Sulfate-modified titanium dioxide-bearing blast furnace slag(STBBFS) photocatalysts were prepared by the high energy ball milling method with(NH4)2SO4 and titanium dioxide-bearing blast furnace slag(TBBFS) as ra...Sulfate-modified titanium dioxide-bearing blast furnace slag(STBBFS) photocatalysts were prepared by the high energy ball milling method with(NH4)2SO4 and titanium dioxide-bearing blast furnace slag(TBBFS) as raw materials.X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD),scanning electron microscopy(SEM),thermogravimetric analysis(TGA),UV-visible diffuse reflectance absorption spectra(UV-Vis),adsorption experiment and photocatalytic degradation measurement were conducted to characterize the structure,surface status,light absorption capacity,adsorption capacity and photocatalytic activity of the obtained photocatalysts.The adsorption equilibrium was described by the Langmuir isotherm model with a maximum adsorption capacity of 8.25 mg/g of Cr(VI) ions onto the STBBFS photocatalysts.As a result,sulfation of TBBFS improved the photocatalytic activities of STBBFSx photocatalysts.At a low calcination temperature,the photocatalytic activity of STBBFS300 photocatalyst was markedly higher compared with TBBFSx prepared at high calcination temperature,indicating that the photocatalytic activity of STBBFSx photocatalyst was determined by the balanced result between adsorption capacity and perovskite content.展开更多
A nano-MoS2/bentonite composite was synthesized by calcinating MoS3 deposited on bentonite in H2. The obtained composite was characterized using thermogravimetric analysis, X-ray diffractometer, scanning electron micr...A nano-MoS2/bentonite composite was synthesized by calcinating MoS3 deposited on bentonite in H2. The obtained composite was characterized using thermogravimetric analysis, X-ray diffractometer, scanning electron microscope and transmission electron microscope. The results show that nano-MoS2 particles are distributed on the surface of bentonite and form layered structures with layer distance of about 0.64 nm. The composite presents an excellent performance for the removal of methyl orange. Some operation conditions affect the removal efficiency of methyl orange, such as dosage of composite, initial concentration of methyl orange, temperature and pH value. However, light source does not influence the removal efficiency. The removal mechanism is attributed to the adsorption of methyl orange on the nano-MoS2/bentonite composite. The adsorption of methyl orange on the composite is in accordance with the pseudo-second-order kinetic model.展开更多
Photocatalysis is regarded as an ideal technology for solving the urgent environmental and energy issues that we face today.Among the reported photocatalysts,molybdenum disulfide(MoS2) is very promising for applicat...Photocatalysis is regarded as an ideal technology for solving the urgent environmental and energy issues that we face today.Among the reported photocatalysts,molybdenum disulfide(MoS2) is very promising for applications in hydrogen production and pollutant photodegradation.However,its lack of active sites and the difficulty of recovering catalysts in powder form have hindered its wide application.Here,we report the successful preparation of a macroscopic visible-light responsive MoS2/reduced graphene oxide(MoS2/RGO) aerogel.The obtained MoS2/RGO aerogel exhibits enhanced photocatalytic activity towards hydrogen production and photoreduction of Cr(Ⅵ) in comparison with the MoS2 powder.In addition,the low density(56.1 mg/cm^3) of the MoS2/RGO aerogel enables it to be used as an efficient adsorption material for organic pollutants.Our results demonstrate that this very promising multifunctional aerogel has potential applications in environmental remediation and clean energy production.展开更多
