The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to C...The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to CO using ultrathin Bi_(12)O_(17)Cl_(2)nanosheets decorated with hydrothermally synthesized bismuth clusters and oxygen vacancies(OVs).The characterizations revealed that the coexistences of OVs and Bi clusters generated in situ contributed to the high efficiency of CO_(2)–CO conversion(64.3μmol g^(−1)h^(−1))and perfect selectivity.The OVs on the facet(001)of the ultrathin Bi_(12)O_(17)Cl_(2)nanosheets serve as sites for CO_(2)adsorption and activation sites,capturing photoexcited electrons and prolonging light absorption due to defect states.In addition,the Bi‐cluster generated in situ offers the ability to trap holes and the surface plasmonic resonance effect.This study offers great potential for the construction of semiconductor hybrids as multiphotocatalysts,capable of being used for the elimination and conversion of CO_(2)in terms of energy and environment.展开更多
The insufficient active sites and slow interfacial charge trans-fer of photocatalysts restrict the efficiency of CO_(2) photoreduction.The synchronized modulation of the above key issues is demanding and chal-lenging....The insufficient active sites and slow interfacial charge trans-fer of photocatalysts restrict the efficiency of CO_(2) photoreduction.The synchronized modulation of the above key issues is demanding and chal-lenging.Herein,strain-induced strategy is developed to construct the Bi–O-bonded interface in Cu porphyrin-based monoatomic layer(PML-Cu)and Bi_(12)O_(17)Br_(2)(BOB),which triggers the surface interface dual polarization of PML-Cu/BOB(PBOB).In this multi-step polarization,the built-in electric field formed between the interfaces induces the electron transfer from con-duction band(CB)of BOB to CB of PML-Cu and suppresses its reverse migration.Moreover,the surface polarization of PML-Cu further promotes the electron converge in Cu atoms.The introduction of PML-Cu endows a high density of dispersed Cu active sites on the surface of PBOB,significantly promoting the adsorption and activation of CO_(2) and CO desorption.The conversion rate of CO_(2) photoreduction to CO for PBOB can reach 584.3μmol g-1,which is 7.83 times higher than BOB and 20.01 times than PML-Cu.This work offers valuable insights into multi-step polarization regulation and active site design for catalysts.展开更多
The construction and application of novel highly efficient photocatalysts have been the focus in the field of environmental pollutant removal.In this work,a novel CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)photocatalysts were s...The construction and application of novel highly efficient photocatalysts have been the focus in the field of environmental pollutant removal.In this work,a novel CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)photocatalysts were synthesized by simple hydrothermal and chemical precipitation method.The fabricated CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)composite exhibited much higher photocatalytic activity than pristine CuFe_(2)O_(4)and Bi_(12)O_(17)Cl_(2)in the removal of bisphenol A(BPA)under visible-light illumination,which ascribed to the intrinsic p-n junction of CuFe_(2)O_(4)and Bi_(12)O_(17)Cl_(2).The photocatalytic degradation rate of BPA on CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)with an optimized CuFe_(2)O_(4)content(1.0 wt.%)reached 93.0%within 30 min.The capture experiments of active species confirmed that the hydroxyl radicals(·OH)and superoxide radicals(·O_(2)^(-))played crucial roles in photocatalytic BPA degradation process.Furthermore,the possible degradation mechanism and pathways of BPA was proposed according to the detected intermediates in photocatalytic reaction process.展开更多
Increasing the utilization efficiency of photogenerated electrons is highly recognized as one of the ef-ficient approaches to boost the photocatalytic CO_(2)conversion efficiency.Herein,ZIF-67-derived porous carbon(PC...Increasing the utilization efficiency of photogenerated electrons is highly recognized as one of the ef-ficient approaches to boost the photocatalytic CO_(2)conversion efficiency.Herein,ZIF-67-derived porous carbon(PC)material was employed for the construction of PC@ultrafine Bi_(12)O_(17)Br_(2)nanotubes(PC@BOB NTs)composites through a facile solvothermal synthesis in order to optimize the use of excited elec-trons in the BOB NTs.Photoelectrochemical characterization results revealed that the introduction of PC material achieved a faster charge separation rate in the PC@BOB composites,ensuring more photogener-ated electrons participate in the CO_(2)adsorption and activation process.Moreover,the pore structures of ZIF-67-derived PC material provided abundant confined spaces for the enrichment of CO_(2)molecules.Af-ter 5 h of Xenon lamp irradiation,PC@BOB composites exhibited obviously increased photocatalytic CO_(2)reduction activity in the pure water.When the addition amount of PC was 5 wt%,the PC@BOB-2 com-posite showed the highest CO evolution rate of 359.70μmol/g,which was 2.95 times higher than that of the pure BOB NTs.This work provides some independent insights into the applications of Metal-Organic Framework(MOF)-derived hierarchical porous structures to strengthen the CO_(2)enrichment,as well as the excited charge utilization efficiency,thus achieving a high solar-to-fuel conversion efficiency.展开更多
