Photothermal synergistic catalytic systems for treating volatile organic compounds(VOCs)have attracted signif-icant attention due to their energy efficiency and potential to reduce carbon emissions.However,the mechani...Photothermal synergistic catalytic systems for treating volatile organic compounds(VOCs)have attracted signif-icant attention due to their energy efficiency and potential to reduce carbon emissions.However,the mechanism underlying the synergistic reaction remains a critical issue.This study introduces a photothermal synergistic system for the removal of ethyl acetate(EA)by synthesizing Cu-doped OMS-2(denoted as Cu-OMS-2).Under ultraviolet-visible(UV–Vis)irradiation in a flow system,the Cu-OMS-2 catalyst exhibited significantly enhanced performance in the EA degradation process,nearly doubling the effectiveness of pure OMS-2,and increasing carbon dioxide yield by 20%.This exceptional performance is attributed to the synergistic effect of increased oxygen vacancies(OV)at OMS-2 active sites and Cu doping,as confirmed by H2-TPR,O_(2)-TPD,and CO consump-tion measurements.This study clarifies the catalytic mechanism of light-assisted thermocatalysis and offers a novel strategy for designing photothermal catalysts with homogeneous Cu-doped nanorods for VOC removal.展开更多
OMS-2 nanorod catalysts were synthesized by a hydrothermal redox reaction method using Mn SO4（OMS-2-SO4） and Mn（CH3COO）2（OMS-2-AC） as precursors. SO4^2--doped OMS-2-AC catalysts with different SO4^2-concentratio...OMS-2 nanorod catalysts were synthesized by a hydrothermal redox reaction method using Mn SO4（OMS-2-SO4） and Mn（CH3COO）2（OMS-2-AC） as precursors. SO4^2--doped OMS-2-AC catalysts with different SO4^2-concentrations were prepared next by adding（NH4）2SO4solution into OMS-2-AC samples to investigate the effect of the anion SO4^2-on the OMS-2-AC catalyst. All catalysts were then tested for the catalytic oxidation of ethanol. The OMS-2-SO4 catalyst synthesized demonstrated much better activity than OMS-2-AC. The SO4^2-doping greatly influenced the activity of the OMS-2-AC catalyst, with a dramatic promotion of activity for suitable concentration of SO4^2-（SO4/catalyst = 0.5% W/W）. The samples were characterized by X-ray diffraction（XRD）, field emission scanning electron microscopy（FE-SEM）, transmission electron microscopy（TEM）, X-ray photoelectron spectroscopy（XPS）,inductively coupled plasma optical emission spectroscopy（ICP-OES）, NH3-TPD and H2-TPR techniques. The results showed that the presence of a suitable amount of SO4^2-species in the OMS-2-AC catalyst could decrease the Mn–O bond strength and also enhance the lattice oxygen and acid site concentrations, which then effectively promoted the catalytic activity of OMS-2-AC toward ethanol oxidation. Thus it was confirmed that the better catalytic performance of OMS-2-SO4 compared to OMS-2-AC is due to the presence of some residual SO4^2-species in OMS-2-SO4 samples.展开更多
In this study,Mn catalysts have been designed based on manganese oxide octahedral molecular sieve(OMS-2) supports to optimize the catalytic activity in the degradation of organic pollutants.Herein,two different synthe...In this study,Mn catalysts have been designed based on manganese oxide octahedral molecular sieve(OMS-2) supports to optimize the catalytic activity in the degradation of organic pollutants.Herein,two different synthetic strategies:Pre-incorporation vs.wet-impregnation have been employed to synthesize[PW]-OMS-2 and [PW]/OMS-2.For [PW]-OMS-2,energy dispersive X-ray spectroscopy(EDX) confirmed that dispersed granular phosphotungstic acid attached and located at the surface of OMS-2,meanwhile some W atoms have been doped into frameworks of OMS-2.However,for [PW]/OMS-2,the W atoms cannot enter the OMS-2 frameworks.A correlation has been established between the different synthetic strategies and catalytic activities.The [PW]-OMS-2 is the most highly effective and stable over than[PW]/OMS-2 and OMS-2 itself for the organic pollutants removal.This may be caused not only by the synergetic effect of [PW] and OMS-2,but also by doping W into frameworks of OMS-2.Therefore,this work provides a new environmentally-friendly and heterogeneous PMS activator and it may be put into practice to degrade organic pollutants.展开更多
基金supported by the Qilu University of Technology(Shandong Academy of Sciences),the Basic Research Project of Science,Education and Industry Integration Pilot Project(No.2022PY047).
