The sulfate radical-based photocatalytic process is supposed to be the most promising way to degrade organic pollutants.However,the development of a suitable and efficient photocatalyst is very challenging.The 40LaFeO...The sulfate radical-based photocatalytic process is supposed to be the most promising way to degrade organic pollutants.However,the development of a suitable and efficient photocatalyst is very challenging.The 40LaFeO_(3)-CuFe_(2)O_(4)(40LFO-CFO)nanocomposite was constructed and its catalytic performance was studied using Rhodamine B(RhB)as the target pollutant.40LFO-CFO exhibited excellent RhB degradation by the persulfate(PS)-assisted photocatalytic process compared to the pristine LFO and CFO.The degradation rate constant for RhB by 40LFO-CFO in the Vis/PS system was 2.22h^(-1)which is 3.04 times and 5.05 times higher than the pristine LFO(0.73 h^(-1))and CFO(0.44h^(-1)),respectively.Furthermore,the trapping experiments and EPR spectra proved that h^(+) plays a leading role in the bleaching of RhB for the 40LFO-CFO/PS/Vis system.The enhanced photocatalytic oxidation activity of 40LFO-CFO could be attributed to the unique charge carriers flow in 40LFO-CFO due to the Z-scheme and the cooperation effect between photocatalysis and PS activation.The recycle tests confessed the stability of 40LFO-CFO.Additionally,the intermediates and products of RhB are detected by liquid chromatographymass spectrometry(LC-MS),and the photocatalytic degradation routes of RhB for the 40LFO-CFO/Vis/PS system were proposed.Moreover,the 40LFO-CFO nanocomposite has a superior catalytic performance for other organics,suggesting that it is a promising heterocatalyst because of its high catalytic activity and stability for the PS-assisted photocatalytic process.展开更多
Fluorinated liquid crystal monomers(LCMs)are begun to emerge as new persistent organic pollutants.Herein,the structure-reactivity relationships of fluorinated LCMs 1,2,3-trifluoro-5-[3-(3-propylcyclohexyl)cyclohexyl]b...Fluorinated liquid crystal monomers(LCMs)are begun to emerge as new persistent organic pollutants.Herein,the structure-reactivity relationships of fluorinated LCMs 1,2,3-trifluoro-5-[3-(3-propylcyclohexyl)cyclohexyl]benzene(TPrCB),1,2-difluoro-4-[trans-4-(trans-4-propylcyclohexyl)cyclohexyl]benzene(DPrCB),4-[(trans,trans)-4'-(3-Buten-1-yl)[1,10-bicyclohexyl]-4-yl]-1,2-difluoro-benzene(BBDB)and 1-[4-(4-ethylcyclohexyl)cyclohexyl]-4(trifluoromethoxy)benzene(ECTB)subject to photocatalysis-generated oxidation species were investigated.The degradation rate constant of BBDB was 3.0,2.6,and 6.8 times higher than DPrCB,TPrCB and ECTB,respectively.The results reveal that BBDB,DPrCB and TPrCB had mainly negative electrostatic potential(ESP)regions which were vulnerable to electrophilic attack by h^(+),·OH and·O_(2)^(-),while ECTB was composed of mainly positive ESP regions which were vulnerable to nucleophilic attack by·OH and·O_(2)^(-).The detoxification processes of BBDB,DPrCB and TPrCB included carbon bond cleavage and benzene ring opening.However,the methoxy group of ECTB reduced the nucleophilic reactivity on the benzene ring,leading to slower detoxification efficiency.These findings may help to develop LCMs treatment technologies based on structure-reactivity relationships。展开更多
In this study, bismuth oxyhalide（Bi OXs（X_Cl, Br, I）） semiconductors were prepared by a simple solvothermal method, with ethanol serving as solvent and a series of tetrabutylammonium halide surfactants as halogen ...In this study, bismuth oxyhalide（Bi OXs（X_Cl, Br, I）） semiconductors were prepared by a simple solvothermal method, with ethanol serving as solvent and a series of tetrabutylammonium halide surfactants as halogen sources. Under identical synthetic conditions, Bi OBr was more readily constructed into regular flower-like hierarchical architectures. The photocatalytic properties of the materials were studied by monitoring the degradation of rhodamine B（Rh B）,with visible light absorption, and colorless salicylic acid（SA）. It was found that both Rh B and SA were rapidly degraded on the surface of Bi OBr. Bi OCl was rather active for the degradation of Rh B,but ineffective toward the degradation of SA. However, neither Rh B nor SA could be degraded effectively in the case of Bi OI. Further experiments such as UV–visible spectroscopy and detection of U OH and O2 Uradicals suggest that the electronic structure of the Bi OX photocatalysts is responsible for the difference in their activities.展开更多
