The CeO_(2)-TiO_(2)@MnO_(x) catalyst was prepared by the co-precipitation method and applied to the photothermocatalysis system of ethyl acetate and NO simultaneous degradation under H_(2)O at low temperature,which in...The CeO_(2)-TiO_(2)@MnO_(x) catalyst was prepared by the co-precipitation method and applied to the photothermocatalysis system of ethyl acetate and NO simultaneous degradation under H_(2)O at low temperature,which introduced Ce into TiO_(2)@MnO_(x) hollow sptrera structure.The optimum TiO_(2)/MnO_(x) ratio and Ce introducing amount were obtained in the process.Among of them,the NO and ethyl acetate conversion percentage of TiO_(2)@MnO_(x)(n_(Mn):n_(Ti)=40:40)is 74%and 62%at 240℃,respectively.CeO_(2)-TiO_(2)@MnO_(x)(n_(Mn):n_(Ce)=1:1)exhibits the best catalytic performance,its efficiency for NO conversion is 83%and the conversion of ethyl acetate reaches 72%at 240℃.In addition,it is confirmed that the Cedoped nanocomposites have more uniform dispersion through various characterization and analysis methods.Meanwhile,these catalysts have a large specific surface area as well as a large number of surface-active oxygen and oxygen vacancies.It can further improve the catalytic performance based on the adjusted ratio of active components.Moreover,this work investigated the relationship between multi-metal interactions and catalytic performance in the presence of H_(2)O.Finally,the possible reaction pathways for the simultaneous removal of NO and ethyl acetate were explored in our system.展开更多
Solar-driven CO_(2)-to-fuel conversion assisted by another major greenhouse gas CH_(4)is promising to concurrently tackle energy shortage and global warming problems.However,current techniques still suffer from drawba...Solar-driven CO_(2)-to-fuel conversion assisted by another major greenhouse gas CH_(4)is promising to concurrently tackle energy shortage and global warming problems.However,current techniques still suffer from drawbacks of low efficiency,poor stability,and low selectivity.Here,a novel nanocomposite composed of interconnected Ni/MgAlOx nanoflakes grown on SiO_(2)particles with excellent spatial confinement of active sites is proposed for direct solar-driven CO_(2)-to-fuel conversion.An ultrahigh light-to-fuel efficiency up to 35.7%,high production rates of H_(2)(136.6 mmol min^(-1)g^(-1))and CO(148.2 mmol min^(-1)g^(-1)),excellent selectivity(H_(2)/CO ratio of 0.92),and good stability are reported simultaneously.These outstanding performances are attributed to strong metal-support interactions,improved CO_(2)absorption and activation,and decreased apparent activation energy under direct light illumination.MgAlO_(x)@SiO_(2)support helps to lower the activation energy of CH^(*) oxidation to CHO^(*) and improve the dissociation of CH_(4)to CH_(3)^(*) as confirmed by DFT calculations.Moreover,the lattice oxygen of MgAlO_(x) participates in the reaction and contributes to the removal of carbon deposition.This work provides promising routes for the conversion of greenhouse gasses into industrially valuable syngas with high efficiency,high selectivity,and benign sustainability.展开更多
In this study,bismuth oxyiodide with coexistence of plasmonic Bi and oxygen vacancy(Bi/BiO_(1-x)I)was successfully prepared and used towards photothermal and photocatalytic disinfection of pathogenic bacteria containi...In this study,bismuth oxyiodide with coexistence of plasmonic Bi and oxygen vacancy(Bi/BiO_(1-x)I)was successfully prepared and used towards photothermal and photocatalytic disinfection of pathogenic bacteria containing water.Plasmonic Bi and oxygen vacancies in Bi/BiO_(1-x)I induced a surface plasmon effect under the irradiation of simulated solar light from 500-900 nm and promoted the generation of hot electrons and reactive species(^(1)O^(2),h^(+)and·O_(2)^(-)).The catalyst showed promising performance for inactivation of E.coli K-12,with a 7.2 log inactivated achieved under the optimum conditions.A synergy between photothermal and photocatalytic inactivation was identified and discussed.The mechanisms of E.coli K-12 destruction were investigated.The destruction of extracellular antioxidant enzymes of E.coli K-12 was identified after inactivation.Moreover,the E.coli's membrane and its intracellular contents were attacked by the reactive species(^(1)O^(2),h^(+)and·O_(2)^(-))and the thermal effects.This work provides useful insights into the rational design of semimetal bismuth-mediated photocatalysts towards effective and sustainable water disinfection.展开更多
基金Project supported by the Foundation of Guangxi Science and Technology of Base&Talent Special Program(AD20159067)Guangxi Key Laboratory of Environmental Pollution Control Theory and Technology(2101Z002)。