Photocatalytic conversion of“greenhouse gas”CO2is considered to be one of the most effective ways to alleviate current energy and environmental problems without additional energy consumption and pollutant emission.T...Photocatalytic conversion of“greenhouse gas”CO2is considered to be one of the most effective ways to alleviate current energy and environmental problems without additional energy consumption and pollutant emission.The performance of many traditional semiconductor photocatalysts is not efficient enough to satisfy the requirements of practical applications because of their limited specific surface area and low CO2adsorption capacity.Therefore,the exploration of photocatalysts with high CO2uptake is significant in the field of CO2conversion.Recently the porous materials appeared to be a kind of superior candidate for enriching the CO2molecules on the surface of photocatalysts for catalytic conversion.This paper first summarizes the advances in the development of nanoporous adsorbents for CO2capture.Three main classes of porous materials are considered:inorganic porous materials,metal organic frameworks,and microporous organic polymers.Based on systematic research on CO2uptake,we then highlight the recent progress in these porous‐material‐based photocatalysts for CO2conversion.Benefiting from the improved CO2uptake capacity,the porous‐material‐based photocatalysts exhibited remarkably enhanced efficiency in the reduction of CO2to chemical fuels,such as CO,CH4,and CH3OH.Based on reported recent achievements,we predict a trend of development in multifunctional materials with both high adsorption capability and photocatalytic performance for CO2utilization.展开更多
A series of In_(x)Sb_(2-x)S_(3) nanosheets modified g-C_(3)N_(4)(In_(x)Sb_(2-x)S_(3)-TCN)heterojunctions with different g-C_(3)N_(4) contents were fabricated by an in situ deposition method.All the In_(x)Sb_(2-x)S_(3)...A series of In_(x)Sb_(2-x)S_(3) nanosheets modified g-C_(3)N_(4)(In_(x)Sb_(2-x)S_(3)-TCN)heterojunctions with different g-C_(3)N_(4) contents were fabricated by an in situ deposition method.All the In_(x)Sb_(2-x)S_(3)-TCN composites were applied as photocatalysts in Cr(Ⅵ)polluted water treatment and the results displayed that In_(x)Sb_(2-x)S_(3)-TCN could effectively remove Cr(Ⅵ)under visible light through synergistic effects of adsorption and photocatalytic reduction.Especially,In_(x)Sb_(2-x)S_(3)-TCN-70(70 mg g-C_(3)N_(4)) exhibited the most excellent adsorption and photocatalytic reduction performance among all composites,which possessed a high equilibrium adsorption capacity of 12.45 mg/g in a 30.0 mg/L Cr(Ⅵ)aqueous solution,and reduced Cr(Ⅵ)to Cr(Ⅲ)within 10 min under visible light irradiation.DRS and PL results indicated that the interfacial coupling effect between g-C_(3)N_(4)and In_(x)Sb_(2-x)S_(3) enhanced the utilization efficiency of visible light and suppressed photoinduced carrier recombination,which improved the photocatalytic activity of composites.Moreover,the photocatalyst exhibited satisfactory reduction activity and good stability after 5 cycles of Cr(Ⅵ)adsorptionphotoreduction.展开更多
In contrast to the exploration of novel photocatalytic materials,vacancy engineering of traditionalphotocatalysts comprising earth‐abundant elements represents an effective method for enhancingphotocatalytic performa...In contrast to the exploration of novel photocatalytic materials,vacancy engineering of traditionalphotocatalysts comprising earth‐abundant elements represents an effective method for enhancingphotocatalytic performance without introducing alien elements.This minireview analyzes the latestprogress in engineering vacancies in photocatalysts,remarks on state‐of‐the‐art characterizationtechniques for vacancies,and reviews the formation chemistry and fundamental benefits of anionand cation vacancies in typical photocatalysts.Although knowledge of these vacancies is increasing,challenges remain in this field,and possible further research is therefore also discussed.展开更多
