In this work,monoclinic Bi_(2)O_(3) was applied for the first time,to the best of our knowledge,as a catalyst in the process of dye degradation by a non-thermal atmospheric-pressure positive pulsating corona discharge...In this work,monoclinic Bi_(2)O_(3) was applied for the first time,to the best of our knowledge,as a catalyst in the process of dye degradation by a non-thermal atmospheric-pressure positive pulsating corona discharge.The research focused on the interaction of the plasma-generated species and the catalyst,as well as the role of the catalyst in the degradation process.Plasma decomposition of the anthraquinone reactive dye Reactive Blue 19(RB 19) was performed in a selfmade reactor system.Bi_(2)O_(3) was prepared by electrodeposition followed by thermal treatment,and characterized by x-ray diffraction,scanning electron microscopy and energy-dispersive xray techniques.It was observed that the catalyst promoted decomposition of plasma-generated H_(2)O_(2) into ·OH radicals,the principal dye-degrading reagent,which further attacked the dye molecules.The catalyst improved the decolorization rate by 2.5 times,the energy yield by 93.4%and total organic carbon removal by 7.1%.Excitation of the catalyst mostly occurred through strikes by plasma-generated reactive ions and radical species from the air,accelerated by the electric field,as well as by fast electrons with an energy of up to 15 eV generated by the streamers reaching the liquid surface.These strikes transferred the energy to the catalyst and created the electrons and holes,which further reacted with H_(2)O_(2) and water,producing ·OH radicals.This was indentified as the primary role of the catalyst in this process.Decolorization reactions followed pseudo first-order kinetics.Production of H_(2)O_(2) and the dye degradation rate increased with increase in the input voltage.The optimal catalyst dose was 500 mg·dm^(-3).The decolorization rate was a little lower in river water compared with that in deionized water due to the side reactions of ·OH radicals with organic matter and inorganic ions dissolved in the river water.展开更多
Unraveling atomic-level active sites of layered photocatalyst towards lowconcentration CO_(2) conversion is still challenging.Herein,the yield and selectivity of photocatalytic CO_(2) reduction of the Aurivillius-rela...Unraveling atomic-level active sites of layered photocatalyst towards lowconcentration CO_(2) conversion is still challenging.Herein,the yield and selectivity of photocatalytic CO_(2) reduction of the Aurivillius-related oxide semiconductor Bi_(2)O_(2)SiO_(3) nanosheet(BOSO)were largely improved using a surface sulfidation strategy.The experiment and theoretical calculation confirmed that surface sulfidation of the Bi_(2)O_(2)SiO_(3) nanosheet(S-BOSO,6.28 nm)redistributed the charge-enriched Bi sites,extended the solar spectrum absorption to the whole visible range,and considerably enhanced the charge separation,in addition to creating new reaction active sites,as compared to pristine BOSO.Subsequently,surface sulfidation played a switchable role,wherein S-BOSO showed a very high CH_(3)OH generation rate(12.78μmol g^(-1) for 4 h,78.6%selectivity)from low-concentration CO_(2)(1000 ppm)under visible light irradiation,which outperforms most of the state-of-the-art photocatalysts under similar conditions.This study presents an atomic-level modification protocol for engineering reactive sites and charge behaviors to promote solar-to-energy conversion.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
Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions...Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions were synthesized by a facile solvothermal route.The resultant materials were examined by X-ray photoelectron spectrometer(XPS),X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDX),transmission electron microscopy(TEM),high-resolution transmission electron microscopy(HRTEM),photoluminescence spectroscopy(PL),Fourier transform infrared spectroscopy(FT-IR),UV-Vis diffuse reflection spectroscopy(UV-vis DRS),photocurrent density,electrochemical impedance spectroscopy(EIS),and Brunauer–Emmett–Teller(BET)analyses.After the integration of Fe-MOF with GCN-NSh/Bi_(5)O_(7)Br,the removal constant of tetracycline over the optimal GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite was promoted 33 times compared with that of the pristine GCN.The GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite showed superior photoactivity to azithromycin,metronidazole,and cephalexin removal that was 36.4,20.2,and 14.6 times higher than that of pure GCN,respectively.Radical quenching tests showed that·O_(2)-and h+mainly contributed to the elimination reaction.In addition,the nanocomposite maintained excellent activity after 4 successive cycles.Based on the developed n–n heterojunctions among n-GCN-NSh,n-Bi_(5)O_(7)Br,and n-Fe-MOF semiconductors,the double S-scheme charge transfer mechanism was proposed for the destruction of the selected antibiotics.展开更多
基金financial support from the Ministry of Education, Science and Technological Development of the Republic of Serbia (No.451-03-47/2023-01/200124)。
