Developing an efficient photocatalytic system for hydrogen peroxide(H_(2)O_(2))activation in Fenton-like processes holds significant promise for advancing water purification technologies.However,challenges such as hig...Developing an efficient photocatalytic system for hydrogen peroxide(H_(2)O_(2))activation in Fenton-like processes holds significant promise for advancing water purification technologies.However,challenges such as high carrier recombination rates,limited active sites,and suboptimal H_(2)O_(2)activation efficiency impede optimal performance.Here we show that single-iron-atom dispersed Bi_(2)WO_(6)monolayers(SIAD-BWOM),designed through a facile hydrothermal approach,can offer abundant active sites for H_(2)O_(2)activation.The SIAD-BWOM catalyst demonstrates superior photo-Fenton degradation capabilities,particularly for the persistent pesticide dinotefuran(DNF),showcasing its potential in addressing recalcitrant organic pollutants.We reveal that the incorporation of iron atoms in place of tungsten within the electron-rich[WO_(4)]^(2-)layers significantly facilitates electron transfer processes and boosts the Fe(II)/Fe(III)cycle efficiency.Complementary experimental investigations and theoretical analyses further elucidate how the atomically dispersed iron induces lattice strain in the Bi_(2)WO_(6)monolayer,thereby modulating the d-band center of iron to improve H_(2)O_(2)adsorption and activation.Our research provides a practical framework for developing advanced photo-Fenton catalysts,which can be used to treat emerging and refractory organic pollutants more effectively.展开更多
Developing an excellent photocatalysis system to remove pesticides from water is an urgent problem in current environment purification field.Herein,a Z-scheme WO_(3)/g-C_(3)N_(4) photocatalyst was prepared by a facile...Developing an excellent photocatalysis system to remove pesticides from water is an urgent problem in current environment purification field.Herein,a Z-scheme WO_(3)/g-C_(3)N_(4) photocatalyst was prepared by a facile in-situ calcination method,and the photocatalytic activity was investigated for degradation of nitenpyram(NTP)under visible light.The optimal Z-scheme WO_(3)/g-C_(3)N_(4) photocatalyst displayed the highest rate constant(0.036 min-1),which is about 1.7 and 25 times higher than that of pure g-C_(3)N_(4) and WO_(3),respectively.The improvement of photocatalytic performance is attributed to fast transfer of photogene rated carriers in the Z-scheme structure,which are testified by electron spin resonance(ESR)experiments,photocurrent and electrochemical impedance spectra(EIS)measurements.Moreover,the effects of typical water environmental factors on the degradation NTP were systematically studied.And the possible degradation pathways of NTP were deduced by the intermediates detected by highperformance liquid chro matography-mass spectrometry(HPLC-MS).This work will not only contribute to understand the degradation mechanism of pesticides in real water environmental condition,but also promote the development of new technologies for pesticide pollution control as well as environmental remediation.展开更多
Photoabsorption charge separation/transfer and surface reaction are the three main factors influencing the efficiency of photocatalysis.Band structure engineering has been extensively applied to improve the light abso...Photoabsorption charge separation/transfer and surface reaction are the three main factors influencing the efficiency of photocatalysis.Band structure engineering has been extensively applied to improve the light absorption of photocatalysts,however,most of the developed photocatalysts still suffer from low photocatalytic performance due to the limited active site(s)and fast recombination of photogenerated charge carriers.In this work,atomically dispersed main group magnesium(Mg)is introduced onto CdS monodispersed nanospheres,which greatly enhances the photocatalytic hydrogen evolution reaction.The photocatalytic hydrogen evolution reaction rate reaches 30.6 mmol·gcatalyst^(-1)·h^(-1),which is about 11.8 and 2.5 times that of pure CdS and Pt(2 wt.%)-CdS.The atomically dispersed Mg on CdS acts as an electron sink to trap photogenerated electrons,and at the same time,greatly reduces the Gibbs free energy of hydrogen evolution reaction(HER)and accelerates HER.展开更多