Adsorption and photodegradation are promising approaches for removing organic pollutions.In this study,we combined these two processes by co-loading Fe-TiO2 and Fe2O3 quantum dots(QDs)on porous MCM-41,using a simple h...Adsorption and photodegradation are promising approaches for removing organic pollutions.In this study,we combined these two processes by co-loading Fe-TiO2 and Fe2O3 quantum dots(QDs)on porous MCM-41,using a simple hydrolysis method.X-ray diffraction,high-resolution transmission electron microscopy,and X-ray photoelectron spectroscopy results indicated that Fe-TiO2 QDs are formed at low Fe precursor concentrations,while additional Fe2O3 QDs are formed at higher Fe precursor concentrations.The Fe2O3 and Fe-TiO2 QDs impart high adsorption capacity and high photoactivity to the porous MCM-41,respectively.Thus,their combination results in a synergic effect of the adsorption and photodegradation.The highest-performing sample exhibits excellent performance in removing rose bengal from aqueous solution.展开更多
Activated carbon/nanosized CdS/chitosan(AC/n-CdS/CS) composites as adsorbent and photoactive catalyst were prepared under low temperature(≤60 ℃) and ambient pressure.Methyl orange(MO) was chosen as a model pollutant...Activated carbon/nanosized CdS/chitosan(AC/n-CdS/CS) composites as adsorbent and photoactive catalyst were prepared under low temperature(≤60 ℃) and ambient pressure.Methyl orange(MO) was chosen as a model pollutant to evaluate synergistic effect of adsorption and photocatalytic decolorization by this innovative photocatalyst under visible light irradiation.Effects of various parameters such as catalyst amount,initial MO concentration,solution pH and reuse of catalyst on the decolorization of MO were investigated to optimize operational conditions.The decolorization of MO catalyzed by AC/n-CdS/CS fits the Langmuir-Hinshelwood kinetics model,and a surface reaction,where the dyes are absorbed,is the controlling step of the process.Decolorization efficiency of MO is improved with the increase in catalyst amount within a certain range.The photodecolorization of MO is more efficient in acidic media than alkaline media.The decolorization efficiency of MO is still higher than 84% after five cycles and 60 min under visible light irradiation,which confirms the reusability of AC/n-CdS/CS composite catalyst.展开更多
Silver‐modified semiconductor photocatalysts typically exhibit enhanced photocatalytic activitytoward the degradation of organic substances.In comparison,their hydrogen‐evolution rates arerelatively low owing to poo...Silver‐modified semiconductor photocatalysts typically exhibit enhanced photocatalytic activitytoward the degradation of organic substances.In comparison,their hydrogen‐evolution rates arerelatively low owing to poor interfacial catalytic reactions to producing hydrogen.In the presentstudy,thiocyanate anions(SCN–)as interfacial catalytic active sites were selectively adsorbed ontothe Ag surface of g‐C3N4/Ag photocatalyst to promote interfacial H2‐evolution reactions.The thiocyanate‐modified g‐C3N4/Ag(g‐C3N4/Ag‐SCN)photocatalysts were synthesized via photodepositionof metallic Ag on g‐C3N4and subsequent selective adsorption of SCN– ions on the Ag surface by animpregnation method.The resulting g‐C3N4/Ag‐SCN photocatalysts exhibited considerably higherphotocatalytic H2‐evolution activity than the g‐C3N4,g‐C3N4/Ag,and g‐C3N4/SCN photocatalysts.Furthermore,the g‐C3N4/Ag‐SCN photocatalyst displayed the highest H2‐evolution rate(3.9μmolh?1)when the concentration of the SCN– ions was adjusted to0.3mmol L?1.The H2‐evolution rateobtained was higher than those of g‐C3N4(0.15μmol h?1)and g‐C3N4/Ag(0.71μmol h?1).Consideringthe enhanced performance of g‐C3N4/Ag upon minimal addition of SCN– ions,a synergistic effectof metallic Ag and SCN– ions is proposed―the Ag nanoparticles act as an effective electron‐transfermediator for the steady capture and rapid transportation of photogenerated electrons,while theadsorbed SCN– ions serve as an interfacial active site to effectively absorb protons from solution andpromote rapid interfacial H2‐evolution reactions.Considering the present facile synthesis and itshigh efficacy,the present work may provide new insights into preparing high‐performance photocatalytic materials展开更多
