NO catalytic oxidation is the key performance of the diesel oxidation catalyst(DOC).We present a facile deposition method for the core-shell rare-earth manganese-zirconium composite oxide that shows the Mn mullite pha...NO catalytic oxidation is the key performance of the diesel oxidation catalyst(DOC).We present a facile deposition method for the core-shell rare-earth manganese-zirconium composite oxide that shows the Mn mullite phase uniform loading on the surface of zirconium-based composite(YMO/CYZO),which demonstrates a superior NO oxidation catalytic performance in simulated diesel combustion conditions and better thermal stability than mullite phase YMn_(2)O_(5)oxide.The NO oxidation at 250℃over YMO/CYZO-a approaches 25.2%in contrast to 13.52%over YMn_(2)O_(5)-a.Then the catalytic performance of YMO/CYZO,YMO and commercial 1 wt%Pt/Al_(2)O_(3)in a NO+O_(2)atmosphere was compared.The maximum conversion rate of YMO/CYZO to NO oxidation is 89.6%at 274℃with a GHSV of 50000 h^(-1),and the performance is superior to that of YMO(82.8%at 293℃)and 1 wt%Pt/Al_(2)O_(3)(68.6%,335℃).The NO-temperature programmed desorption(NO-TPD)and diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)results reveal that YMO/CYZO has multiple NO adsorption sites and high storage capacity.Furthermore,density functional theory(DFT)calculation indicates that YMO/CYZO has lower oxygen vacancy formation energies(E_(v)=0.93 eV)and favorable NO adsorption energies(E_(ads)=2.1 eV).Moreover,in situ X-ray photoelectron spectroscopy(XPS)characterization shows that the core-shell structure of YMO/CYZO has the potential to transmit active oxygen species to help realize Mn3+to Mn4+during the reaction process to enhance the conversion of NO*molecules,while NO oxidation reactions follow the MvK mechanism.展开更多
Normal photocatalysts cannot effectively remove low-concentration NO because of the high recombination rate of the photogenerated carriers.To overcome this problem,S-scheme composites have been developed to fabricate ...Normal photocatalysts cannot effectively remove low-concentration NO because of the high recombination rate of the photogenerated carriers.To overcome this problem,S-scheme composites have been developed to fabricate photocatalysts.Herein,a novel S-scheme Sb2WO6/g-C3N4 nanocomposite was fabricated by an ultrasound-assisted method,which exhibited excellent performance for photocatalytic ppb-level NO removal.Compared with the pure constituents of the nanocomposite,the as-prepared 15%-Sb2WO6/g-C3N4 photocatalyst could remove more than 68%continuous-flowing NO(initial concentration:400 ppb)under visible-light irradiation in 30 min.The findings of the trapping experiments confirmed that•O2^–and h+were the important active species in the NO oxidation reaction.Meanwhile,the transient photocurrent response and PL spectroscopy analyses proved that the unique S-scheme structure of the samples could enhance the charge separation efficiency.In situ DRIFTS revealed that the photocatalytic reaction pathway of NO removal over the Sb2WO6/g-C3N4 nanocomposite occurred via an oxygen-induced route.The present work proposes a new concept for fabricating efficient photocatalysts for photocatalytic ppb-level NO oxidation and provides deeper insights into the mechanism of photocatalytic NO oxidation.展开更多
MnO and CeO2 powders were mechanically mixed by a spatula and by milling to obtain loose-contact and tight-contact mixed oxides,respectively.The monoxides and their physical mixtures were characterized by X-ray diffra...MnO and CeO2 powders were mechanically mixed by a spatula and by milling to obtain loose-contact and tight-contact mixed oxides,respectively.The monoxides and their physical mixtures were characterized by X-ray diffraction（XRD）,Brunauer-Emmett-Teller（BET）,X-ray photoelectron spectroscopy（XPS）,Raman,O2 temperature-programmed desorption（O2-TPD）,H2 temperature-programmed reduction（H2-TPR） and NO temperature-programmed oxidation（NO-TPO）.The MnOx-CeO2 solid solutions did not form without any calcination process.The oxidation state of manganese tended to increase while the ionic valence of cerium decreased in the mixed oxides,accompanied with the formation of oxygen vacancies.This long-ranged electronic interaction occured more significantly in the tight-contact mixture of MnO and CeO2.The formation of more Mn4＋and oxygen vacancies promoted the catalytic oxidation of NO in an oxygen-rich atmosphere.展开更多
One of the core issues in the photocatalytic oxidation of nitric oxide is the effective co nversion of NO into the final product(nitrate).More than just improving the visible light photocatalytic performance of BiOCl,...One of the core issues in the photocatalytic oxidation of nitric oxide is the effective co nversion of NO into the final product(nitrate).More than just improving the visible light photocatalytic performance of BiOCl,we aim to inhibit the generation of toxic by-product NO_(2) during this process.In this study,we demonstrate that the oxygen vacancies(OVs)modulate its surface photogene rated carrier transfer to inflect the NO conversion pathway by a facile mixed solvent method to induce OVs on the surface of BiOCl.The photocatalytic NO removal efficiency under visible light increased from 5.6%to 36.4%.In addition,the production rate of NO_(2) is effectively controlled.The effects of OVs on the generation of reactive oxygen species,electronic transfer,optical properties,and photocatalytic NO oxidation are investigated by combining density functional theory(DFT)theoretical calculations,the in situ FTIR spectra and experimental characterization.The OVs on the surface of BiOCl speed the trapping and transfer of localized electrons to activate the O_(2),producing O_(2)·,which avoid NO_(2) formation,resulting in complete oxidation of NO(NO+O_(2)·→NO_(3)).These findings can serve as the basis for controlling and blocking the generation of highly toxic intermediates through regulating the reactive species during the NO oxidation.It also can help us to understand the role of OV on the BiOCl surface and application of photocatalytic technology for safe air purification.展开更多
Ce-A12O3 catalysts prepared by co-precipitation are investigated both in NO oxidation by 02 and in selective catalytic reduction of NO by C2H2 （C2H2-SCR）. It is found that C2H2-SCR is initiated and controlled by NO ...Ce-A12O3 catalysts prepared by co-precipitation are investigated both in NO oxidation by 02 and in selective catalytic reduction of NO by C2H2 （C2H2-SCR）. It is found that C2H2-SCR is initiated and controlled by NO oxidation to NO2 over A12O3. Ce loading on A12O3 is almost inactive for NO oxidation below 350℃, since NO2 strongly adsorbs on cerium oxide, leading to the active sites being blocked, which was characterized by temperature-programmed desorption of NO and NO2 and Fourier transform infrared spectroscopy after NO＋O2 coadsorption over the samples. However, in the case of C2H2-SCR, Ce loading on A1203 significantly improves the reaction by accelerating the NO oxidation step in the temperature range of 250-450℃, since the nitrate species produced by NO2 adsorption is an active intermediate required by C2H2-SCR.展开更多