Low dimension nano photocatalysts show great potential in the field of treating contaminated water for their large surface area and size effect.In this study,a 0 D/1 D AgI/MoO_(3)Z-scheme photocatalyst with striking p...Low dimension nano photocatalysts show great potential in the field of treating contaminated water for their large surface area and size effect.In this study,a 0 D/1 D AgI/MoO_(3)Z-scheme photocatalyst with striking photocatalytic performance was constructed successfully.The one-dimensional MoO_(3)nanobelts were prepared by a simple hydrothermal method,and then it was modified by AgI nanoparticles in a handy deposition approach.When choosing sulfamethoxazole(SMZ)as the target contaminant,the rate constant value of the optimal 0 D/1 D AgI/MoO_(3)composite could hit up to 0.13 min^(-1),which is nearly 22.4 times and 32.5 times as that of pure MoO_(3)(0.0058 min^(-1))and AgI(0.0040 min^(-1)),respectively.A series of detailed characterizations give evidences that the charge transfer in the composite followed Z scheme mechanism.Therefore,efficient separation/transfer and the remained high redox activity of photogenerated carriers played a vital role in the sharply enhanced photocatalytic properties.The possible degradation pathways of SMZ were proposed based on the intermediates detected by high-performance liquid chromatography-mass spectrometry(HPLC-MS).Meanwhile,the magnificent cyclic stability makes the material a promising material in the practical application.展开更多
The quasi-homogeneous photocatalytic system can be formed by iodide ions induced fragmented and ultrathin structured TP-PCN.The TP-PCN possesses abundant edge active sites,which can greatly enhance the O_(2)adsorption...The quasi-homogeneous photocatalytic system can be formed by iodide ions induced fragmented and ultrathin structured TP-PCN.The TP-PCN possesses abundant edge active sites,which can greatly enhance the O_(2)adsorption/activation capacity and the 2e-ORR selectivity.As expected,the quasi-homogeneous system affords a remarkably increased photocatalytic H_(2)O_(2)production activity.展开更多
TiO2 films have received increasing attention for the removal of organic pollutants via photocatalysis. To develop a simple and effective method for improving the photodegradation efficiency of pollutants in surface w...TiO2 films have received increasing attention for the removal of organic pollutants via photocatalysis. To develop a simple and effective method for improving the photodegradation efficiency of pollutants in surface water, we herein examined the preparation of a P25-TiO2 composite film on a cement substrate via a sol–gel method. In this case, Rhodamine B（Rh B）was employed as the target organic pollutant. The self-generated TiO2 film and the P25-TiO2 composite film were characterized by X-ray diffraction（XRD）, N2 adsorption/desorption measurements, scanning electron microscopy（SEM）, transmission electron microscopy（TEM）, and diffuse reflectance spectroscopy（DRS）. The photodegradation efficiencies of the two films were studied by Rh B removal in water under UV（ultraviolet） irradiation. Over 4 day exposure, the P25-TiO2 composite film exhibited higher photocatalytic performance than the self-generated TiO2 film. The photodegradation rate indicated that the efficiency of the P25-TiO2 composite film was enhanced by the addition of the rutile phase Degussa P25 powder. As such, cooperation between the anatase TiO2 and rutile P25 nanoparticles was beneficial for separation of the photo-induced electrons and holes. In addition, the influence of P25 doping on the P25-TiO2 composite films was evaluated. We found that up to a certain saturation point, increased doping enhanced the photodegradation ability of the composite film. Thus, we herein demonstrated that the doping of P25 powders is a simple but effective strategy to prepare a P25-TiO2 composite film on a cement substrate, and the resulting film exhibits excellent removal efficiency in the degradation of organic pollutants.展开更多
Atrazine(ATZ),as one of the most extensively employed organochlorine-based herbicides,exhibits persistence and environmental toxicity.Photocatalytic technology based on polymer carbon nitride is regarded as a sus-tain...Atrazine(ATZ),as one of the most extensively employed organochlorine-based herbicides,exhibits persistence and environmental toxicity.Photocatalytic technology based on polymer carbon nitride is regarded as a sus-tainable and promising approach for the degradation of emerging organic pollutants.Regrettably,the inherent shortcomings of pure carbon nitride greatly limit its practical application.Herein,S-doped carbon nitride was elaborately constructed for efficient degradation of ATZ.The removal efficiency of ATZ by the optimal sample(0.052 min^(-1))is 3.25 times as that of pure carbon nitride(0.016 min^(-1)).Experiments and DFT calculations show that S doping optimizes electronic structure of carbon nitride,which significantly enhances the spatial separation and transfer efficiency of photogenerated electrons and holes.Moreover,the reactive sites and degradation paths of ATZ were predicted by Fukui function and LC-MS determination.Our work provides an effective approach for the design of efficient photocatalysts to achieve efficient environmental remediation.展开更多
基金financial support from the Natural Science Foundation of China(51979081,52100179)Fundamental Research Funds for the Central Universities(B200202103)+1 种基金National Science Funds for Creative Research Groups of China(No.51421006)PAPD and Photon Science Research center for Carbon Dioxide.