In recent years, serious heavy oil pollution has frequently occurred in the ocean. Heavy oil has escaped from grounded oil carrier and drifted ashore. Drifted heavy oil contains hazardous chemical such as benzo （a） ...In recent years, serious heavy oil pollution has frequently occurred in the ocean. Heavy oil has escaped from grounded oil carrier and drifted ashore. Drifted heavy oil contains hazardous chemical such as benzo （a） pyrene and other poly aromatic hydrocarbons （PAHs）. These hazardous chemicals have worse affected on sea plants and animals. Thus, it is important to develop effective elimination of hazardous chemicals or drifted petroleum from sea shore. In this study, we have investigated the decomposition of benzo （a） pyrene on artificial sea water using UV/photocatalytic oxidation process. From this study, it was found that about 90% of benzo （a） pyrene on artificial seawater was decomposed by UV/photocatalytic oxidation process. And there were no by-product from decomposition of benzo （a） pyrene. It was supposed that benzo （a） pyrene was completely decomposed using UV/photocatalytic oxidation process.展开更多
Graphite-phase polymeric carbon nitride （CN） was reported to be a promising material in photoelectrochemical solar energy conversion. However, its high recombination rate of photogenerated carriers limits its potent...Graphite-phase polymeric carbon nitride （CN） was reported to be a promising material in photoelectrochemical solar energy conversion. However, its high recombination rate of photogenerated carriers limits its potential applications. In this article, a heterojunction of CN and sulfur-doped CN （CNS） was constructed through a solution-based processing way. Interestingly, it was observed that the photocatalytic hydrogen production of the as-prepared composite was 32.6 times higher than that of bulk carbon nitride and 2.3 times higher than that of the composites by conventional impregnating method. This study opens a new avenue to construct heterojunction of CN for large-scale industrial applications in environmental remediation.展开更多
Solar-driven photocatalytic hydrogen production via water splitting is considered as one of the most promising green and sustainable strategies,with the potential to replace traditional fossil fuels[1,2].Generally,thi...Solar-driven photocatalytic hydrogen production via water splitting is considered as one of the most promising green and sustainable strategies,with the potential to replace traditional fossil fuels[1,2].Generally,this photocatalytic reaction process includes the following steps:First,the semiconductor photocatalyst is photoexcited to generate photoinduced excitons on a femtosecond timescale.Next,the photoinduced excitons are separated into photogenerated electrons and holes,occurring within a femtosecond to picosecond timescale.Subsequently,only a small fraction of the photogenerated electrons and holes can overcome kinetic barriers,such as phonon scattering and bulk defects,to migrate to the surface。展开更多
Formaldehyde(HCHO)is formed through the oxidation of volatile organic compounds(VOCs)and can cause human cancer.Bismuth oxide and titanium oxide nanoparticles-functionalized nanographene oxide(Bi_(2)O_(3)/TiO_(2)@NGO)...Formaldehyde(HCHO)is formed through the oxidation of volatile organic compounds(VOCs)and can cause human cancer.Bismuth oxide and titanium oxide nanoparticles-functionalized nanographene oxide(Bi_(2)O_(3)/TiO_(2)@NGO)were used to rapidly remove the HCHO from the air by a photocatalytic degradation-adsorption process(PC-DAP).The formaldehyde vapor in pure air was generated in a dynamic system within a chamber,and flowed over Bi_(2)O_(3)/TiO_(2)@NGO adsorbent inside a fixed-bed quartz reactor(FBQR)under UV irradiation at optimized conditions(250C).At atmospheric pressure,the flow rate and gas hourly space velocity(GHSV)were adjusted to 300 mL/min and 100-450 L/h,respectively.The radicals of HCHO and nanographene oxide(NGO)were generated through the UV-photochemical process,enhancing the chemical adsorption through the