文摘Photothermal synergistic catalytic systems for treating volatile organic compounds(VOCs)have attracted signif-icant attention due to their energy efficiency and potential to reduce carbon emissions.However,the mechanism underlying the synergistic reaction remains a critical issue.This study introduces a photothermal synergistic system for the removal of ethyl acetate(EA)by synthesizing Cu-doped OMS-2(denoted as Cu-OMS-2).Under ultraviolet-visible(UV–Vis)irradiation in a flow system,the Cu-OMS-2 catalyst exhibited significantly enhanced performance in the EA degradation process,nearly doubling the effectiveness of pure OMS-2,and increasing carbon dioxide yield by 20%.This exceptional performance is attributed to the synergistic effect of increased oxygen vacancies(OV)at OMS-2 active sites and Cu doping,as confirmed by H2-TPR,O_(2)-TPD,and CO consump-tion measurements.This study clarifies the catalytic mechanism of light-assisted thermocatalysis and offers a novel strategy for designing photothermal catalysts with homogeneous Cu-doped nanorods for VOC removal.
基金financially supported by the National Natural Science Foundation of China (No. 21422706)the Program of the Ministry of Science and Technology of China (No. 2012AA062702)
文摘OMS-2 nanorod catalysts were synthesized by a hydrothermal redox reaction method using Mn SO4（OMS-2-SO4） and Mn（CH3COO）2（OMS-2-AC） as precursors. SO4^2--doped OMS-2-AC catalysts with different SO4^2-concentrations were prepared next by adding（NH4）2SO4solution into OMS-2-AC samples to investigate the effect of the anion SO4^2-on the OMS-2-AC catalyst. All catalysts were then tested for the catalytic oxidation of ethanol. The OMS-2-SO4 catalyst synthesized demonstrated much better activity than OMS-2-AC. The SO4^2-doping greatly influenced the activity of the OMS-2-AC catalyst, with a dramatic promotion of activity for suitable concentration of SO4^2-（SO4/catalyst = 0.5% W/W）. The samples were characterized by X-ray diffraction（XRD）, field emission scanning electron microscopy（FE-SEM）, transmission electron microscopy（TEM）, X-ray photoelectron spectroscopy（XPS）,inductively coupled plasma optical emission spectroscopy（ICP-OES）, NH3-TPD and H2-TPR techniques. The results showed that the presence of a suitable amount of SO4^2-species in the OMS-2-AC catalyst could decrease the Mn–O bond strength and also enhance the lattice oxygen and acid site concentrations, which then effectively promoted the catalytic activity of OMS-2-AC toward ethanol oxidation. Thus it was confirmed that the better catalytic performance of OMS-2-SO4 compared to OMS-2-AC is due to the presence of some residual SO4^2-species in OMS-2-SO4 samples.
基金supported by the National Natural Science Foundation of China (Nos.21805166,21403256 and 21573261)the 111 Project (No.D20015)+3 种基金the Engineering Research Center of Eco-environment in Three Gorges Reservoir Region,Ministry of Education,China Three Gorges University (No.KF2019-05)the Outstanding Young and Middle-Aged Science and Technology Innovation Teams,Ministry of Education,Hubei province,China (No.T2020004)the Youth Innovation Promotion Association CAS (No.2018456)LICP Cooperation Foundation for Young Scholars (No.HZJJ20-10)。
文摘In this study,Mn catalysts have been designed based on manganese oxide octahedral molecular sieve(OMS-2) supports to optimize the catalytic activity in the degradation of organic pollutants.Herein,two different synthetic strategies:Pre-incorporation vs.wet-impregnation have been employed to synthesize[PW]-OMS-2 and [PW]/OMS-2.For [PW]-OMS-2,energy dispersive X-ray spectroscopy(EDX) confirmed that dispersed granular phosphotungstic acid attached and located at the surface of OMS-2,meanwhile some W atoms have been doped into frameworks of OMS-2.However,for [PW]/OMS-2,the W atoms cannot enter the OMS-2 frameworks.A correlation has been established between the different synthetic strategies and catalytic activities.The [PW]-OMS-2 is the most highly effective and stable over than[PW]/OMS-2 and OMS-2 itself for the organic pollutants removal.This may be caused not only by the synergetic effect of [PW] and OMS-2,but also by doping W into frameworks of OMS-2.Therefore,this work provides a new environmentally-friendly and heterogeneous PMS activator and it may be put into practice to degrade organic pollutants.