The development of a high-performance ferroelectric piezo-photocatalyst is an efficient strategy for advancing sustainability within the environmental and energy sectors.Yet,a major challenge lies in the creation of a...The development of a high-performance ferroelectric piezo-photocatalyst is an efficient strategy for advancing sustainability within the environmental and energy sectors.Yet,a major challenge lies in the creation of a strong polarized electric field that can effectively hinder charge recombination,both within the bulk and on the surface of catalysts.Herein,we synthesize a series of Nb-doped Bi_(4)Ti_(3)O_(12)nanosheets via a facile one-pot hydrothermal method to achieve synergistically enhanced piezo-photocatalytic performance in CO_(2)reduction and pollutant degradation.The optimized doped Bi_(4)Ti_(3)O_(12)demonstrates remarkable efficiency in the conversion of CO_(2)into CO,with a high production rate of 72.7μmol∙g−1∙h−1 without using co-catalysts or any sacrificial agent,surpassing the performance of unmodified Bi_(4)Ti_(3)O_(12)by up to 4.69 folds.Additionally,our catalyst demonstrates ultra-fast piezo-photocatalytic degradation of organic pollutant Rhodamine B(RhB)at low concentrations and exceptional piezo-photocatalytic activity at high concentrations,outperforming most previously reported state-of-the-art catalysts.The systematic corroboration of catalyst characterization and experimental analysis reveals that the synergistic effect arises from the amplified macroscopic polarization induced by lattice distortion caused by the larger Nb ions,thereby improving piezo-photocatalytic efficiency.This research thus offers valuable insights into the direct design and fabrication of versatile catalytic systems,with applications spanning CO_(2)valorization and beyond.展开更多
Bismuth titanate (Bi_(4)Ti_(3)O_(12),BIT)piezoelectric materials have attracted increasing attention due to their high-temperature applications.However,it is quite challenging to simultaneously achieve outstanding pie...Bismuth titanate (Bi_(4)Ti_(3)O_(12),BIT)piezoelectric materials have attracted increasing attention due to their high-temperature applications.However,it is quite challenging to simultaneously achieve outstanding piezoelectric properties and high Curie temperature in BIT-based systems.In this study,oxygen vacancy defects tailoring strategy was utilized to solve this problem,excellent piezoelectric coefficient(32.1 pC/N),and ultrahigh Curie temperature(659℃)are gotten in Bi_(4)Ti_(3)-x(Mn_(1/3)Nb_(2/3))xO_(12)(BTMN)ceramics,which are among the top values in the BIT-based ceramics.More importantly,the(Mn_(1/3)Nb_(2/3))(4+d)+complex-ion modified Bi_(4)Ti_(3)O_(12)-based ceramics are characterized with excellent piezoelectric stability up to 500℃(d33>30.0 pC/N at 500℃))and significantly reduced conductivity(only~10^(-7)U-1 cm^(-1)at 500℃).Moreover,enhanced ferroelectricity and good dielectric stability were also obtained.The better comprehensive properties can be ascribed to two aspects.First,the concentration of oxygen vacancy defects is obviously reduced,and their distribution is effectively controlled in BITMN ceramics.Second,the introduction of(Mn_(1/3)Nb_(2/3))^((4+δ)+)complex-ion gives rise to the antiphase boundaries and massive ferroelectric domain walls.This works not only reveal the high potential of BITMN ceramics for high-temperature piezoelectric applications but also deepen the understanding of the structure-properties relationship in BIT-based materials.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Natural Science Foundation of Shandong Province,Grant/Award Number:ZR2022MB106national training program of innovation and entrepreneurship for undergraduates,Grant/Award Number:202210424099National Natural Science Foundation of China,Grant/Award Numbers:21601067,21701057,21905147。
文摘The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to CO using ultrathin Bi_(12)O_(17)Cl_(2)nanosheets decorated with hydrothermally synthesized bismuth clusters and oxygen vacancies(OVs).The characterizations revealed that the coexistences of OVs and Bi clusters generated in situ contributed to the high efficiency of CO_(2)–CO conversion(64.3μmol g^(−1)h^(−1))and perfect selectivity.The OVs on the facet(001)of the ultrathin Bi_(12)O_(17)Cl_(2)nanosheets serve as sites for CO_(2)adsorption and activation sites,capturing photoexcited electrons and prolonging light absorption due to defect states.In addition,the Bi‐cluster generated in situ offers the ability to trap holes and the surface plasmonic resonance effect.This study offers great potential for the construction of semiconductor hybrids as multiphotocatalysts,capable of being used for the elimination and conversion of CO_(2)in terms of energy and environment.