radicals’interactions.On the other hand,the semi-degradation process by catalytic oxidation process converted some HCHO into raw materials of CO_(2)and H_(2)O,while the unconverted HCHO was physically absorbed by NGO.Finally,the HCHO concentration in the outlet system was measured by gas chromatography with a flame ionization detector(GC-FID)after derivatizing formaldehyde with 2,4-dinitrophenylhydrazine(DNPH)and acetonitrile.Therefore,efficient removal of HCHO from the air,the removal efficiency of more than 95%,was achieved through physical/chemical adsorption and the semi-degradation.The mean removal efficiencies for HCHO with Bi_(2)O_(3)-TiO_(2)@NGO,TiO_(2)@NGO,Bi_(2)O_(3)@NGO,and NGO were 98.7%,73.6%,61.8%,and 11.4%,respectively(n=10,RSD<5%).The methodology was validated by spiking different concentrations of standard HCHO into pure air.展开更多
Zinc oxide, which has photocatalytic activity, is used as white pigment for cosmetics. A certain degree of sebum on the skin is decomposed by ultraviolet radiation in sunlight. In this work, zinc oxide was shaken with...Zinc oxide, which has photocatalytic activity, is used as white pigment for cosmetics. A certain degree of sebum on the skin is decomposed by ultraviolet radiation in sunlight. In this work, zinc oxide was shaken with phosphoric acid to synthesize a white pigment for cosmetics. Zinc oxide was set with 0.1 mol/L of phosphoric acid at P/Zn = 1/1 and 1/2, and then shaking in hot water for 1 h. The chemical composition, powder properties, photocatalytic activity, color phase, and smoothness of the obtained powder were studied. The P/Zn ratio in preparation had an effect on the reaction between phosphoric acid and zinc oxide. The photocatalytic activity of zinc oxide was inhibited by phosphoric acid treatment. The obtained samples had enough high reflectance at the visible light region.展开更多
基金funded by the National Natural Science Foundation of China(52062047)the Innovation Capacity Support Plan of Shaanxi Province(2020TD-032)+2 种基金Yulin Science and Technology Plan(2019-81-1,CXY-2021-101-02 and 2023-CXY-154)Joint Fund of Clean Energy Innovation Institute of Chinese Academy of Sciences and Yulin University(YLUDNL202202)Yulin University Science and Technology Plan(2020TZRC01).
文摘The sulfate radical-based photocatalytic process is supposed to be the most promising way to degrade organic pollutants.However,the development of a suitable and efficient photocatalyst is very challenging.The 40LaFeO_(3)-CuFe_(2)O_(4)(40LFO-CFO)nanocomposite was constructed and its catalytic performance was studied using Rhodamine B(RhB)as the target pollutant.40LFO-CFO exhibited excellent RhB degradation by the persulfate(PS)-assisted photocatalytic process compared to the pristine LFO and CFO.The degradation rate constant for RhB by 40LFO-CFO in the Vis/PS system was 2.22h^(-1)which is 3.04 times and 5.05 times higher than the pristine LFO(0.73 h^(-1))and CFO(0.44h^(-1)),respectively.Furthermore,the trapping experiments and EPR spectra proved that h^(+) plays a leading role in the bleaching of RhB for the 40LFO-CFO/PS/Vis system.The enhanced photocatalytic oxidation activity of 40LFO-CFO could be attributed to the unique charge carriers flow in 40LFO-CFO due to the Z-scheme and the cooperation effect between photocatalysis and PS activation.The recycle tests confessed the stability of 40LFO-CFO.Additionally,the intermediates and products of RhB are detected by liquid chromatographymass spectrometry(LC-MS),and the photocatalytic degradation routes of RhB for the 40LFO-CFO/Vis/PS system were proposed.Moreover,the 40LFO-CFO nanocomposite has a superior catalytic performance for other organics,suggesting that it is a promising heterocatalyst because of its high catalytic activity and stability for the PS-assisted photocatalytic process.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(No.2020B1515020038)the Pearl River Talent Recruitment Program of Guangdong Province(2019QN01L148)+3 种基金the National Natural Science Foundation of China(21876063 and 22076064)the Guangdong Special Support Program(2019TX05L129)the Guangdong(China)Innovative and Entrepreneurial Research Team Program(2016ZT06N258)the Special Fund Project for Science and Technology Innovation Strategy of Guangdong Province(2019B121205004).