This paper studies the adsorption of diethyl phthalate (DEP,an environmental hormone) on the surface of nanoscale TiO2, effects of pH value of solutions, initial concentrations of DEP and additive surfactant on phot...This paper studies the adsorption of diethyl phthalate (DEP,an environmental hormone) on the surface of nanoscale TiO2, effects of pH value of solutions, initial concentrations of DEP and additive surfactant on photocatalytic degradation and dynamics of DEP. Under ultra violet illumination, the interaction between DEP and surfactants including DBS (sodium dodecylbenzenesulfonate), CTAB (cetyltrimethylammonium bromide), and OP-10 (nonylphenol polyoxyethylene ether) was exploited from the perspective of degradation speed calculated by the data of high pressure liquid chromatography (HPLC) and UV-Vis spectra, respectively. Photocatalytic degradation of DEP followed pseudo first-order reaction kinetics. DEP as substrate degraded fast when its initial concentration was 130 mg/L. TiO2 had certain adsorption ability of DEP. TiO2 could adsorb the most DEP at the approximately neutral pH of 6.91. Degradation of DEP was not affected obviously by additives OP-10 and DBS. Degradation rate of DEP was not enhanced greatly in the presence of surfactants, but degradation of DBS was sped up. Degradation rate of DEP was depressed in the presence of additive CTAB. The more CTAB was added, the less DEP was degraded. Degradation rate of CTAB became slow with the increase of initial CTAB concentration. The possible adsorption models among TiO2, DEP and surfactants were given.展开更多
ZnTixFe2-xO4 and ZnTi0.6Fe1.4O4/Carbon nanotubes (ZT0.6F1.4/CNTs) composites were prepared by chemical co-precipitation method. The composition, microstructure, magnetic property, adsorption and photocatalytic activ...ZnTixFe2-xO4 and ZnTi0.6Fe1.4O4/Carbon nanotubes (ZT0.6F1.4/CNTs) composites were prepared by chemical co-precipitation method. The composition, microstructure, magnetic property, adsorption and photocatalytic activity of the prepared samples were characterized by means of modem analytical techniques. The results indicated that ZT0.6F1.4CNTs composites not only held the original special structure and excellent adsorption properties of CNTs, but also had suitable magnetic property and excellent photocatalytic activity. The removal rate of the samples on Rhodamine B (RhB) depended on the adsorption of CNTs and the photocatalytic degradation of ZTo.6F1.4 in the composites. The maximum adsorption amount (qm) of ZT0.6F1.4/CNTs with the mass ratios of ZT0.6F1.4 to CNTs (mz/c)=l was up to 17.153 mg g-t for RhB, its adsorption behavior was in accord with Langmuir model, and its photocatalytic degradation activity on RhB had a positive correlation with the content of ZT0.6F1.4 in the sample. The experimental results indicate that the total removal rate of composite with rnz/c=l on RhB was more than 95% and the composite had good decontamination capability on industrial dye wastewater. In addition, the samples can be recovered conveniently, activated easily and had good performance for recycling.展开更多
Dynamic defects on halide perovskite materials,caused by ion dissociation and migration under light illumination,typically result in undesirable energy dissipation and limited energy conversion efficiency.However,in t...Dynamic defects on halide perovskite materials,caused by ion dissociation and migration under light illumination,typically result in undesirable energy dissipation and limited energy conversion efficiency.However,in this work,we demonstrated that dynamic halogen defects generated by the same process in bismuth oxyhalide(Bi_(5)O_(7)Cl)materials can act as active sites to promote charge separation and photocatalytic efficiency.Mechanistic studies and density functional theory calculations revealed that dynamic Cl defects affected the electronic structure of Bi_(5)O_(7)Cl and photocatalytic CO_(2)reduction process.As active sites,these defects promoted charge transfer,leading to the activation of adsorbed CO_(2)molecules and reduction of the energy barrier of the rate-determining step.Thus,CO_(2)was spontaneously converted into COOH−intermediate and finally reduced to CO with a high efficiency of 108.60μmol g^(−1) and selectivity of 100%after 4-h of CO_(2)photoreduction.This work is highly instructive and valuable to the exploration of dynamic defects on halide-containing materials applied in solar energy conversion.展开更多