文摘In this work,monoclinic Bi_(2)O_(3) was applied for the first time,to the best of our knowledge,as a catalyst in the process of dye degradation by a non-thermal atmospheric-pressure positive pulsating corona discharge.The research focused on the interaction of the plasma-generated species and the catalyst,as well as the role of the catalyst in the degradation process.Plasma decomposition of the anthraquinone reactive dye Reactive Blue 19(RB 19) was performed in a selfmade reactor system.Bi_(2)O_(3) was prepared by electrodeposition followed by thermal treatment,and characterized by x-ray diffraction,scanning electron microscopy and energy-dispersive xray techniques.It was observed that the catalyst promoted decomposition of plasma-generated H_(2)O_(2) into ·OH radicals,the principal dye-degrading reagent,which further attacked the dye molecules.The catalyst improved the decolorization rate by 2.5 times,the energy yield by 93.4%and total organic carbon removal by 7.1%.Excitation of the catalyst mostly occurred through strikes by plasma-generated reactive ions and radical species from the air,accelerated by the electric field,as well as by fast electrons with an energy of up to 15 eV generated by the streamers reaching the liquid surface.These strikes transferred the energy to the catalyst and created the electrons and holes,which further reacted with H_(2)O_(2) and water,producing ·OH radicals.This was indentified as the primary role of the catalyst in this process.Decolorization reactions followed pseudo first-order kinetics.Production of H_(2)O_(2) and the dye degradation rate increased with increase in the input voltage.The optimal catalyst dose was 500 mg·dm^(-3).The decolorization rate was a little lower in river water compared with that in deionized water due to the side reactions of ·OH radicals with organic matter and inorganic ions dissolved in the river water.
基金Natural Science Foundation of Hubei Province,Grant/Award Number:2021CFB242Research Project of Hubei Provincial Department of Education,Grant/Award Number:Q20202501+3 种基金China Postdoctoral Science Foundation,Grant/Award Number:2020M682878National Natural Science Foundation of China,Grant/Award Numbers:51971124,52104254,52171217State Key Laboratory of Electrical Insulation and Power Equipment,Xi'an Jiaotong University,Grant/Award Number:EIPE22208National Postdoctoral Program for Innovative Talents,Grant/Award Number:BX20200222。
文摘Unraveling atomic-level active sites of layered photocatalyst towards lowconcentration CO_(2) conversion is still challenging.Herein,the yield and selectivity of photocatalytic CO_(2) reduction of the Aurivillius-related oxide semiconductor Bi_(2)O_(2)SiO_(3) nanosheet(BOSO)were largely improved using a surface sulfidation strategy.The experiment and theoretical calculation confirmed that surface sulfidation of the Bi_(2)O_(2)SiO_(3) nanosheet(S-BOSO,6.28 nm)redistributed the charge-enriched Bi sites,extended the solar spectrum absorption to the whole visible range,and considerably enhanced the charge separation,in addition to creating new reaction active sites,as compared to pristine BOSO.Subsequently,surface sulfidation played a switchable role,wherein S-BOSO showed a very high CH_(3)OH generation rate(12.78μmol g^(-1) for 4 h,78.6%selectivity)from low-concentration CO_(2)(1000 ppm)under visible light irradiation,which outperforms most of the state-of-the-art photocatalysts under similar conditions.This study presents an atomic-level modification protocol for engineering reactive sites and charge behaviors to promote solar-to-energy conversion.
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Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions were synthesized by a facile solvothermal route.The resultant materials were examined by X-ray photoelectron spectrometer(XPS),X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDX),transmission electron microscopy(TEM),high-resolution transmission electron microscopy(HRTEM),photoluminescence spectroscopy(PL),Fourier transform infrared spectroscopy(FT-IR),UV-Vis diffuse reflection spectroscopy(UV-vis DRS),photocurrent density,electrochemical impedance spectroscopy(EIS),and Brunauer–Emmett–Teller(BET)analyses.After the integration of Fe-MOF with GCN-NSh/Bi_(5)O_(7)Br,the removal constant of tetracycline over the optimal GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite was promoted 33 times compared with that of the pristine GCN.The GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite showed superior photoactivity to azithromycin,metronidazole,and cephalexin removal that was 36.4,20.2,and 14.6 times higher than that of pure GCN,respectively.Radical quenching tests showed that·O_(2)-and h+mainly contributed to the elimination reaction.In addition,the nanocomposite maintained excellent activity after 4 successive cycles.Based on the developed n–n heterojunctions among n-GCN-NSh,n-Bi_(5)O_(7)Br,and n-Fe-MOF semiconductors,the double S-scheme charge transfer mechanism was proposed for the destruction of the selected antibiotics.