In this work,a series of BiOBr nanoplates with oxygen vacancies(OVs)were synthesized by a solvothermal method using a water/ethylene glycol solution.The number of OVs and facets of BiOBr were tuned by changing the wat...In this work,a series of BiOBr nanoplates with oxygen vacancies(OVs)were synthesized by a solvothermal method using a water/ethylene glycol solution.The number of OVs and facets of BiOBr were tuned by changing the water/ethylene glycol ratio.Although the role of OVs in photocatalysis has been investigated,the underlying mechanisms of charge transfer and reactant activation remain unknown.To unravel the effect of OVs on the reactant activation and photocatalytic NO oxidation process,in situ diffuse reflectance infrared Fourier transform spectroscopy,so‐called DRIFTS,and theoretical calculations were performed and their results combined.The photocatalytic efficiency of the as‐prepared BiOBr was significantly increased by increasing the amount of OVs.The oxygen vacancies had several effects on the photocatalysts,including the introduction of intermediate energy levels that enhanced light absorption,promoted electron transfer,acted as active sites for catalytic reaction and the activation of oxygen molecules,and facilitated the conversion of the intermediate products to the final product,thus increasing the overall visible light photocatalysis efficiency.The present work provides new insights into the understanding of the role of OVs in photocatalysts and the mechanism of photocatalytic NO oxidation.展开更多
Hierarchical TiO2 hollow nanoboxes(TiO2‐HNBs)assembled from TiO2 nanosheets(TiO2‐NSs)show improved photoreactivity when compared with the building blocks of discrete TiO2‐NSs.However,TiO2‐HNBs can only be excited ...Hierarchical TiO2 hollow nanoboxes(TiO2‐HNBs)assembled from TiO2 nanosheets(TiO2‐NSs)show improved photoreactivity when compared with the building blocks of discrete TiO2‐NSs.However,TiO2‐HNBs can only be excited by ultraviolet light.In this paper,visible‐light‐responsive N and S co‐doped TiO2‐HNBs were prepared by calcining the mixture of cubic TiOF2 and methionine(C5H11NO2S),a N‐and S‐containing biomacromolecule.The effect of calcination temperature on the structure and performance of the TiO2‐HNBs was systematically studied.It was found that methionine can prevent TiOF2‐to‐anatase TiO2 phase transformation.Both N and S elements are doped into the lattice of TiO2‐HNBs when the mixture of TiOF2 and methionine undergoes calcination at 400°C,which is responsible for the visible‐light response.When compared with that of pure 400°C‐calcined TiO2‐HNBs(T400),the photoreactivity of 400°C‐calcined methionine‐modified TiO2‐HNBs(TM400)improves 1.53 times in photocatalytic degradation of rhodamine‐B dye under visible irradiation(?>420 nm).The enhanced visible photoreactivity of methionine‐modified TiO2‐HNBs is also confirmed by photocatalytic oxidation of NO.The successful doping of N and S elements into the lattice of TiO2‐HNBs,resulting in the improved light‐harvesting ability and efficient separation of photo‐generated electron‐hole pairs,is responsible for the enhanced visible photocatalytic activity of methionine‐modified TiO2‐HNBs.The photoreactivity of methionine modified TiO2‐HNBs remains nearly unchanged even after being recycled five times,indicating its promising use in practical applications.展开更多
The NO oxidation reaction was studied over MnOx-CeO2 catalysts prepared by co-precipitation, impregnation and mechanical mixing method, respectively. It was found that the co-precipitation was the most active and a 60...The NO oxidation reaction was studied over MnOx-CeO2 catalysts prepared by co-precipitation, impregnation and mechanical mixing method, respectively. It was found that the co-precipitation was the most active and a 60% NO conversion was achieved at 250 oC. X-ray diffraction （XRD）, Brumauer-Emmett （BET）, H2-temperature programmed reduction （H2-TPR） and oxygen storage capacity （OSC） techniques were employed to characterize the physical and chemical properties of the catalysts. XRD results showed that amorphous MnOx or Mn-O-Ce solid solution existed in co-precipitation and impregnation prepared sample, while crystalline MnOx was found in mechanical mixing catalyst. A larger surface area was observed on co-precipitation prepared catalyst compared to those prepared by impregnation and mechanical mixing. The strong interaction between MnOx and CeO2 enhanced the reducibility of the oxides and increased the amount of Mn4＋ and activated oxygen, which are favorable for NO oxidation to NO2.展开更多
Environmental contamination such as soot particles and NO_(x)has aroused extensive attraction recently.However,the main challenge lies in the oxidation of soot at mild temperature with the assistance of NO_(x).Here,a ...Environmental contamination such as soot particles and NO_(x)has aroused extensive attraction recently.However,the main challenge lies in the oxidation of soot at mild temperature with the assistance of NO_(x).Here,a series of core-shell MnCeO_x catalysts were successfully synthesized by hydrothermal method and employed for low-temperature catalytic oxidation of soot in the presence of NO_(x).X-ray diffraction(XRD),inductively coupled plasma-optical emission spectrometry(ICP-OES),energy-dispersive X-ray spectroscopy(EDS),transmission electron microscopy(TEM),N_(2)adsorptio n/deso rption,H_(2)-tempe rature programmed reduction(H_(2)-TPR),O_(2)-temperature programmed desorption(O_(2)-TPD),X-ray photoelectron spectroscopy(XPS)and Raman analyses were conducted for identifying the structure of prepared catalysts and investigating redox properties of the core-shell mixed oxide,which shows excellent performance for NO oxidation and the T_(50)about 350℃for soot oxidation.Besides,soot particle is oxided at 304℃in the presence of NO,while T_(50)augments up to 340℃in the absence of NO.In the NO_(x)assisted elimination cases of soot,NO_(2)generated from NO in emission gas is generally reckoned as a facilitator which significantly reduces ignition temperature of soot particles.Possible catalytic mechanism over core-shell MnCeO_(x)catalysts is also proposed in this paper.展开更多