基金Project (2007CB613504) supported by the National Basic Research Program of ChinaProject (307009) supported by the Foundation for Key Program of Ministry of Education,China+1 种基金Project (N110423003) supported by the Fundamental Research Funds for the Central Universities,ChinaProject (E2012501012) supported by Natural Science Foundation-Steel and Iron Foundation of Hebei Province,China
文摘Sulfate-modified titanium dioxide-bearing blast furnace slag(STBBFS) photocatalysts were prepared by the high energy ball milling method with(NH4)2SO4 and titanium dioxide-bearing blast furnace slag(TBBFS) as raw materials.X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD),scanning electron microscopy(SEM),thermogravimetric analysis(TGA),UV-visible diffuse reflectance absorption spectra(UV-Vis),adsorption experiment and photocatalytic degradation measurement were conducted to characterize the structure,surface status,light absorption capacity,adsorption capacity and photocatalytic activity of the obtained photocatalysts.The adsorption equilibrium was described by the Langmuir isotherm model with a maximum adsorption capacity of 8.25 mg/g of Cr(VI) ions onto the STBBFS photocatalysts.As a result,sulfation of TBBFS improved the photocatalytic activities of STBBFSx photocatalysts.At a low calcination temperature,the photocatalytic activity of STBBFS300 photocatalyst was markedly higher compared with TBBFSx prepared at high calcination temperature,indicating that the photocatalytic activity of STBBFSx photocatalyst was determined by the balanced result between adsorption capacity and perovskite content.
基金Project (2011M500110) supported by the Postdoctoral Science Foundation of ChinaProject (50905054) supported by the National Natural Science Foundation of ChinaProject (12RC03) supported by Hefei University, China
文摘A nano-MoS2/bentonite composite was synthesized by calcinating MoS3 deposited on bentonite in H2. The obtained composite was characterized using thermogravimetric analysis, X-ray diffractometer, scanning electron microscope and transmission electron microscope. The results show that nano-MoS2 particles are distributed on the surface of bentonite and form layered structures with layer distance of about 0.64 nm. The composite presents an excellent performance for the removal of methyl orange. Some operation conditions affect the removal efficiency of methyl orange, such as dosage of composite, initial concentration of methyl orange, temperature and pH value. However, light source does not influence the removal efficiency. The removal mechanism is attributed to the adsorption of methyl orange on the nano-MoS2/bentonite composite. The adsorption of methyl orange on the composite is in accordance with the pseudo-second-order kinetic model.
基金supported by the National Natural Science Foundation of China (U1232119, 21403172)the Sichuan Youth Science and Technology Foundation (2013JQ0034, 2014JQ0017)the Innovative Research Team of Sichuan Province (2016TD0011)~~
文摘Photocatalysis is regarded as an ideal technology for solving the urgent environmental and energy issues that we face today.Among the reported photocatalysts,molybdenum disulfide(MoS2) is very promising for applications in hydrogen production and pollutant photodegradation.However,its lack of active sites and the difficulty of recovering catalysts in powder form have hindered its wide application.Here,we report the successful preparation of a macroscopic visible-light responsive MoS2/reduced graphene oxide(MoS2/RGO) aerogel.The obtained MoS2/RGO aerogel exhibits enhanced photocatalytic activity towards hydrogen production and photoreduction of Cr(Ⅵ) in comparison with the MoS2 powder.In addition,the low density(56.1 mg/cm^3) of the MoS2/RGO aerogel enables it to be used as an efficient adsorption material for organic pollutants.Our results demonstrate that this very promising multifunctional aerogel has potential applications in environmental remediation and clean energy production.