文摘The CeO_(2)-TiO_(2)@MnO_(x) catalyst was prepared by the co-precipitation method and applied to the photothermocatalysis system of ethyl acetate and NO simultaneous degradation under H_(2)O at low temperature,which introduced Ce into TiO_(2)@MnO_(x) hollow sptrera structure.The optimum TiO_(2)/MnO_(x) ratio and Ce introducing amount were obtained in the process.Among of them,the NO and ethyl acetate conversion percentage of TiO_(2)@MnO_(x)(n_(Mn):n_(Ti)=40:40)is 74%and 62%at 240℃,respectively.CeO_(2)-TiO_(2)@MnO_(x)(n_(Mn):n_(Ce)=1:1)exhibits the best catalytic performance,its efficiency for NO conversion is 83%and the conversion of ethyl acetate reaches 72%at 240℃.In addition,it is confirmed that the Cedoped nanocomposites have more uniform dispersion through various characterization and analysis methods.Meanwhile,these catalysts have a large specific surface area as well as a large number of surface-active oxygen and oxygen vacancies.It can further improve the catalytic performance based on the adjusted ratio of active components.Moreover,this work investigated the relationship between multi-metal interactions and catalytic performance in the presence of H_(2)O.Finally,the possible reaction pathways for the simultaneous removal of NO and ethyl acetate were explored in our system.
基金This work was financially supported by the Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China(51888103)the National Key R&D Program of China(2021YFF0500700)Jiangsu Natural Science Foundation Project(BE2022024 and BK20202008).
文摘Solar-driven CO_(2)-to-fuel conversion assisted by another major greenhouse gas CH_(4)is promising to concurrently tackle energy shortage and global warming problems.However,current techniques still suffer from drawbacks of low efficiency,poor stability,and low selectivity.Here,a novel nanocomposite composed of interconnected Ni/MgAlOx nanoflakes grown on SiO_(2)particles with excellent spatial confinement of active sites is proposed for direct solar-driven CO_(2)-to-fuel conversion.An ultrahigh light-to-fuel efficiency up to 35.7%,high production rates of H_(2)(136.6 mmol min^(-1)g^(-1))and CO(148.2 mmol min^(-1)g^(-1)),excellent selectivity(H_(2)/CO ratio of 0.92),and good stability are reported simultaneously.These outstanding performances are attributed to strong metal-support interactions,improved CO_(2)absorption and activation,and decreased apparent activation energy under direct light illumination.MgAlO_(x)@SiO_(2)support helps to lower the activation energy of CH^(*) oxidation to CHO^(*) and improve the dissociation of CH_(4)to CH_(3)^(*) as confirmed by DFT calculations.Moreover,the lattice oxygen of MgAlO_(x) participates in the reaction and contributes to the removal of carbon deposition.This work provides promising routes for the conversion of greenhouse gasses into industrially valuable syngas with high efficiency,high selectivity,and benign sustainability.
基金financially supported by the National Natural Science Foundation of China(Nos.21876212,21976214,41603097,21673086 and 52070195)the Science and Technology Research Programs of Guangdong Province(No.2019A1515011015)+2 种基金the Science and Technology Program of Guangzhou(No.201904010353)the Fundamental Research Funds for the Central Universities(No.19lgpy157)supported by the Start-up Funds for High-Level Talents of Sun Yat-sen University(No.3800018821111)。
文摘In this study,bismuth oxyiodide with coexistence of plasmonic Bi and oxygen vacancy(Bi/BiO_(1-x)I)was successfully prepared and used towards photothermal and photocatalytic disinfection of pathogenic bacteria containing water.Plasmonic Bi and oxygen vacancies in Bi/BiO_(1-x)I induced a surface plasmon effect under the irradiation of simulated solar light from 500-900 nm and promoted the generation of hot electrons and reactive species(^(1)O^(2),h^(+)and·O_(2)^(-)).The catalyst showed promising performance for inactivation of E.coli K-12,with a 7.2 log inactivated achieved under the optimum conditions.A synergy between photothermal and photocatalytic inactivation was identified and discussed.The mechanisms of E.coli K-12 destruction were investigated.The destruction of extracellular antioxidant enzymes of E.coli K-12 was identified after inactivation.Moreover,the E.coli's membrane and its intracellular contents were attacked by the reactive species(^(1)O^(2),h^(+)and·O_(2)^(-))and the thermal effects.This work provides useful insights into the rational design of semimetal bismuth-mediated photocatalysts towards effective and sustainable water disinfection.