Perovskite-like oxide La2-xSrxCuO4 (x = 0, 1) single crystallites with microrod-like morphologies and tetragonal crystal structures were prepared hydrothermally at 240 ℃ with poly(ethylene glycol) (PEG) or hexa...Perovskite-like oxide La2-xSrxCuO4 (x = 0, 1) single crystallites with microrod-like morphologies and tetragonal crystal structures were prepared hydrothermally at 240 ℃ with poly(ethylene glycol) (PEG) or hexadecyltrimethyl ammonium bromide (CTAB) as a surfactant and after calcination at 850 ℃. The physicochemical properties of the materials were characterized by means of XRD, BET, SEM, TEM/SAED (selected-area electron diffraction), XPS and H2-TPR techniques. It is found that doping Sr2+ to La2CuO4 lattice enhanced the catalytic activity for methane combustion and the LaSrCuO4 catalyst derived from PEG is the best among the tested ones. It is concluded that factors, such as adsorbed oxygen species concentration, reducibility and surface area, determined the catalytic performance of such single-crystalline materials.展开更多
A series of single-phase T-structured NdSrCu 1-x Co x O 4-δ with oxygen vacancies and T -structured Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ (x: 0–0.4) with oxygen excess were prepared using ultrasound-assisted citric ac...A series of single-phase T-structured NdSrCu 1-x Co x O 4-δ with oxygen vacancies and T -structured Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ (x: 0–0.4) with oxygen excess were prepared using ultrasound-assisted citric acid complexing method, and characterized by means of techniques such as thermogravimetric analysis and NO temperature-programmed desorption (NO-TPD). The catalytic activities of these materials were evaluated for the decomposition of NO. It was found that the NdSrCu 1-x Co x O 4-δ catalysts were of oxygen vacancies whereas the Sm 1.8 Ce 0.2 Cu 1?x Co x O 4-δ ones possessed excessive oxygen (i.e., over-stoichiometric oxygen); with a rise in Co doping level, the oxygen vacancy density of NdSrCu 1-x Co x O 4-δ decreased while the over-stoichiometric oxygen amount of Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ increased. The NO-TPD results revealed that NO could be activated much easier over the oxygen-deficient perovskite-like oxides than over the oxygen-excessive perovskite-like oxides, with the NdSrCuO 3.702 catalyst showing the best efficiency in activating NO molecules. Under the conditions of 1.0% NO/helium, 2800 hr -1 , and 600–900°C, the catalytic activity of NO decomposition followed the order of NdSrCuO 3.702 〉 NdSrCu 0.8 Co 0.2 O 3.736 〉 NdSrCu 0.6 Co 0.4 O 3.789 〉 Sm 1.8 Ce 0.2 Cu 0.6 Co 0.4 O 4.187 〉 Sm 1.8 Ce 0.2 Cu 0.8 Co 0.2 O 4.104 〉 Sm 1.8 Ce 0.2 CuO 4.045 , in concord with the sequence of decreasing oxygen vacancy or oxygen excess density. Based on the results, we concluded that the higher oxygen vacancy density and the stronger Cu 3+ /Cu 2+ redox ability of NdSrCu 1-x Co x O 4-δ account for the easier activation of NO and consequently improve the catalytic activity of NO decomposition over the catalysts.展开更多
The Fe-modi fied sepiolite-supported Mn–Cu mixed oxide(Cux Mny/Fe-Sep) catalysts were prepared using the co-precipitation method.These materials were characterized by means of the XRD,N_2 adsorption–desorption,XPS,H...The Fe-modi fied sepiolite-supported Mn–Cu mixed oxide(Cux Mny/Fe-Sep) catalysts were prepared using the co-precipitation method.These materials were characterized by means of the XRD,N_2 adsorption–desorption,XPS,H_2-TPR,and O_2-TPD techniques,and their catalytic activities for CO and ethyl acetate oxidation were evaluated.The results show that catalytic activities of the Cux Mny/Fe-Sep samples were higher than those of the Cu1/Fe-Sep and Mn2/Fe-Sep samples,and the Mn/Cu molar ratio had a distinct in fluence on catalytic activity of the sample.Among the Cux Mny/Fe-Sep and Cu1Mn2/Sep samples,Cu1Mn2/Fe-Sep performed the best for CO and ethyl acetate oxidation,showing the highest reaction rate and the lowest T50 and T90 of 4.4×10^(-6) mmol·g-1·s-1,110,and 140 °C for CO oxidation,and 1.9×10^(-6) mmol·g-1·s-1,170,and210 °C for ethyl acetate oxidation,respectively.Moreover,the Cu1Mn2/Fe-Sep sample possessed the best lowtemperature reducibility and the lowest temperature of oxygen desorption as well as the highest surface Mn^(4+)/Mn^(3+) and Cu^(2+)/CuO atomic ratios.It is concluded that factors,such as the strong interaction between the Cu or Mn and the Fe-Sep support,good low-temperature reducibility,and good mobility of chemisorbed oxygen species,might account for the excellent catalytic activity of Cu1Mn2/Fe-Sep.展开更多