基金supported by the National Natural Science Foundation of China(21771070,21571071)~~
文摘Photocatalytic conversion of“greenhouse gas”CO2is considered to be one of the most effective ways to alleviate current energy and environmental problems without additional energy consumption and pollutant emission.The performance of many traditional semiconductor photocatalysts is not efficient enough to satisfy the requirements of practical applications because of their limited specific surface area and low CO2adsorption capacity.Therefore,the exploration of photocatalysts with high CO2uptake is significant in the field of CO2conversion.Recently the porous materials appeared to be a kind of superior candidate for enriching the CO2molecules on the surface of photocatalysts for catalytic conversion.This paper first summarizes the advances in the development of nanoporous adsorbents for CO2capture.Three main classes of porous materials are considered:inorganic porous materials,metal organic frameworks,and microporous organic polymers.Based on systematic research on CO2uptake,we then highlight the recent progress in these porous‐material‐based photocatalysts for CO2conversion.Benefiting from the improved CO2uptake capacity,the porous‐material‐based photocatalysts exhibited remarkably enhanced efficiency in the reduction of CO2to chemical fuels,such as CO,CH4,and CH3OH.Based on reported recent achievements,we predict a trend of development in multifunctional materials with both high adsorption capability and photocatalytic performance for CO2utilization.
基金Projects(41977129,21607176,42007138) supported by the National Natural Science Foundation of ChinaProject(kq1802011) supported by the Changsha Outstanding Innovative Youth Training Program,ChinaProject(2017JJ3516)supported by the Natural Science Foundation of Hunan Province,China。
文摘A series of In_(x)Sb_(2-x)S_(3) nanosheets modified g-C_(3)N_(4)(In_(x)Sb_(2-x)S_(3)-TCN)heterojunctions with different g-C_(3)N_(4) contents were fabricated by an in situ deposition method.All the In_(x)Sb_(2-x)S_(3)-TCN composites were applied as photocatalysts in Cr(Ⅵ)polluted water treatment and the results displayed that In_(x)Sb_(2-x)S_(3)-TCN could effectively remove Cr(Ⅵ)under visible light through synergistic effects of adsorption and photocatalytic reduction.Especially,In_(x)Sb_(2-x)S_(3)-TCN-70(70 mg g-C_(3)N_(4)) exhibited the most excellent adsorption and photocatalytic reduction performance among all composites,which possessed a high equilibrium adsorption capacity of 12.45 mg/g in a 30.0 mg/L Cr(Ⅵ)aqueous solution,and reduced Cr(Ⅵ)to Cr(Ⅲ)within 10 min under visible light irradiation.DRS and PL results indicated that the interfacial coupling effect between g-C_(3)N_(4)and In_(x)Sb_(2-x)S_(3) enhanced the utilization efficiency of visible light and suppressed photoinduced carrier recombination,which improved the photocatalytic activity of composites.Moreover,the photocatalyst exhibited satisfactory reduction activity and good stability after 5 cycles of Cr(Ⅵ)adsorptionphotoreduction.
基金supported by the National Natural Science Foundation of China (21377084)Special Fund for Agro-scientific Research in the Public Interest (201503107)~~
文摘In contrast to the exploration of novel photocatalytic materials,vacancy engineering of traditionalphotocatalysts comprising earth‐abundant elements represents an effective method for enhancingphotocatalytic performance without introducing alien elements.This minireview analyzes the latestprogress in engineering vacancies in photocatalysts,remarks on state‐of‐the‐art characterizationtechniques for vacancies,and reviews the formation chemistry and fundamental benefits of anionand cation vacancies in typical photocatalysts.Although knowledge of these vacancies is increasing,challenges remain in this field,and possible further research is therefore also discussed.