文摘Developing an efficient photocatalytic system for hydrogen peroxide(H_(2)O_(2))activation in Fenton-like processes holds significant promise for advancing water purification technologies.However,challenges such as high carrier recombination rates,limited active sites,and suboptimal H_(2)O_(2)activation efficiency impede optimal performance.Here we show that single-iron-atom dispersed Bi_(2)WO_(6)monolayers(SIAD-BWOM),designed through a facile hydrothermal approach,can offer abundant active sites for H_(2)O_(2)activation.The SIAD-BWOM catalyst demonstrates superior photo-Fenton degradation capabilities,particularly for the persistent pesticide dinotefuran(DNF),showcasing its potential in addressing recalcitrant organic pollutants.We reveal that the incorporation of iron atoms in place of tungsten within the electron-rich[WO_(4)]^(2-)layers significantly facilitates electron transfer processes and boosts the Fe(II)/Fe(III)cycle efficiency.Complementary experimental investigations and theoretical analyses further elucidate how the atomically dispersed iron induces lattice strain in the Bi_(2)WO_(6)monolayer,thereby modulating the d-band center of iron to improve H_(2)O_(2)adsorption and activation.Our research provides a practical framework for developing advanced photo-Fenton catalysts,which can be used to treat emerging and refractory organic pollutants more effectively.
基金financially supported by the National Science Funds for Creative Research Groups of China(No.51421006)National Natural Science Foundation of China(No.51679063)+2 种基金the Key Program of National Natural Science Foundation of China(No.91647206)the National key Plan for Research and Development of China(No.2016YFC0502203)A Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(No.51479064)。
文摘Developing an excellent photocatalysis system to remove pesticides from water is an urgent problem in current environment purification field.Herein,a Z-scheme WO_(3)/g-C_(3)N_(4) photocatalyst was prepared by a facile in-situ calcination method,and the photocatalytic activity was investigated for degradation of nitenpyram(NTP)under visible light.The optimal Z-scheme WO_(3)/g-C_(3)N_(4) photocatalyst displayed the highest rate constant(0.036 min-1),which is about 1.7 and 25 times higher than that of pure g-C_(3)N_(4) and WO_(3),respectively.The improvement of photocatalytic performance is attributed to fast transfer of photogene rated carriers in the Z-scheme structure,which are testified by electron spin resonance(ESR)experiments,photocurrent and electrochemical impedance spectra(EIS)measurements.Moreover,the effects of typical water environmental factors on the degradation NTP were systematically studied.And the possible degradation pathways of NTP were deduced by the intermediates detected by highperformance liquid chro matography-mass spectrometry(HPLC-MS).This work will not only contribute to understand the degradation mechanism of pesticides in real water environmental condition,but also promote the development of new technologies for pesticide pollution control as well as environmental remediation.
基金We are grateful for the financial support from the Natural Science Foundation of China(51979081)Fundamental Research Funds for the Central Universities(No.B200202103)+2 种基金Ministry of Education of Singapore(Tier 1:RG4/20 and Tier 2:MOET2EP10120-0002)Agency for Science,Technology and Research(AME IRG:A20E5c0080)PAPD。
文摘Photoabsorption charge separation/transfer and surface reaction are the three main factors influencing the efficiency of photocatalysis.Band structure engineering has been extensively applied to improve the light absorption of photocatalysts,however,most of the developed photocatalysts still suffer from low photocatalytic performance due to the limited active site(s)and fast recombination of photogenerated charge carriers.In this work,atomically dispersed main group magnesium(Mg)is introduced onto CdS monodispersed nanospheres,which greatly enhances the photocatalytic hydrogen evolution reaction.The photocatalytic hydrogen evolution reaction rate reaches 30.6 mmol·gcatalyst^(-1)·h^(-1),which is about 11.8 and 2.5 times that of pure CdS and Pt(2 wt.%)-CdS.The atomically dispersed Mg on CdS acts as an electron sink to trap photogenerated electrons,and at the same time,greatly reduces the Gibbs free energy of hydrogen evolution reaction(HER)and accelerates HER.