Bi12O17Br2and Bi4O5Br2visible‐light driven photocatalysts,were respectively fabricated by hydrothermal and room‐temperature deposition methods with the use of BiBr3and NaOH as precursors.Both Bi12O17Br2and Bi4O5Br2w...Bi12O17Br2and Bi4O5Br2visible‐light driven photocatalysts,were respectively fabricated by hydrothermal and room‐temperature deposition methods with the use of BiBr3and NaOH as precursors.Both Bi12O17Br2and Bi4O5Br2were composed of irregular nanosheets.The Bi4O5Br2nanosheets exhibited high and stable visible‐light photocatalytic efficiency for ppb‐level NO removal.The performance of Bi4O5Br2was markedly higher than that of the Bi12O17Br2nanosheets.The hydroxyl radical(?OH)was determined to be the main reactive oxygen species for the photo‐degradation processes of both Bi12O17Br2and Bi4O5Br2.However,in situ diffuse reflectance infrared Fourier transform spectroscopy analysis revealed that Bi12O17Br2and Bi4O5Br2featured different conversion pathways for visible light driven photocatalytic NO oxidation.The excellent photocatalytic activity of Bi4O5Br2resulted from a high surface area and large pore volumes,which facilitated the transport of reactants and intermediate products,and provided more active sites for photochemical reaction.Furthermore,the Bi4O5Br2nanosheets produced more?OH and presented stronger valence band holeoxidation.In addition,the oxygen atoms of NO could insert into oxygen‐vacancies of Bi4O5Br2,whichprovided more active sites for the reaction.This work gives insight into the photocatalytic pollutant‐degradation mechanism of bismuth oxyhalide.展开更多
MnO_x-CeO_2 catalysts were synthesized to investigate the active sites for NO oxidation by varying the calcination temperature. XRD and TEM results showed that cubic CeO_2 and amorphous MnO_x existed in MnO_x-CeO_2 ca...MnO_x-CeO_2 catalysts were synthesized to investigate the active sites for NO oxidation by varying the calcination temperature. XRD and TEM results showed that cubic CeO_2 and amorphous MnO_x existed in MnO_x-CeO_2 catalysts. High temperature calcination caused the sintering of amorphous MnO_x and transforming to bulk crystalline Mn_2O_3, H_2-TPR and XPS results suggested the valence of Mn in MnO_x-CeO_2 was higher than pure MnO_x, and decreased with the increasing calcination temperature, The turnover frequency（TOF） was calculated based on the initial reducibility according to H_2-TPR quantitation and kinetic study. The TOF results indicated that the initial reducibility of amorphous MnO_x with high valence manganese ions was equivalent to the active sites for NO oxidation. It can be inferred that the amorphous MnO_x plays a key role in low-temperature NO oxidation.展开更多
Oxygen-vacancies(OVs)play significant roles in semiconductor-based photocatalysis,such as elevating light absorption property,photogenerated carries separation efficiency,molecular activation,and photocatalytic activi...Oxygen-vacancies(OVs)play significant roles in semiconductor-based photocatalysis,such as elevating light absorption property,photogenerated carries separation efficiency,molecular activation,and photocatalytic activity.However,heat-treatment of semiconductors in dangerous H_(2)atmosphere is usually indispensable for OVs formation.In this work,C-doped Bi_(12)O_(17)C_(12)nanosheets were facially heat-treated in H_(2)O vapor(~2.3 vol%)mixed with Ar at 300℃to in-situ introduce OVs by the proposed reactions of C(s)+H_(2)O(g)→CO(g)+H_(2)(g)and H_(2)(g)+O_(Lattice)→H_(2)O(g)+OV.The formation of OVs,which was confirmed by electron paramagnetic resonance(EPR),can narrow the band gap,and enhance the photogenerated e~-/h~+separation efficiency on Bi_(12)O_(17)C_(12).Moreover,OVs-rich Bi_(12)O_(17)C_(12)nanosheets can facilitate molecular O_(2)activation and produce more reactive oxygen species(ROS),especially~1 O_(2),which greatly improve the NO to NO_(3)~-conversion efficiency with NO removal rate of~63%and NO_(3)~-production selectivity of~92.6%.The present work will bring new insights into the construction and roles of OVs in semiconductor-based photocatalysis.展开更多
Catalytic oxidation of NO at room temperature was carried out over nitrogen(N)-doped sludge char(SC)prepared from pyrolysis ofmunicipal sewage sludge,and urea was adopted as nitrogen source.The effects of different N-...Catalytic oxidation of NO at room temperature was carried out over nitrogen(N)-doped sludge char(SC)prepared from pyrolysis ofmunicipal sewage sludge,and urea was adopted as nitrogen source.The effects of different N-doping methods(one-step and two-step method),dried sludge(DS)/urea mass ratios(5:1,4:1,3:1,2:1,and 1:1),SC preparation procedures(pyrolysis only,pyrolysis with acid washing,and pyrolysis with KOH activation and acid washing),and different pyrolysis temperatures(500,600,700,and 800°C)on the catalytic oxidation of NO were compared to optimize the procedure for SC preparation.The results indicated that N-doping could obviously promote the catalytic performance of SC.The one-step method with simultaneous sludge pyrolysis(at 700°C),KOH activation,and N-doping(DS/urea of 3:1)was the optimal procedure for preparing the N-doped SC with the NO conversion rate of 54.7%,whereas the optimal NO conversion rate of SC without N-doping was only 47.3%.Urea worked both as carbon and nitrogen source,which could increase about 2.9%-16.5%of carbon and 24.8%-42.7%of nitrogen content in SC pyrolyzed at 700°C.N-doping significantly promoted microporosity of SC.The optimal N-doped SC showed specific surface areas of 571.38 m^(2)/g,much higher than 374.34 m^(2)/g of the optimal SC without N-doping.In addition,N-doping also increased amorphousness and surface basicity of SC through the formation of N-containing groups.Finally,three reaction paths,i.e.microporous reactor,active sites,and basic site control path,were proposed to explain the mechanism of N-doping on promoting the catalytic performance of NO.展开更多
NO oxidation with H_(2)O_(2)as the oxidant is a promising green denitration technology.However,the current metal oxide catalysts still have many disadvantages for this reaction,such as insufficient catalytic activity ...NO oxidation with H_(2)O_(2)as the oxidant is a promising green denitration technology.However,the current metal oxide catalysts still have many disadvantages for this reaction,such as insufficient catalytic activity for H_(2)O_(2)activation,poor selectivity,and low stability.In this study,we employ atomically dispersed Co anchored on SBA-15 with Co-O_(4)structure for NO oxidation,which achieves a 90%removal efficiency of NO under low molar ratio of H_(2)O_(2)to NO(1.56),ultra-low temperature(80℃),and ultra-high space velocity(720,000 h^(-1)),representing the top-level performance among previously reported catalysts.More interestingly,our work reveals that by taking advantage of the uniform Co-O_(4)structure,H_(2)O_(2)is mainly directionally converted into·O_(2)^(-)at the Co-O_(4)site,and·O_(2)^(-)plays a key role for achieving the deep-oxidation of NO to produce NO_(3)^(-),which is contrast to the previously reports that^(1)O_(2)is the main free radical for NO oxidation.This study highlights the great potentials of single-atom catalysts for improving the H_(2)O_(2)utilization performance for NO oxidation.展开更多