文摘Adsorption and photodegradation are promising approaches for removing organic pollutions.In this study,we combined these two processes by co-loading Fe-TiO2 and Fe2O3 quantum dots(QDs)on porous MCM-41,using a simple hydrolysis method.X-ray diffraction,high-resolution transmission electron microscopy,and X-ray photoelectron spectroscopy results indicated that Fe-TiO2 QDs are formed at low Fe precursor concentrations,while additional Fe2O3 QDs are formed at higher Fe precursor concentrations.The Fe2O3 and Fe-TiO2 QDs impart high adsorption capacity and high photoactivity to the porous MCM-41,respectively.Thus,their combination results in a synergic effect of the adsorption and photodegradation.The highest-performing sample exhibits excellent performance in removing rose bengal from aqueous solution.
基金Project(21007044) supported by the National Natural Science Foundation of ChinaProject(20050532009) supported by the Doctoral Foundation of Ministry of Education of China
文摘Activated carbon/nanosized CdS/chitosan(AC/n-CdS/CS) composites as adsorbent and photoactive catalyst were prepared under low temperature(≤60 ℃) and ambient pressure.Methyl orange(MO) was chosen as a model pollutant to evaluate synergistic effect of adsorption and photocatalytic decolorization by this innovative photocatalyst under visible light irradiation.Effects of various parameters such as catalyst amount,initial MO concentration,solution pH and reuse of catalyst on the decolorization of MO were investigated to optimize operational conditions.The decolorization of MO catalyzed by AC/n-CdS/CS fits the Langmuir-Hinshelwood kinetics model,and a surface reaction,where the dyes are absorbed,is the controlling step of the process.Decolorization efficiency of MO is improved with the increase in catalyst amount within a certain range.The photodecolorization of MO is more efficient in acidic media than alkaline media.The decolorization efficiency of MO is still higher than 84% after five cycles and 60 min under visible light irradiation,which confirms the reusability of AC/n-CdS/CS composite catalyst.
基金supported by the National Natural Science Foundation of China(51472192,21477094,21771142)the Fundamental Research Funds for the Central Universities(WUT 2017IB002)~~
文摘Silver‐modified semiconductor photocatalysts typically exhibit enhanced photocatalytic activitytoward the degradation of organic substances.In comparison,their hydrogen‐evolution rates arerelatively low owing to poor interfacial catalytic reactions to producing hydrogen.In the presentstudy,thiocyanate anions(SCN–)as interfacial catalytic active sites were selectively adsorbed ontothe Ag surface of g‐C3N4/Ag photocatalyst to promote interfacial H2‐evolution reactions.The thiocyanate‐modified g‐C3N4/Ag(g‐C3N4/Ag‐SCN)photocatalysts were synthesized via photodepositionof metallic Ag on g‐C3N4and subsequent selective adsorption of SCN– ions on the Ag surface by animpregnation method.The resulting g‐C3N4/Ag‐SCN photocatalysts exhibited considerably higherphotocatalytic H2‐evolution activity than the g‐C3N4,g‐C3N4/Ag,and g‐C3N4/SCN photocatalysts.Furthermore,the g‐C3N4/Ag‐SCN photocatalyst displayed the highest H2‐evolution rate(3.9μmolh?1)when the concentration of the SCN– ions was adjusted to0.3mmol L?1.The H2‐evolution rateobtained was higher than those of g‐C3N4(0.15μmol h?1)and g‐C3N4/Ag(0.71μmol h?1).Consideringthe enhanced performance of g‐C3N4/Ag upon minimal addition of SCN– ions,a synergistic effectof metallic Ag and SCN– ions is proposed―the Ag nanoparticles act as an effective electron‐transfermediator for the steady capture and rapid transportation of photogenerated electrons,while theadsorbed SCN– ions serve as an interfacial active site to effectively absorb protons from solution andpromote rapid interfacial H2‐evolution reactions.Considering the present facile synthesis and itshigh efficacy,the present work may provide new insights into preparing high‐performance photocatalytic materials
基金Supported by Tianjin Natural Science Foundation (No. 033604711) and Science and Technology Foundation of Construction Ministry (No. 03-2-064).
