that the p orbital of Pb plays the major role in the conduction band,and the p orbital of Br plays the major role in the valance band of CPB and CPB:SCN−.While the p orbital of O plays the major role in both the conduction band and valance band of MOF.The heat capacity of CPB and CPB:SCN−separately reaches the Dulong–Petit limit at 200 and 400 K,indicating that the thermal stability of CsPbBr_(3)increases after SCN−doping.
基金supported by National Key Basic Research Program of China(Nos.2020YFA0406104 and 2020YFA0406101)National MCF Energy R&D Program(No.2018YFE0306105)+5 种基金Innovative Research Group Project of the National Natural Science Foundation of China(No.51821002)National Natural Science Foundation of China(Nos.51725204,21771132,21471106,and 51972216)Natural Science Foundation of Jiangsu Province(No.BK20190041)Natural Science Foundation of Jiangsu Province-Excellent Youth Foundation(No.BK20190102)Key-Area Research and Development Program of GuangDong Province(No.2019B010933001)Collaborative Innovation Center of Suzhou Nano Science&Technology,the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD),the 111 Project,and Suzhou Key Laboratory of Functional Nano&Soft Materials.
文摘Halide perovskite nanocrystals are potential catalysts for CO_(2) photoreduction,while,the strong radiative recombination and insufficient stability limit their catalytic performance and application.Herein,we report that layered double hydroxide nanosheets activate CsPbBr_(3) nanocrystals(CLDH)for enhanced photocatalytic CO_(2) reduction.These CLDH heterojunctions show the remarkably enhanced CO_(2) photoreduction performance;without cocatalyst and sacrificial agent,the average electron consumption rate of CLDH(49.16μmol·g^(−1)·h^(−1))is approximately 3.7 times higher than that of pristine CsPbBr_(3).Also,CLDH catalyst exhibits a robust stability after ten cycles over 30 h.
基金financially supported by the National Natural Science Foundation of China (Nos. 52002254, 52272160)Sichuan Science and Technology Foundation (Nos. 2020YJ0262, 2021YFH0127, 2022YFH0083, 2022YFSY0045)+2 种基金the Chunhui plan of Ministry of Education, Fundamental Research Funds for the Central Universities, China (No. YJ201893)the Open-Foundation of Key Laboratory of Laser Device Technology, China North Industries Group Corporation Limited (No. KLLDT202104)Supported by the fund of the State Key Laboratory of Solidification Processing in NWPU (No. SKLSP202210)。
文摘Tuning the photoresponse of monolayer MoS_(2) could extend its potential application in many fields,however,it is still a challenge.In this study,CsPbBr_(3) nanoparticles were prepared and spin-coated on the surface of monolayer MoS_(2) to fabricate hybrid CsPbBr_(3)/MoS_(2) photodetectors.By combing the photoelectrical property of the CsPbBr_(3),the synergistic effect has been systematically studied from its carrier mobility,photoresponse and detectivity.It was found that nanofilm-coating of CsPbBr_(3)would impede the photoelectric performance due to the electron-hole recombination facilitated by the defects at the interface of C PbBr_(3) and MoS_(2) films.While the nanoparticles decorating was observed to significantly improve the conductivity of the monolayer Mo S_(2),which also increased the on/off ratio of the MoS_(2) transistor from 8.2×10~3 to 4.4×10^(4),and enhanced the carrier mobility from 0.090 cm^(2)V^(-1)s^(-1)to 0.202 cm^(2)V^(-1)s^(-1),ascribing to a mixed electron recombination-injection process.Furthermore,the CsPbBr_(3) nanofilm would decrease the responsivity to 136 and 178 A/W under the light wavelength of 400 and 500 nm,respectively,while decorating CsPbBr_(3) nanoparticles improve the photoresponse to 948 and 883 A/W with the detectivity at the level of 10^(11)Jones.This work may provide an easy and cost-efficient way to tune the photoresponse of MoS_(2) photodetectors.
基金National Natural Science Foundation of China(11974063,61904023)Key Program Science Foundation of Natural Science Foundation of Chongqing(cstc2020jcyj-jqX0028)Chongqing Special Postdoctoral Science Foundation(cstc2019jcyj-54bsh0026).
文摘Owing to their outstanding optoelectronic properties,all-inorganic CsPbBr_(3) perovskite nanocrystals(NCs)are regarded as excellent materials for various optoelectronic applications.Unfortunately,their practical applications are limited by poor stability against water,heat,and polar solvents.Here,we propose a facile synthesis strategy for CsPbBr_(3)@Cs_(4)PbBr_(6) NCs via tetraoctylammonium bromide ligand induction at room temperature.The resulting CsPbBr_(3)@Cs_(4)PbBr_(6) NCs show a high photoluminescence quantum yield of 94%.In order to prevent Cs4PbBr6 from being converted back to CsPbBr_(3) NCs when exposed to water,a second coating layer of SiO2 is formed on the surface of the CsPbBr_(3)@Cs_(4)PbBr_(6) NCs by the facile hydrolysis of tetramethoxysilane.The resulting CsPbBr_(3)@Cs_(4)PbBr_(6)/SiO_(2) NCs with their double coating structure have outstanding stability against not only a polar solvent(ethanol)but also water and heat.The as-prepared CsPbBr_(3)@Cs_(4)PbBr_(6)/SiO_(2) NCs serve as green emitters in efficient white light-emitting diodes(WLEDs)with a high color rendering index(CRI)of 91 and a high power efficiency 59.87 lm W−1.Furthermore,the use of these WLEDs in visible light communication(VLC)results in a maximum rate of 44.53 Mbps,suggesting the great potential of the reported methods and materials for solid-state illumination and VLC.