文摘Fluorinated liquid crystal monomers(LCMs)are begun to emerge as new persistent organic pollutants.Herein,the structure-reactivity relationships of fluorinated LCMs 1,2,3-trifluoro-5-[3-(3-propylcyclohexyl)cyclohexyl]benzene(TPrCB),1,2-difluoro-4-[trans-4-(trans-4-propylcyclohexyl)cyclohexyl]benzene(DPrCB),4-[(trans,trans)-4'-(3-Buten-1-yl)[1,10-bicyclohexyl]-4-yl]-1,2-difluoro-benzene(BBDB)and 1-[4-(4-ethylcyclohexyl)cyclohexyl]-4(trifluoromethoxy)benzene(ECTB)subject to photocatalysis-generated oxidation species were investigated.The degradation rate constant of BBDB was 3.0,2.6,and 6.8 times higher than DPrCB,TPrCB and ECTB,respectively.The results reveal that BBDB,DPrCB and TPrCB had mainly negative electrostatic potential(ESP)regions which were vulnerable to electrophilic attack by h^(+),·OH and·O_(2)^(-),while ECTB was composed of mainly positive ESP regions which were vulnerable to nucleophilic attack by·OH and·O_(2)^(-).The detoxification processes of BBDB,DPrCB and TPrCB included carbon bond cleavage and benzene ring opening.However,the methoxy group of ECTB reduced the nucleophilic reactivity on the benzene ring,leading to slower detoxification efficiency.These findings may help to develop LCMs treatment technologies based on structure-reactivity relationships。
基金supported by the National Natural Science Foundation of China (Nos. 21377067, 21177072, 21207079)Natural Science Foundation for Innovation Group of Hubei Province, China (No. 2009CDA020)open fund (KF2011-07) from the State Key Laboratory of Environmental Chemistry and Ecotoxicology, RCEES, CAS
文摘In this study, bismuth oxyhalide（Bi OXs（X_Cl, Br, I）） semiconductors were prepared by a simple solvothermal method, with ethanol serving as solvent and a series of tetrabutylammonium halide surfactants as halogen sources. Under identical synthetic conditions, Bi OBr was more readily constructed into regular flower-like hierarchical architectures. The photocatalytic properties of the materials were studied by monitoring the degradation of rhodamine B（Rh B）,with visible light absorption, and colorless salicylic acid（SA）. It was found that both Rh B and SA were rapidly degraded on the surface of Bi OBr. Bi OCl was rather active for the degradation of Rh B,but ineffective toward the degradation of SA. However, neither Rh B nor SA could be degraded effectively in the case of Bi OI. Further experiments such as UV–visible spectroscopy and detection of U OH and O2 Uradicals suggest that the electronic structure of the Bi OX photocatalysts is responsible for the difference in their activities.
文摘In recent years, serious heavy oil pollution has frequently occurred in the ocean. Heavy oil has escaped from grounded oil carrier and drifted ashore. Drifted heavy oil contains hazardous chemical such as benzo （a） pyrene and other poly aromatic hydrocarbons （PAHs）. These hazardous chemicals have worse affected on sea plants and animals. Thus, it is important to develop effective elimination of hazardous chemicals or drifted petroleum from sea shore. In this study, we have investigated the decomposition of benzo （a） pyrene on artificial sea water using UV/photocatalytic oxidation process. From this study, it was found that about 90% of benzo （a） pyrene on artificial seawater was decomposed by UV/photocatalytic oxidation process. And there were no by-product from decomposition of benzo （a） pyrene. It was supposed that benzo （a） pyrene was completely decomposed using UV/photocatalytic oxidation process.