基金financially supported by the National Key Plan for Research and Development of China(No.2016YFC0502203)Natural Science Foundation of China(No.51979081)+3 种基金Fundamental Research Funds for the Central Universities(No.B200202103)National Science Funds for Creative Research Groups of China(No.51421006)the Key Program of National Natural Science Foundation of China(No.91647206)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘Low dimension nano photocatalysts show great potential in the field of treating contaminated water for their large surface area and size effect.In this study,a 0 D/1 D AgI/MoO_(3)Z-scheme photocatalyst with striking photocatalytic performance was constructed successfully.The one-dimensional MoO_(3)nanobelts were prepared by a simple hydrothermal method,and then it was modified by AgI nanoparticles in a handy deposition approach.When choosing sulfamethoxazole(SMZ)as the target contaminant,the rate constant value of the optimal 0 D/1 D AgI/MoO_(3)composite could hit up to 0.13 min^(-1),which is nearly 22.4 times and 32.5 times as that of pure MoO_(3)(0.0058 min^(-1))and AgI(0.0040 min^(-1)),respectively.A series of detailed characterizations give evidences that the charge transfer in the composite followed Z scheme mechanism.Therefore,efficient separation/transfer and the remained high redox activity of photogenerated carriers played a vital role in the sharply enhanced photocatalytic properties.The possible degradation pathways of SMZ were proposed based on the intermediates detected by high-performance liquid chromatography-mass spectrometry(HPLC-MS).Meanwhile,the magnificent cyclic stability makes the material a promising material in the practical application.
文摘The quasi-homogeneous photocatalytic system can be formed by iodide ions induced fragmented and ultrathin structured TP-PCN.The TP-PCN possesses abundant edge active sites,which can greatly enhance the O_(2)adsorption/activation capacity and the 2e-ORR selectivity.As expected,the quasi-homogeneous system affords a remarkably increased photocatalytic H_(2)O_(2)production activity.
基金supported by the National Science Funds for Creative Research Groups of China (No. 51421006)the National Major Projects of Water Pollution Control and Management Technology (No. 2017ZX07204003)+2 种基金the National Key Plan for Research and Development of China (2016YFC0502203)the Key Program of National Natural Science Foundation of China (No. 91647206)the Qing Lan Project of Jiangsu Province, and PAPD
文摘TiO2 films have received increasing attention for the removal of organic pollutants via photocatalysis. To develop a simple and effective method for improving the photodegradation efficiency of pollutants in surface water, we herein examined the preparation of a P25-TiO2 composite film on a cement substrate via a sol–gel method. In this case, Rhodamine B（Rh B）was employed as the target organic pollutant. The self-generated TiO2 film and the P25-TiO2 composite film were characterized by X-ray diffraction（XRD）, N2 adsorption/desorption measurements, scanning electron microscopy（SEM）, transmission electron microscopy（TEM）, and diffuse reflectance spectroscopy（DRS）. The photodegradation efficiencies of the two films were studied by Rh B removal in water under UV（ultraviolet） irradiation. Over 4 day exposure, the P25-TiO2 composite film exhibited higher photocatalytic performance than the self-generated TiO2 film. The photodegradation rate indicated that the efficiency of the P25-TiO2 composite film was enhanced by the addition of the rutile phase Degussa P25 powder. As such, cooperation between the anatase TiO2 and rutile P25 nanoparticles was beneficial for separation of the photo-induced electrons and holes. In addition, the influence of P25 doping on the P25-TiO2 composite films was evaluated. We found that up to a certain saturation point, increased doping enhanced the photodegradation ability of the composite film. Thus, we herein demonstrated that the doping of P25 powders is a simple but effective strategy to prepare a P25-TiO2 composite film on a cement substrate, and the resulting film exhibits excellent removal efficiency in the degradation of organic pollutants.
基金support from National Key Research and Development Program of China(2022YFC3202402)the Fundamental Research Funds for the Cornell University(B230205044)+2 种基金Natural Science Foundation of China(51979081,52100179)Fundamental Research Funds for the Central Universities(B200202103)PAPD,Postgraduate Research&Practice Innovation Program of Jiangsu Province.
文摘Atrazine(ATZ),as one of the most extensively employed organochlorine-based herbicides,exhibits persistence and environmental toxicity.Photocatalytic technology based on polymer carbon nitride is regarded as a sus-tainable and promising approach for the degradation of emerging organic pollutants.Regrettably,the inherent shortcomings of pure carbon nitride greatly limit its practical application.Herein,S-doped carbon nitride was elaborately constructed for efficient degradation of ATZ.The removal efficiency of ATZ by the optimal sample(0.052 min^(-1))is 3.25 times as that of pure carbon nitride(0.016 min^(-1)).Experiments and DFT calculations show that S doping optimizes electronic structure of carbon nitride,which significantly enhances the spatial separation and transfer efficiency of photogenerated electrons and holes.Moreover,the reactive sites and degradation paths of ATZ were predicted by Fukui function and LC-MS determination.Our work provides an effective approach for the design of efficient photocatalysts to achieve efficient environmental remediation.