Graphitic carbon nitride(g-C_(3)N_(4),CN)is recognized as the most extensively studied organic polymeric photo-catalyst for pollution control and energy conversion due to its facile synthesis and suitable electronic b...Graphitic carbon nitride(g-C_(3)N_(4),CN)is recognized as the most extensively studied organic polymeric photo-catalyst for pollution control and energy conversion due to its facile synthesis and suitable electronic band structure.The aim of the present work is to explore the effect of precursors,such as urea(U,(NH_(2))_(2)CO),dicyandiamide(D,C_(2)H_(4)N_(4))and melamine(M,C_(3)H_(6)N_(6)),on the structure and photocatalytic activity of the ob-tained CN samples,denoted as UCN,DCN and MCN,respectively.The sheet-like UCN sample shows significantly enhanced photoreactivity in both NO oxidation and CO_(2)reduction compared to the bulk DCN and MCN materials.In addition,UCN demonstrates the ability to suppress the formation of toxic NO_(2)intermediate during the photocatalytic oxidation of NO.The improved photocatalytic activity of UCN can be attributed to a dual effect:first,its increased specific surface area provides more active sites for the photocatalytic reaction;second,it ex-hibits a stronger affinity for substrates like NO and CO_(2),which facilitates charge migration at the interface.展开更多
NO adsorption behavior on H-ZSM-5 was investigated using a fixed-bed reactor and the adsorption mechanism was studied by temperature programmed desorption(TPD),in-situ Fourier transform infrared spectroscopy(FTIR)and ...NO adsorption behavior on H-ZSM-5 was investigated using a fixed-bed reactor and the adsorption mechanism was studied by temperature programmed desorption(TPD),in-situ Fourier transform infrared spectroscopy(FTIR)and thermogravimetric(TG)analysis.Results showed that heat releasing area(HRA)occurred at the beginning of NO and O_(2) co-adsorption on H-ZSM-5,and after the disappearance of HRA,zeolites with different silicate-aluminum ratios showed different adsorption efficiency.The impurities in flue gas had a negative effect on the adsorption of NO and the influence could be ranked in descending order as follows:SO_(2)>H_(2)O>CO_(2).TPD and FTIR analyses suggested that nitrates were formed during exposure of zeolites to NO without O_(2) and different kinds of nitrogen oxides were observed after O_(2) was added into the system.An adsorption mechanism involving rapid oxidation of NO was proposed to explain the NO adsorption behavior under aerobic atmosphere.This work may be crucial for understanding the catalysis mechanism of metal ion-based ZSM-5 zeolites and the design of proper catalyst supporter.展开更多
Due to the increasingly strict emission standards of NOx on various industries,many traditional flue gas treatment methods have been gradually improved.Except for selective catalytic reduction(SCR)and selective non-ca...Due to the increasingly strict emission standards of NOx on various industries,many traditional flue gas treatment methods have been gradually improved.Except for selective catalytic reduction(SCR)and selective non-catalytic reduction(SNCR)methods to remove NOx from flue gas,theoxidation method is paying more attention to NOx removal now because of the potential to simultaneously remove multiple pollutants from flue gas.This paper summarizes the efficiency,reaction conditions,effect factors,and reaction mechanism of NO oxidation from the aspects of liquid-phase oxidation,gas-phase oxidation,plasma technology,and catalytic oxidation.The effects of free radicals and active components of catalysts on NO oxidation and the combination of various oxidation methods are discussed in detail.The advantages and disadvantages of different oxidation methods are summarized,and the suggestions for future research on NO oxidation are put forward at the end.The review on the NO removal by oxidation methods can provide new ideas for future studies on the NO removal from flue gas.展开更多
La1-x Cax MnO3 （x=0-0.3） perovskite-type oxides were synthesized by citrate sol-gel method. The physical and chemical properties were characterized by X-ray diffraction （XRD）, Brumauer-Emmett-Teller method （BET）...La1-x Cax MnO3 （x=0-0.3） perovskite-type oxides were synthesized by citrate sol-gel method. The physical and chemical properties were characterized by X-ray diffraction （XRD）, Brumauer-Emmett-Teller method （BET）, X-ray photoelectron spectroscopy （XPS）, NO＋O2 -TPD （temperature-programmed desorption）, activated oxygen evaluation and H2 -TPR （temperature-programmed reduction） technologies. The results showed that NO catalytic oxidation activity was significantly improved by Ca substitution, especially for lower temperature activity. The La0.9 Ca0.1 MnO 3 sample showed the maximum conversion of 82% at 300 oC. The monodentate nitrates played a crucial role for the formation of NO2 . The reducibility of Mn 4＋ ions and reactivity of activated oxygen were favorable for the catalytic performances of NO oxidation.展开更多
Photocatalysis is considered a promising technique for removal of pollutants from indoor air.However,the low selectivity and limited recyclability of photocatalysts in powder form currently limit their practical appli...Photocatalysis is considered a promising technique for removal of pollutants from indoor air.However,the low selectivity and limited recyclability of photocatalysts in powder form currently limit their practical application.In this work,we reported the successful preparation of a monolithic tungsten oxide(WO3)/graphene oxide(GO)aerogel photocatalyst through a cost‐effective freeze‐drying method.GO not only acts as a macroscopic support,but also increases the catalyst surface area from 46 to 57 m2/g,enhances the light absorption in the visible‐light region,and raises the separation efficiency of photogenerated electron‐hole pairs.The Obtained WO3/GO aerogel exhibited an outstanding visible‐light photocatalytic degradation rate of nitric oxide of 51%,which was 3.3 times that of pristine WO3 powder.In addition,the aerogel displayed excellent selectivity,with a generation fraction of toxic nitrogen dioxide of as low as 0.5%.This work presents a facile synthesis route to fabricate a monolithic WO3/GO aerogel photocatalyst with great promise for air purification.展开更多
A series of La1-xCexMnO3+δ(x=D,0.05,0.1,0.2,and 0.3)perovskites and Mn-Ce mixed oxides were prepared.Their physico-chemical properties were systematically characterized and the NO oxidation activities of the catalyst...A series of La1-xCexMnO3+δ(x=D,0.05,0.1,0.2,and 0.3)perovskites and Mn-Ce mixed oxides were prepared.Their physico-chemical properties were systematically characterized and the NO oxidation activities of the catalysts were investigated.The La0.9Ce0.1MnO3+δhas the best activity among all of the catalysts,with a maximum NO conversion of 85%at 300℃.The characterization results indicate that the doping of Ce improves the properties of the perovsidtes in terms of the specific surface area,the average valence state of Mn ions,the number of reactive oxygen species and the NOx desorption behaviors.The Mn-Ce mixed oxide calcined at 500℃shows a similar NO oxidation activity with La0.9Ce0.1MnO3+δ.However,the activity of the mixed oxide obtained at 750℃decreases a lot,which results from the loss of active sites and active oxygen species.展开更多
