Carbon-based adsorption and TiO_(2)-based photocatalysis are both safe and low-cost ways of pollutant pu-rification.Constructing C-TiO_(2)architectures can effectively improve removal efficiency.However,most of those ...Carbon-based adsorption and TiO_(2)-based photocatalysis are both safe and low-cost ways of pollutant pu-rification.Constructing C-TiO_(2)architectures can effectively improve removal efficiency.However,most of those carbon frames only acted as supporting substrates,exhibiting rather limited synergistic action from TiO_(2)and carbon.Herein,Fe/N co-doped nano-TiO_(2)wrapped on mesoporous carbon spheres with a core-shell structure was designed.The Fe,N co-doped carbon sphere with a hierarchical structure im-proved the synergy of adsorption and transfer during the photocatalytic process.Without extra dopant,the Fe and N partly exposed on the surface realized the in-situ migrating into the TiO_(2)shell to en-hance the interface effect,which significantly promoted the photocatalytic efficiency of the composite.Furthermore,the photocatalytic efficiency of the composite was investigated through two typical pollu-tants under visible-light irradiation.The degradation efficiencies for rhodamine B and paraxylene were 96.2%in 60 min and 94.1%in 20 min,respectively,with the apparent rate constant of 0.045 min^(-1)and 0.049 min^(-1),8.3 and 11.4 times of that for bare TiO_(2).The composite is likely advantageous for treating diverse environmental pollutants.展开更多
Adsorption and the combination of adsorption and photocatalysis are prospective strategies for treating lowconcentrationvolatile organic compounds (VOCs). Behind the adsorption technology of VOC treatments are carbon-...Adsorption and the combination of adsorption and photocatalysis are prospective strategies for treating lowconcentrationvolatile organic compounds (VOCs). Behind the adsorption technology of VOC treatments are carbon-basedmaterials with large surface areas and high VOC uptake. This review summarizes the research progress in carbon-basedadsorbents and adsorbent-photocatalysts for VOC removal. Firstly, the VOC adsorption performances of various carbonmaterials, including activated carbon, activated carbon fiber, biochar, graphene and its derivatives, and carbon nanotubes,are summarized, and the adsorption mechanism of VOCs on carbon materials is analyzed. Then, the VOC adsorptionphotocatalyticproperties of composites comprised of different carbon materials and photocatalysts are presented. Finally,perspectives on the adsorption and adsorption-photocatalysis of VOCs via carbon materials are proposed. This reviewprovides an optimal reference for the research and development of adsorbents and adsorption-photocatalysts of VOCs.展开更多
The extraction of uranium from seawater is challenging though it offers tremendous potential for the sustainable production of nuclear fuel for the energy sector.Herein,we report a new strategy for efficient extractio...The extraction of uranium from seawater is challenging though it offers tremendous potential for the sustainable production of nuclear fuel for the energy sector.Herein,we report a new strategy for efficient extraction of uranium from seawater via converging the cooperative functions of adsorption-photocatalysis into the nanospace of covalent organic frameworks(COFs).Functionalization of the organic linkers in the multicomponent COFs allowed exploration of the relationship between material composition and adsorption-photocatalytic activity for uranium extraction.The presence of amidoxime groups in the COFs offered selective binding sites for uranyl,whilst triazine units and bipyridine-Pd groups acted cooperatively to photocatalytically reduce adsorbed U(Ⅵ)to a U(Ⅳ)solid product(UO2)for facile collection.One of our developed COFs,4-Pd-AO,displayed exceptional performance in sequestering and reducing uranyl from natural seawater,with a high extraction capacity of 4.62 mg U/g per day(average data)under visible light irradiation.Mechanistic studies revealed that 4-Pd-AO not only reduced adsorbed uranyl(Ⅵ)to U(Ⅳ)O_(2),but also generated ^(1)O_(2) and superoxide radicals under visible light excitation,thus affording excellent antibacterial and antialgal activities(i.e.,antibiofouling properties)for sustained efficient uranium extraction performance.This proof-ofconcept study establishes multicomponent COFs as promising candidates for efficient uranium extraction from seawater.展开更多
基金The work was supported by the National Natural Science Foun-dation of China(No.21974057).