文摘This paper studies the adsorption of diethyl phthalate (DEP,an environmental hormone) on the surface of nanoscale TiO2, effects of pH value of solutions, initial concentrations of DEP and additive surfactant on photocatalytic degradation and dynamics of DEP. Under ultra violet illumination, the interaction between DEP and surfactants including DBS (sodium dodecylbenzenesulfonate), CTAB (cetyltrimethylammonium bromide), and OP-10 (nonylphenol polyoxyethylene ether) was exploited from the perspective of degradation speed calculated by the data of high pressure liquid chromatography (HPLC) and UV-Vis spectra, respectively. Photocatalytic degradation of DEP followed pseudo first-order reaction kinetics. DEP as substrate degraded fast when its initial concentration was 130 mg/L. TiO2 had certain adsorption ability of DEP. TiO2 could adsorb the most DEP at the approximately neutral pH of 6.91. Degradation of DEP was not affected obviously by additives OP-10 and DBS. Degradation rate of DEP was not enhanced greatly in the presence of surfactants, but degradation of DBS was sped up. Degradation rate of DEP was depressed in the presence of additive CTAB. The more CTAB was added, the less DEP was degraded. Degradation rate of CTAB became slow with the increase of initial CTAB concentration. The possible adsorption models among TiO2, DEP and surfactants were given.
基金the National Nature Science Foundation of China (21071125) for financial support
文摘ZnTixFe2-xO4 and ZnTi0.6Fe1.4O4/Carbon nanotubes (ZT0.6F1.4/CNTs) composites were prepared by chemical co-precipitation method. The composition, microstructure, magnetic property, adsorption and photocatalytic activity of the prepared samples were characterized by means of modem analytical techniques. The results indicated that ZT0.6F1.4CNTs composites not only held the original special structure and excellent adsorption properties of CNTs, but also had suitable magnetic property and excellent photocatalytic activity. The removal rate of the samples on Rhodamine B (RhB) depended on the adsorption of CNTs and the photocatalytic degradation of ZTo.6F1.4 in the composites. The maximum adsorption amount (qm) of ZT0.6F1.4/CNTs with the mass ratios of ZT0.6F1.4 to CNTs (mz/c)=l was up to 17.153 mg g-t for RhB, its adsorption behavior was in accord with Langmuir model, and its photocatalytic degradation activity on RhB had a positive correlation with the content of ZT0.6F1.4 in the sample. The experimental results indicate that the total removal rate of composite with rnz/c=l on RhB was more than 95% and the composite had good decontamination capability on industrial dye wastewater. In addition, the samples can be recovered conveniently, activated easily and had good performance for recycling.
基金supported by the National Natural Science Foundation of China(21822601,22176029)Excellent Youth Foundation of Sichuan Scientific Committee(2021JDJQ0006)+1 种基金Fundamental Research Funds for the Central Universities(ZYGX2019Z021)111 Project(B20030)。
文摘Dynamic defects on halide perovskite materials,caused by ion dissociation and migration under light illumination,typically result in undesirable energy dissipation and limited energy conversion efficiency.However,in this work,we demonstrated that dynamic halogen defects generated by the same process in bismuth oxyhalide(Bi_(5)O_(7)Cl)materials can act as active sites to promote charge separation and photocatalytic efficiency.Mechanistic studies and density functional theory calculations revealed that dynamic Cl defects affected the electronic structure of Bi_(5)O_(7)Cl and photocatalytic CO_(2)reduction process.As active sites,these defects promoted charge transfer,leading to the activation of adsorbed CO_(2)molecules and reduction of the energy barrier of the rate-determining step.Thus,CO_(2)was spontaneously converted into COOH−intermediate and finally reduced to CO with a high efficiency of 108.60μmol g^(−1) and selectivity of 100%after 4-h of CO_(2)photoreduction.This work is highly instructive and valuable to the exploration of dynamic defects on halide-containing materials applied in solar energy conversion.