基金supported by National Natural Science Foundation of China(52204376)Open Project of Yunnan Precious Metals Laboratory Co.(YPML-2023050266)Youth Foundation of Hebei Province(E2022103007)。
文摘NO catalytic oxidation is the key performance of the diesel oxidation catalyst(DOC).We present a facile deposition method for the core-shell rare-earth manganese-zirconium composite oxide that shows the Mn mullite phase uniform loading on the surface of zirconium-based composite(YMO/CYZO),which demonstrates a superior NO oxidation catalytic performance in simulated diesel combustion conditions and better thermal stability than mullite phase YMn_(2)O_(5)oxide.The NO oxidation at 250℃over YMO/CYZO-a approaches 25.2%in contrast to 13.52%over YMn_(2)O_(5)-a.Then the catalytic performance of YMO/CYZO,YMO and commercial 1 wt%Pt/Al_(2)O_(3)in a NO+O_(2)atmosphere was compared.The maximum conversion rate of YMO/CYZO to NO oxidation is 89.6%at 274℃with a GHSV of 50000 h^(-1),and the performance is superior to that of YMO(82.8%at 293℃)and 1 wt%Pt/Al_(2)O_(3)(68.6%,335℃).The NO-temperature programmed desorption(NO-TPD)and diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)results reveal that YMO/CYZO has multiple NO adsorption sites and high storage capacity.Furthermore,density functional theory(DFT)calculation indicates that YMO/CYZO has lower oxygen vacancy formation energies(E_(v)=0.93 eV)and favorable NO adsorption energies(E_(ads)=2.1 eV).Moreover,in situ X-ray photoelectron spectroscopy(XPS)characterization shows that the core-shell structure of YMO/CYZO has the potential to transmit active oxygen species to help realize Mn3+to Mn4+during the reaction process to enhance the conversion of NO*molecules,while NO oxidation reactions follow the MvK mechanism.
文摘Normal photocatalysts cannot effectively remove low-concentration NO because of the high recombination rate of the photogenerated carriers.To overcome this problem,S-scheme composites have been developed to fabricate photocatalysts.Herein,a novel S-scheme Sb2WO6/g-C3N4 nanocomposite was fabricated by an ultrasound-assisted method,which exhibited excellent performance for photocatalytic ppb-level NO removal.Compared with the pure constituents of the nanocomposite,the as-prepared 15%-Sb2WO6/g-C3N4 photocatalyst could remove more than 68%continuous-flowing NO(initial concentration:400 ppb)under visible-light irradiation in 30 min.The findings of the trapping experiments confirmed that•O2^–and h+were the important active species in the NO oxidation reaction.Meanwhile,the transient photocurrent response and PL spectroscopy analyses proved that the unique S-scheme structure of the samples could enhance the charge separation efficiency.In situ DRIFTS revealed that the photocatalytic reaction pathway of NO removal over the Sb2WO6/g-C3N4 nanocomposite occurred via an oxygen-induced route.The present work proposes a new concept for fabricating efficient photocatalysts for photocatalytic ppb-level NO oxidation and provides deeper insights into the mechanism of photocatalytic NO oxidation.
基金supported by National Natural Science Foundation of China(51072096)National Basic Research Program of China(2010CB732304)National High-Tech Research and Development Program of China(2013AA065302)
文摘MnO and CeO2 powders were mechanically mixed by a spatula and by milling to obtain loose-contact and tight-contact mixed oxides,respectively.The monoxides and their physical mixtures were characterized by X-ray diffraction（XRD）,Brunauer-Emmett-Teller（BET）,X-ray photoelectron spectroscopy（XPS）,Raman,O2 temperature-programmed desorption（O2-TPD）,H2 temperature-programmed reduction（H2-TPR） and NO temperature-programmed oxidation（NO-TPO）.The MnOx-CeO2 solid solutions did not form without any calcination process.The oxidation state of manganese tended to increase while the ionic valence of cerium decreased in the mixed oxides,accompanied with the formation of oxygen vacancies.This long-ranged electronic interaction occured more significantly in the tight-contact mixture of MnO and CeO2.The formation of more Mn4＋and oxygen vacancies promoted the catalytic oxidation of NO in an oxygen-rich atmosphere.
基金the National Natural Science Foundation of China(Nos.21822601,21777011 and 21501016)the Plan for"National Youth Talents"of the Organization Department of the Central Committee。
文摘One of the core issues in the photocatalytic oxidation of nitric oxide is the effective co nversion of NO into the final product(nitrate).More than just improving the visible light photocatalytic performance of BiOCl,we aim to inhibit the generation of toxic by-product NO_(2) during this process.In this study,we demonstrate that the oxygen vacancies(OVs)modulate its surface photogene rated carrier transfer to inflect the NO conversion pathway by a facile mixed solvent method to induce OVs on the surface of BiOCl.The photocatalytic NO removal efficiency under visible light increased from 5.6%to 36.4%.In addition,the production rate of NO_(2) is effectively controlled.The effects of OVs on the generation of reactive oxygen species,electronic transfer,optical properties,and photocatalytic NO oxidation are investigated by combining density functional theory(DFT)theoretical calculations,the in situ FTIR spectra and experimental characterization.The OVs on the surface of BiOCl speed the trapping and transfer of localized electrons to activate the O_(2),producing O_(2)·,which avoid NO_(2) formation,resulting in complete oxidation of NO(NO+O_(2)·→NO_(3)).These findings can serve as the basis for controlling and blocking the generation of highly toxic intermediates through regulating the reactive species during the NO oxidation.It also can help us to understand the role of OV on the BiOCl surface and application of photocatalytic technology for safe air purification.
基金supported by the National Natural Science Foundation of China (Grant No. 20833011 and 20877015)the State Hi-tech Research and Development Project of the Ministry of Science and Technology of China (Grant No. 2008AA06Z319)
文摘Ce-A12O3 catalysts prepared by co-precipitation are investigated both in NO oxidation by 02 and in selective catalytic reduction of NO by C2H2 （C2H2-SCR）. It is found that C2H2-SCR is initiated and controlled by NO oxidation to NO2 over A12O3. Ce loading on A12O3 is almost inactive for NO oxidation below 350℃, since NO2 strongly adsorbs on cerium oxide, leading to the active sites being blocked, which was characterized by temperature-programmed desorption of NO and NO2 and Fourier transform infrared spectroscopy after NO＋O2 coadsorption over the samples. However, in the case of C2H2-SCR, Ce loading on A1203 significantly improves the reaction by accelerating the NO oxidation step in the temperature range of 250-450℃, since the nitrate species produced by NO2 adsorption is an active intermediate required by C2H2-SCR.