基金This work was supported by the National Natural Science Foundation of China(Nos.22138011,22205108,22378206)Open Research Fund of Key Laboratory of the Ministry of Education for Advanced Catalysis Materials and Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces(KLMEACM 202201),Zhejiang Normal University.
文摘The insufficient active sites and slow interfacial charge trans-fer of photocatalysts restrict the efficiency of CO_(2) photoreduction.The synchronized modulation of the above key issues is demanding and chal-lenging.Herein,strain-induced strategy is developed to construct the Bi–O-bonded interface in Cu porphyrin-based monoatomic layer(PML-Cu)and Bi_(12)O_(17)Br_(2)(BOB),which triggers the surface interface dual polarization of PML-Cu/BOB(PBOB).In this multi-step polarization,the built-in electric field formed between the interfaces induces the electron transfer from con-duction band(CB)of BOB to CB of PML-Cu and suppresses its reverse migration.Moreover,the surface polarization of PML-Cu further promotes the electron converge in Cu atoms.The introduction of PML-Cu endows a high density of dispersed Cu active sites on the surface of PBOB,significantly promoting the adsorption and activation of CO_(2) and CO desorption.The conversion rate of CO_(2) photoreduction to CO for PBOB can reach 584.3μmol g-1,which is 7.83 times higher than BOB and 20.01 times than PML-Cu.This work offers valuable insights into multi-step polarization regulation and active site design for catalysts.
基金the financial support from the National Natural Science Foundation of China (No.21964006)the Changsha Science and Technology Planning Project (No.kq2203003)+2 种基金the Natural Science Foundation of Hunan Province (No.2020JJ4640)the Scientific Research Fund of Hunan Provincial Education Department (No.20A050)the Scientific Research Found of Changsha University (No.SF1934)。
文摘The construction and application of novel highly efficient photocatalysts have been the focus in the field of environmental pollutant removal.In this work,a novel CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)photocatalysts were synthesized by simple hydrothermal and chemical precipitation method.The fabricated CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)composite exhibited much higher photocatalytic activity than pristine CuFe_(2)O_(4)and Bi_(12)O_(17)Cl_(2)in the removal of bisphenol A(BPA)under visible-light illumination,which ascribed to the intrinsic p-n junction of CuFe_(2)O_(4)and Bi_(12)O_(17)Cl_(2).The photocatalytic degradation rate of BPA on CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)with an optimized CuFe_(2)O_(4)content(1.0 wt.%)reached 93.0%within 30 min.The capture experiments of active species confirmed that the hydroxyl radicals(·OH)and superoxide radicals(·O_(2)^(-))played crucial roles in photocatalytic BPA degradation process.Furthermore,the possible degradation mechanism and pathways of BPA was proposed according to the detected intermediates in photocatalytic reaction process.
基金supported by the National Natural Science Foundation of China(Nos.22108108,22108106,22109055)China Postdoctoral Science Foundation(No.2022M721381).
文摘Increasing the utilization efficiency of photogenerated electrons is highly recognized as one of the ef-ficient approaches to boost the photocatalytic CO_(2)conversion efficiency.Herein,ZIF-67-derived porous carbon(PC)material was employed for the construction of PC@ultrafine Bi_(12)O_(17)Br_(2)nanotubes(PC@BOB NTs)composites through a facile solvothermal synthesis in order to optimize the use of excited elec-trons in the BOB NTs.Photoelectrochemical characterization results revealed that the introduction of PC material achieved a faster charge separation rate in the PC@BOB composites,ensuring more photogener-ated electrons participate in the CO_(2)adsorption and activation process.Moreover,the pore structures of ZIF-67-derived PC material provided abundant confined spaces for the enrichment of CO_(2)molecules.Af-ter 5 h of Xenon lamp irradiation,PC@BOB composites exhibited obviously increased photocatalytic CO_(2)reduction activity in the pure water.When the addition amount of PC was 5 wt%,the PC@BOB-2 com-posite showed the highest CO evolution rate of 359.70μmol/g,which was 2.95 times higher than that of the pure BOB NTs.This work provides some independent insights into the applications of Metal-Organic Framework(MOF)-derived hierarchical porous structures to strengthen the CO_(2)enrichment,as well as the excited charge utilization efficiency,thus achieving a high solar-to-fuel conversion efficiency.