基金financially supported in part by the National Natural Science Foundation of China(No. 21305065)Natural Science Foundation of Jiangsu Province(Nos. BK20160028, BK20170084)+1 种基金the Open Funds of the State Key Laboratory of Electroanalytical Chemistry (No. SKLEAC201703)the Fundamental Research Funds for the Central Universities
文摘Graphite-phase polymeric carbon nitride （CN） was reported to be a promising material in photoelectrochemical solar energy conversion. However, its high recombination rate of photogenerated carriers limits its potential applications. In this article, a heterojunction of CN and sulfur-doped CN （CNS） was constructed through a solution-based processing way. Interestingly, it was observed that the photocatalytic hydrogen production of the as-prepared composite was 32.6 times higher than that of bulk carbon nitride and 2.3 times higher than that of the composites by conventional impregnating method. This study opens a new avenue to construct heterojunction of CN for large-scale industrial applications in environmental remediation.
文摘Solar-driven photocatalytic hydrogen production via water splitting is considered as one of the most promising green and sustainable strategies,with the potential to replace traditional fossil fuels[1,2].Generally,this photocatalytic reaction process includes the following steps:First,the semiconductor photocatalyst is photoexcited to generate photoinduced excitons on a femtosecond timescale.Next,the photoinduced excitons are separated into photogenerated electrons and holes,occurring within a femtosecond to picosecond timescale.Subsequently,only a small fraction of the photogenerated electrons and holes can overcome kinetic barriers,such as phonon scattering and bulk defects,to migrate to the surface。
基金the Science and Research Branch,Islamic Azad Universitythe Research Institute of Petroleum Industry(RIPI)for supporting this work
文摘Formaldehyde(HCHO)is formed through the oxidation of volatile organic compounds(VOCs)and can cause human cancer.Bismuth oxide and titanium oxide nanoparticles-functionalized nanographene oxide(Bi_(2)O_(3)/TiO_(2)@NGO)were used to rapidly remove the HCHO from the air by a photocatalytic degradation-adsorption process(PC-DAP).The formaldehyde vapor in pure air was generated in a dynamic system within a chamber,and flowed over Bi_(2)O_(3)/TiO_(2)@NGO adsorbent inside a fixed-bed quartz reactor(FBQR)under UV irradiation at optimized conditions(250C).At atmospheric pressure,the flow rate and gas hourly space velocity(GHSV)were adjusted to 300 mL/min and 100-450 L/h,respectively.The radicals of HCHO and nanographene oxide(NGO)were generated through the UV-photochemical process,enhancing the chemical adsorption through the radicals’interactions.On the other hand,the semi-degradation process by catalytic oxidation process converted some HCHO into raw materials of CO_(2)and H_(2)O,while the unconverted HCHO was physically absorbed by NGO.Finally,the HCHO concentration in the outlet system was measured by gas chromatography with a flame ionization detector(GC-FID)after derivatizing formaldehyde with 2,4-dinitrophenylhydrazine(DNPH)and acetonitrile.Therefore,efficient removal of HCHO from the air,the removal efficiency of more than 95%,was achieved through physical/chemical adsorption and the semi-degradation.The mean removal efficiencies for HCHO with Bi_(2)O_(3)-TiO_(2)@NGO,TiO_(2)@NGO,Bi_(2)O_(3)@NGO,and NGO were 98.7%,73.6%,61.8%,and 11.4%,respectively(n=10,RSD<5%).The methodology was validated by spiking different concentrations of standard HCHO into pure air.
文摘Zinc oxide, which has photocatalytic activity, is used as white pigment for cosmetics. A certain degree of sebum on the skin is decomposed by ultraviolet radiation in sunlight. In this work, zinc oxide was shaken with phosphoric acid to synthesize a white pigment for cosmetics. Zinc oxide was set with 0.1 mol/L of phosphoric acid at P/Zn = 1/1 and 1/2, and then shaking in hot water for 1 h. The chemical composition, powder properties, photocatalytic activity, color phase, and smoothness of the obtained powder were studied. The P/Zn ratio in preparation had an effect on the reaction between phosphoric acid and zinc oxide. The photocatalytic activity of zinc oxide was inhibited by phosphoric acid treatment. The obtained samples had enough high reflectance at the visible light region.