文摘In this work,a series of BiOBr nanoplates with oxygen vacancies(OVs)were synthesized by a solvothermal method using a water/ethylene glycol solution.The number of OVs and facets of BiOBr were tuned by changing the water/ethylene glycol ratio.Although the role of OVs in photocatalysis has been investigated,the underlying mechanisms of charge transfer and reactant activation remain unknown.To unravel the effect of OVs on the reactant activation and photocatalytic NO oxidation process,in situ diffuse reflectance infrared Fourier transform spectroscopy,so‐called DRIFTS,and theoretical calculations were performed and their results combined.The photocatalytic efficiency of the as‐prepared BiOBr was significantly increased by increasing the amount of OVs.The oxygen vacancies had several effects on the photocatalysts,including the introduction of intermediate energy levels that enhanced light absorption,promoted electron transfer,acted as active sites for catalytic reaction and the activation of oxygen molecules,and facilitated the conversion of the intermediate products to the final product,thus increasing the overall visible light photocatalysis efficiency.The present work provides new insights into the understanding of the role of OVs in photocatalysts and the mechanism of photocatalytic NO oxidation.
基金supported by the National Natural Science Foundation of China(31402137,51672312,21373275)Hubei Province Science Fund for Distinguished Yong Scholars(2013CFA034)+2 种基金the Program for Excellent Talents in Hubei Province(RCJH15001)the Science and Technology Program of Wuhan(2016010101010018)the Fundamental Research Funds for the Central University,South-Central University for Nationalities(CZP17077,CZP18016)~~
文摘Hierarchical TiO2 hollow nanoboxes(TiO2‐HNBs)assembled from TiO2 nanosheets(TiO2‐NSs)show improved photoreactivity when compared with the building blocks of discrete TiO2‐NSs.However,TiO2‐HNBs can only be excited by ultraviolet light.In this paper,visible‐light‐responsive N and S co‐doped TiO2‐HNBs were prepared by calcining the mixture of cubic TiOF2 and methionine(C5H11NO2S),a N‐and S‐containing biomacromolecule.The effect of calcination temperature on the structure and performance of the TiO2‐HNBs was systematically studied.It was found that methionine can prevent TiOF2‐to‐anatase TiO2 phase transformation.Both N and S elements are doped into the lattice of TiO2‐HNBs when the mixture of TiOF2 and methionine undergoes calcination at 400°C,which is responsible for the visible‐light response.When compared with that of pure 400°C‐calcined TiO2‐HNBs(T400),the photoreactivity of 400°C‐calcined methionine‐modified TiO2‐HNBs(TM400)improves 1.53 times in photocatalytic degradation of rhodamine‐B dye under visible irradiation(?>420 nm).The enhanced visible photoreactivity of methionine‐modified TiO2‐HNBs is also confirmed by photocatalytic oxidation of NO.The successful doping of N and S elements into the lattice of TiO2‐HNBs,resulting in the improved light‐harvesting ability and efficient separation of photo‐generated electron‐hole pairs,is responsible for the enhanced visible photocatalytic activity of methionine‐modified TiO2‐HNBs.The photoreactivity of methionine modified TiO2‐HNBs remains nearly unchanged even after being recycled five times,indicating its promising use in practical applications.
基金supported by National High Technology Research and Development Program of China(863Program,2011AA03A405)grant support from GM Global Research & Development
文摘The NO oxidation reaction was studied over MnOx-CeO2 catalysts prepared by co-precipitation, impregnation and mechanical mixing method, respectively. It was found that the co-precipitation was the most active and a 60% NO conversion was achieved at 250 oC. X-ray diffraction （XRD）, Brumauer-Emmett （BET）, H2-temperature programmed reduction （H2-TPR） and oxygen storage capacity （OSC） techniques were employed to characterize the physical and chemical properties of the catalysts. XRD results showed that amorphous MnOx or Mn-O-Ce solid solution existed in co-precipitation and impregnation prepared sample, while crystalline MnOx was found in mechanical mixing catalyst. A larger surface area was observed on co-precipitation prepared catalyst compared to those prepared by impregnation and mechanical mixing. The strong interaction between MnOx and CeO2 enhanced the reducibility of the oxides and increased the amount of Mn4＋ and activated oxygen, which are favorable for NO oxidation to NO2.
基金Project supported by the National Natural Science Foundation of China(42077201)Science and Technology Innovation Project of Higher Education Institutions in Shanxi Province(2019L0615)Youth Science Foundation of Shanxi Province(201901D211291)。
文摘Environmental contamination such as soot particles and NO_(x)has aroused extensive attraction recently.However,the main challenge lies in the oxidation of soot at mild temperature with the assistance of NO_(x).Here,a series of core-shell MnCeO_x catalysts were successfully synthesized by hydrothermal method and employed for low-temperature catalytic oxidation of soot in the presence of NO_(x).X-ray diffraction(XRD),inductively coupled plasma-optical emission spectrometry(ICP-OES),energy-dispersive X-ray spectroscopy(EDS),transmission electron microscopy(TEM),N_(2)adsorptio n/deso rption,H_(2)-tempe rature programmed reduction(H_(2)-TPR),O_(2)-temperature programmed desorption(O_(2)-TPD),X-ray photoelectron spectroscopy(XPS)and Raman analyses were conducted for identifying the structure of prepared catalysts and investigating redox properties of the core-shell mixed oxide,which shows excellent performance for NO oxidation and the T_(50)about 350℃for soot oxidation.Besides,soot particle is oxided at 304℃in the presence of NO,while T_(50)augments up to 340℃in the absence of NO.In the NO_(x)assisted elimination cases of soot,NO_(2)generated from NO in emission gas is generally reckoned as a facilitator which significantly reduces ignition temperature of soot particles.Possible catalytic mechanism over core-shell MnCeO_(x)catalysts is also proposed in this paper.