基金the Natural Science Foundation of Jiangsu Province(No.BK20220596)Innovative Science and Technology Platform Project of Cooperation between Yangzhou City and Yangzhou University,China(No.YZ202026305)+3 种基金the Natural Science Foundation of China(Nos.21922202 and 21673202)the Priority Academic Program Development of Jiangsu Higher Education Institutions,Shaanxi Province High-level Talent Introduction Program(Youth Project)Doctoral Research Start-up Fund project of Xi’an Polytechnic University(No.107020589)the Biological Resources Development and the Textile Wastewater Treatment Innovation Team(No.23JP055).
文摘The development of a high-performance ferroelectric piezo-photocatalyst is an efficient strategy for advancing sustainability within the environmental and energy sectors.Yet,a major challenge lies in the creation of a strong polarized electric field that can effectively hinder charge recombination,both within the bulk and on the surface of catalysts.Herein,we synthesize a series of Nb-doped Bi_(4)Ti_(3)O_(12)nanosheets via a facile one-pot hydrothermal method to achieve synergistically enhanced piezo-photocatalytic performance in CO_(2)reduction and pollutant degradation.The optimized doped Bi_(4)Ti_(3)O_(12)demonstrates remarkable efficiency in the conversion of CO_(2)into CO,with a high production rate of 72.7μmol∙g−1∙h−1 without using co-catalysts or any sacrificial agent,surpassing the performance of unmodified Bi_(4)Ti_(3)O_(12)by up to 4.69 folds.Additionally,our catalyst demonstrates ultra-fast piezo-photocatalytic degradation of organic pollutant Rhodamine B(RhB)at low concentrations and exceptional piezo-photocatalytic activity at high concentrations,outperforming most previously reported state-of-the-art catalysts.The systematic corroboration of catalyst characterization and experimental analysis reveals that the synergistic effect arises from the amplified macroscopic polarization induced by lattice distortion caused by the larger Nb ions,thereby improving piezo-photocatalytic efficiency.This research thus offers valuable insights into the direct design and fabrication of versatile catalytic systems,with applications spanning CO_(2)valorization and beyond.
基金supported by the National Natural Science Foundation of China,China(Grant No.51932010)by the National Natural Science Foundation of Shanghai,China(Grant No.19ZR1464600).
文摘Bismuth titanate (Bi_(4)Ti_(3)O_(12),BIT)piezoelectric materials have attracted increasing attention due to their high-temperature applications.However,it is quite challenging to simultaneously achieve outstanding piezoelectric properties and high Curie temperature in BIT-based systems.In this study,oxygen vacancy defects tailoring strategy was utilized to solve this problem,excellent piezoelectric coefficient(32.1 pC/N),and ultrahigh Curie temperature(659℃)are gotten in Bi_(4)Ti_(3)-x(Mn_(1/3)Nb_(2/3))xO_(12)(BTMN)ceramics,which are among the top values in the BIT-based ceramics.More importantly,the(Mn_(1/3)Nb_(2/3))(4+d)+complex-ion modified Bi_(4)Ti_(3)O_(12)-based ceramics are characterized with excellent piezoelectric stability up to 500℃(d33>30.0 pC/N at 500℃))and significantly reduced conductivity(only~10^(-7)U-1 cm^(-1)at 500℃).Moreover,enhanced ferroelectricity and good dielectric stability were also obtained.The better comprehensive properties can be ascribed to two aspects.First,the concentration of oxygen vacancy defects is obviously reduced,and their distribution is effectively controlled in BITMN ceramics.Second,the introduction of(Mn_(1/3)Nb_(2/3))^((4+δ)+)complex-ion gives rise to the antiphase boundaries and massive ferroelectric domain walls.This works not only reveal the high potential of BITMN ceramics for high-temperature piezoelectric applications but also deepen the understanding of the structure-properties relationship in BIT-based materials.
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.
