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
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.