文摘Carbon-based adsorption and TiO_(2)-based photocatalysis are both safe and low-cost ways of pollutant pu-rification.Constructing C-TiO_(2)architectures can effectively improve removal efficiency.However,most of those carbon frames only acted as supporting substrates,exhibiting rather limited synergistic action from TiO_(2)and carbon.Herein,Fe/N co-doped nano-TiO_(2)wrapped on mesoporous carbon spheres with a core-shell structure was designed.The Fe,N co-doped carbon sphere with a hierarchical structure im-proved the synergy of adsorption and transfer during the photocatalytic process.Without extra dopant,the Fe and N partly exposed on the surface realized the in-situ migrating into the TiO_(2)shell to en-hance the interface effect,which significantly promoted the photocatalytic efficiency of the composite.Furthermore,the photocatalytic efficiency of the composite was investigated through two typical pollu-tants under visible-light irradiation.The degradation efficiencies for rhodamine B and paraxylene were 96.2%in 60 min and 94.1%in 20 min,respectively,with the apparent rate constant of 0.045 min^(-1)and 0.049 min^(-1),8.3 and 11.4 times of that for bare TiO_(2).The composite is likely advantageous for treating diverse environmental pollutants.
文摘Adsorption and the combination of adsorption and photocatalysis are prospective strategies for treating lowconcentrationvolatile organic compounds (VOCs). Behind the adsorption technology of VOC treatments are carbon-basedmaterials with large surface areas and high VOC uptake. This review summarizes the research progress in carbon-basedadsorbents and adsorbent-photocatalysts for VOC removal. Firstly, the VOC adsorption performances of various carbonmaterials, including activated carbon, activated carbon fiber, biochar, graphene and its derivatives, and carbon nanotubes,are summarized, and the adsorption mechanism of VOCs on carbon materials is analyzed. Then, the VOC adsorptionphotocatalyticproperties of composites comprised of different carbon materials and photocatalysts are presented. Finally,perspectives on the adsorption and adsorption-photocatalysis of VOCs via carbon materials are proposed. This reviewprovides an optimal reference for the research and development of adsorbents and adsorption-photocatalysts of VOCs.
基金funding support from the National Science Foundation of China(grant nos.U2167218 and 22006036)National Key Research and Development Program of China(grant nos.2017YFA0207002 and 2018YFC1900105)+4 种基金the Science Challenge Project(grant no.TZ2016004)the Beijing Outstanding Young Scientist Programthe Students Innovation Training Program(grant no.202106014)the Robert A.Welch Foundation(B-0027)(S.M.)support from the 14W station in Shanghai Synchrotron Radiation Facility(SSRF).
文摘The extraction of uranium from seawater is challenging though it offers tremendous potential for the sustainable production of nuclear fuel for the energy sector.Herein,we report a new strategy for efficient extraction of uranium from seawater via converging the cooperative functions of adsorption-photocatalysis into the nanospace of covalent organic frameworks(COFs).Functionalization of the organic linkers in the multicomponent COFs allowed exploration of the relationship between material composition and adsorption-photocatalytic activity for uranium extraction.The presence of amidoxime groups in the COFs offered selective binding sites for uranyl,whilst triazine units and bipyridine-Pd groups acted cooperatively to photocatalytically reduce adsorbed U(Ⅵ)to a U(Ⅳ)solid product(UO2)for facile collection.One of our developed COFs,4-Pd-AO,displayed exceptional performance in sequestering and reducing uranyl from natural seawater,with a high extraction capacity of 4.62 mg U/g per day(average data)under visible light irradiation.Mechanistic studies revealed that 4-Pd-AO not only reduced adsorbed uranyl(Ⅵ)to U(Ⅳ)O_(2),but also generated ^(1)O_(2) and superoxide radicals under visible light excitation,thus affording excellent antibacterial and antialgal activities(i.e.,antibiofouling properties)for sustained efficient uranium extraction performance.This proof-ofconcept study establishes multicomponent COFs as promising candidates for efficient uranium extraction from seawater.