基金supported by the National Natural Science Foundation of China(51708078,21576034)Chongqing Postdoctoral Science Foundation funded project(Xm2016027)the Innovative Research Team of Chongqing(CXTDG201602014,CXTDX201601016)~~
文摘Bi12O17Br2and Bi4O5Br2visible‐light driven photocatalysts,were respectively fabricated by hydrothermal and room‐temperature deposition methods with the use of BiBr3and NaOH as precursors.Both Bi12O17Br2and Bi4O5Br2were composed of irregular nanosheets.The Bi4O5Br2nanosheets exhibited high and stable visible‐light photocatalytic efficiency for ppb‐level NO removal.The performance of Bi4O5Br2was markedly higher than that of the Bi12O17Br2nanosheets.The hydroxyl radical(?OH)was determined to be the main reactive oxygen species for the photo‐degradation processes of both Bi12O17Br2and Bi4O5Br2.However,in situ diffuse reflectance infrared Fourier transform spectroscopy analysis revealed that Bi12O17Br2and Bi4O5Br2featured different conversion pathways for visible light driven photocatalytic NO oxidation.The excellent photocatalytic activity of Bi4O5Br2resulted from a high surface area and large pore volumes,which facilitated the transport of reactants and intermediate products,and provided more active sites for photochemical reaction.Furthermore,the Bi4O5Br2nanosheets produced more?OH and presented stronger valence band holeoxidation.In addition,the oxygen atoms of NO could insert into oxygen‐vacancies of Bi4O5Br2,whichprovided more active sites for the reaction.This work gives insight into the photocatalytic pollutant‐degradation mechanism of bismuth oxyhalide.
基金Project supported by the National key research and development program(2016YFC0204901)the National Natural Science Foundation of China(21576207)the introduction of talent and technology cooperation plan of Tianjin(14RCGFGX00849)
文摘MnO_x-CeO_2 catalysts were synthesized to investigate the active sites for NO oxidation by varying the calcination temperature. XRD and TEM results showed that cubic CeO_2 and amorphous MnO_x existed in MnO_x-CeO_2 catalysts. High temperature calcination caused the sintering of amorphous MnO_x and transforming to bulk crystalline Mn_2O_3, H_2-TPR and XPS results suggested the valence of Mn in MnO_x-CeO_2 was higher than pure MnO_x, and decreased with the increasing calcination temperature, The turnover frequency（TOF） was calculated based on the initial reducibility according to H_2-TPR quantitation and kinetic study. The TOF results indicated that the initial reducibility of amorphous MnO_x with high valence manganese ions was equivalent to the active sites for NO oxidation. It can be inferred that the amorphous MnO_x plays a key role in low-temperature NO oxidation.
基金financially supported by the National Natural Science Foundation of China(Nos.21703075,51872107,52073110,22002047)Natural Science Foundation of Hubei Province(Nos.2020CFB694,2020CFB394)Fundamental Research Funds for the Central Universities(Nos.2662020LXPY005,2662019QD018)。
文摘Oxygen-vacancies(OVs)play significant roles in semiconductor-based photocatalysis,such as elevating light absorption property,photogenerated carries separation efficiency,molecular activation,and photocatalytic activity.However,heat-treatment of semiconductors in dangerous H_(2)atmosphere is usually indispensable for OVs formation.In this work,C-doped Bi_(12)O_(17)C_(12)nanosheets were facially heat-treated in H_(2)O vapor(~2.3 vol%)mixed with Ar at 300℃to in-situ introduce OVs by the proposed reactions of C(s)+H_(2)O(g)→CO(g)+H_(2)(g)and H_(2)(g)+O_(Lattice)→H_(2)O(g)+OV.The formation of OVs,which was confirmed by electron paramagnetic resonance(EPR),can narrow the band gap,and enhance the photogenerated e~-/h~+separation efficiency on Bi_(12)O_(17)C_(12).Moreover,OVs-rich Bi_(12)O_(17)C_(12)nanosheets can facilitate molecular O_(2)activation and produce more reactive oxygen species(ROS),especially~1 O_(2),which greatly improve the NO to NO_(3)~-conversion efficiency with NO removal rate of~63%and NO_(3)~-production selectivity of~92.6%.The present work will bring new insights into the construction and roles of OVs in semiconductor-based photocatalysis.
基金supported by Shanghai Pujiang Program(No.22PJD001)the Fundamental Research Funds for the Central Universities(No.2232021G-11).
文摘Catalytic oxidation of NO at room temperature was carried out over nitrogen(N)-doped sludge char(SC)prepared from pyrolysis ofmunicipal sewage sludge,and urea was adopted as nitrogen source.The effects of different N-doping methods(one-step and two-step method),dried sludge(DS)/urea mass ratios(5:1,4:1,3:1,2:1,and 1:1),SC preparation procedures(pyrolysis only,pyrolysis with acid washing,and pyrolysis with KOH activation and acid washing),and different pyrolysis temperatures(500,600,700,and 800°C)on the catalytic oxidation of NO were compared to optimize the procedure for SC preparation.The results indicated that N-doping could obviously promote the catalytic performance of SC.The one-step method with simultaneous sludge pyrolysis(at 700°C),KOH activation,and N-doping(DS/urea of 3:1)was the optimal procedure for preparing the N-doped SC with the NO conversion rate of 54.7%,whereas the optimal NO conversion rate of SC without N-doping was only 47.3%.Urea worked both as carbon and nitrogen source,which could increase about 2.9%-16.5%of carbon and 24.8%-42.7%of nitrogen content in SC pyrolyzed at 700°C.N-doping significantly promoted microporosity of SC.The optimal N-doped SC showed specific surface areas of 571.38 m^(2)/g,much higher than 374.34 m^(2)/g of the optimal SC without N-doping.In addition,N-doping also increased amorphousness and surface basicity of SC through the formation of N-containing groups.Finally,three reaction paths,i.e.microporous reactor,active sites,and basic site control path,were proposed to explain the mechanism of N-doping on promoting the catalytic performance of NO.
基金funded by the National Natural Science Foundation of China(Nos.52176104 and 52006073)the Natural Science Foundation of Hebei Province(No.B2023502023)Fundamental Research Fund for the Central Universities(Nos.2023MS125 and 2024MS154).
文摘NO oxidation with H_(2)O_(2)as the oxidant is a promising green denitration technology.However,the current metal oxide catalysts still have many disadvantages for this reaction,such as insufficient catalytic activity for H_(2)O_(2)activation,poor selectivity,and low stability.In this study,we employ atomically dispersed Co anchored on SBA-15 with Co-O_(4)structure for NO oxidation,which achieves a 90%removal efficiency of NO under low molar ratio of H_(2)O_(2)to NO(1.56),ultra-low temperature(80℃),and ultra-high space velocity(720,000 h^(-1)),representing the top-level performance among previously reported catalysts.More interestingly,our work reveals that by taking advantage of the uniform Co-O_(4)structure,H_(2)O_(2)is mainly directionally converted into·O_(2)^(-)at the Co-O_(4)site,and·O_(2)^(-)plays a key role for achieving the deep-oxidation of NO to produce NO_(3)^(-),which is contrast to the previously reports that^(1)O_(2)is the main free radical for NO oxidation.This study highlights the great potentials of single-atom catalysts for improving the H_(2)O_(2)utilization performance for NO oxidation.
基金supported by the National Natural Science Foundation of China(51672312)Hubei Provincial Natural Science Foundation and Huangshi of China(2022CFD001)+2 种基金The Fundamental Research Funds for the Central Universities of South-Central Minzu University(CZP22001)the Fund for Academic Innovation Teams of South-Central Minzu University(XTZ24019)Portuguese Foundation for Science and Technology/Ministry of Science and Technology and Higher Teaching(FCT/MCTES).
文摘Graphitic carbon nitride(g-C_(3)N_(4),CN)is recognized as the most extensively studied organic polymeric photo-catalyst for pollution control and energy conversion due to its facile synthesis and suitable electronic band structure.The aim of the present work is to explore the effect of precursors,such as urea(U,(NH_(2))_(2)CO),dicyandiamide(D,C_(2)H_(4)N_(4))and melamine(M,C_(3)H_(6)N_(6)),on the structure and photocatalytic activity of the ob-tained CN samples,denoted as UCN,DCN and MCN,respectively.The sheet-like UCN sample shows significantly enhanced photoreactivity in both NO oxidation and CO_(2)reduction compared to the bulk DCN and MCN materials.In addition,UCN demonstrates the ability to suppress the formation of toxic NO_(2)intermediate during the photocatalytic oxidation of NO.The improved photocatalytic activity of UCN can be attributed to a dual effect:first,its increased specific surface area provides more active sites for the photocatalytic reaction;second,it ex-hibits a stronger affinity for substrates like NO and CO_(2),which facilitates charge migration at the interface.
基金the Ministry of Industry and Information Technology of the People’s Republic of China(No.CDGC01-KT16)。
文摘NO adsorption behavior on H-ZSM-5 was investigated using a fixed-bed reactor and the adsorption mechanism was studied by temperature programmed desorption(TPD),in-situ Fourier transform infrared spectroscopy(FTIR)and thermogravimetric(TG)analysis.Results showed that heat releasing area(HRA)occurred at the beginning of NO and O_(2) co-adsorption on H-ZSM-5,and after the disappearance of HRA,zeolites with different silicate-aluminum ratios showed different adsorption efficiency.The impurities in flue gas had a negative effect on the adsorption of NO and the influence could be ranked in descending order as follows:SO_(2)>H_(2)O>CO_(2).TPD and FTIR analyses suggested that nitrates were formed during exposure of zeolites to NO without O_(2) and different kinds of nitrogen oxides were observed after O_(2) was added into the system.An adsorption mechanism involving rapid oxidation of NO was proposed to explain the NO adsorption behavior under aerobic atmosphere.This work may be crucial for understanding the catalysis mechanism of metal ion-based ZSM-5 zeolites and the design of proper catalyst supporter.
基金supported by National Key Research and Development Program of China(No.2018YFB0605101)the Key Project Natural Science Foundation of Tianjin(No.18JCZDJC39800)+4 种基金the Key R&D projects in Hebei Province(No.20373701D)the National Natural Science Foundation of China(No.51808181)the Science and Technology Key Project of Tianjin(Nos.18ZXSZSF00040,18KPXMSF00080,18PTZWHZ00010)Department of Education of Hebei Province(No.BJ2017032)Joint Doctoral Training Foundation of HEBUT(No.2017HW0002)。
文摘Due to the increasingly strict emission standards of NOx on various industries,many traditional flue gas treatment methods have been gradually improved.Except for selective catalytic reduction(SCR)and selective non-catalytic reduction(SNCR)methods to remove NOx from flue gas,theoxidation method is paying more attention to NOx removal now because of the potential to simultaneously remove multiple pollutants from flue gas.This paper summarizes the efficiency,reaction conditions,effect factors,and reaction mechanism of NO oxidation from the aspects of liquid-phase oxidation,gas-phase oxidation,plasma technology,and catalytic oxidation.The effects of free radicals and active components of catalysts on NO oxidation and the combination of various oxidation methods are discussed in detail.The advantages and disadvantages of different oxidation methods are summarized,and the suggestions for future research on NO oxidation are put forward at the end.The review on the NO removal by oxidation methods can provide new ideas for future studies on the NO removal from flue gas.
基金Project supported by National High Technology Research and Development Program of China(863Program,2011AA03A405)
文摘La1-x Cax MnO3 （x=0-0.3） perovskite-type oxides were synthesized by citrate sol-gel method. The physical and chemical properties were characterized by X-ray diffraction （XRD）, Brumauer-Emmett-Teller method （BET）, X-ray photoelectron spectroscopy （XPS）, NO＋O2 -TPD （temperature-programmed desorption）, activated oxygen evaluation and H2 -TPR （temperature-programmed reduction） technologies. The results showed that NO catalytic oxidation activity was significantly improved by Ca substitution, especially for lower temperature activity. The La0.9 Ca0.1 MnO 3 sample showed the maximum conversion of 82% at 300 oC. The monodentate nitrates played a crucial role for the formation of NO2 . The reducibility of Mn 4＋ ions and reactivity of activated oxygen were favorable for the catalytic performances of NO oxidation.
文摘Photocatalysis is considered a promising technique for removal of pollutants from indoor air.However,the low selectivity and limited recyclability of photocatalysts in powder form currently limit their practical application.In this work,we reported the successful preparation of a monolithic tungsten oxide(WO3)/graphene oxide(GO)aerogel photocatalyst through a cost‐effective freeze‐drying method.GO not only acts as a macroscopic support,but also increases the catalyst surface area from 46 to 57 m2/g,enhances the light absorption in the visible‐light region,and raises the separation efficiency of photogenerated electron‐hole pairs.The Obtained WO3/GO aerogel exhibited an outstanding visible‐light photocatalytic degradation rate of nitric oxide of 51%,which was 3.3 times that of pristine WO3 powder.In addition,the aerogel displayed excellent selectivity,with a generation fraction of toxic nitrogen dioxide of as low as 0.5%.This work presents a facile synthesis route to fabricate a monolithic WO3/GO aerogel photocatalyst with great promise for air purification.
基金Project supported by the National Key R&D Program of China(2016YFE0126600 and 2017YFC0211002)。
文摘A series of La1-xCexMnO3+δ(x=D,0.05,0.1,0.2,and 0.3)perovskites and Mn-Ce mixed oxides were prepared.Their physico-chemical properties were systematically characterized and the NO oxidation activities of the catalysts were investigated.The La0.9Ce0.1MnO3+δhas the best activity among all of the catalysts,with a maximum NO conversion of 85%at 300℃.The characterization results indicate that the doping of Ce improves the properties of the perovsidtes in terms of the specific surface area,the average valence state of Mn ions,the number of reactive oxygen species and the NOx desorption behaviors.The Mn-Ce mixed oxide calcined at 500℃shows a similar NO oxidation activity with La0.9Ce0.1MnO3+δ.However,the activity of the mixed oxide obtained at 750℃decreases a lot,which results from the loss of active sites and active oxygen species.