Semiconductor photocatalytic technology has shown great prospects in converting solar energy into chemical energy to mitigate energy crisis and solve environmental pollution problems.The key issue is the development o...Semiconductor photocatalytic technology has shown great prospects in converting solar energy into chemical energy to mitigate energy crisis and solve environmental pollution problems.The key issue is the development of high-efficiency photocatalysts.Various strategies in the state-of-the-art advancements,such as heterostructure construction,heteroatom doping,metal/single atom loading,and defect engineering,have been presented for the graphitic carbon nitride(g-C3N4)-based nanocomposite catalysts to design their surface chemical environments and internal electronic structures to make them more suitable for different photocatalytic applications.In this review,nanoarchitecture design,synthesis methods,photochemical properties,potential photocatalytic applications,and related reaction mechanisms of the modified high-efficiency carbon nitride-based photocatalysts were briefly summarized.The superior photocatalytic performance was identified to be associated with the enhanced visible-light response,fast photoinduced electron-hole separation,efficient charge migration,and increased unsaturated active sites.Moreover,the further advance of the visible-light harvesting and solar-to-energy conversions are proposed.展开更多
Volatile organic compounds(VOCs),methane,carbon monoxide,soot,automotive exhaust,and nitrogen oxides are harmful to the atmosphere and human health.It is urgent to strictly control their emissions.Heterogeneous cataly...Volatile organic compounds(VOCs),methane,carbon monoxide,soot,automotive exhaust,and nitrogen oxides are harmful to the atmosphere and human health.It is urgent to strictly control their emissions.Heterogeneous catalysis is an effective pathway for the removal of these pollutants,and the critical issue is the development of novel and high-performance catalysts.In this review,we briefly summarize the preparation methods,physicochemical properties,catalytic activities,and related reaction mechanisms for the above pollutants removal of the rare earth oxides,mixed rare earth oxide,rare earth oxidesupported noble metal,and mixed rare earth oxide-supported noble metal catalysts that have been investigated by our group and other researchers.It was found that catalytic performance was associated with the factors,such as specific surface area,pore structure,particle size and dispersion,adsorbed oxygen species concentration,reducibility,reactant activation ability or interaction between metal nanoparticles and support.Furthermore,we also envision the development trend of such a topic in future work.展开更多
The PdPtVO_(x)/CeO_(2)-ZrO_(2)(PdPtVO_(x)/CZO)catalysts were obtained by using different approaches,and their physical and chemical properties were determined by various techniques.Catalytic activities of these materi...The PdPtVO_(x)/CeO_(2)-ZrO_(2)(PdPtVO_(x)/CZO)catalysts were obtained by using different approaches,and their physical and chemical properties were determined by various techniques.Catalytic activities of these materials in the presence of H_(2)O or SO_(2)were evaluated for the oxidation of ethylbenzene(EB).The PdPtVO_(x)/CZO sample exhibited high catalytic activity,good hydrothermal stability,and reversible sulfur dioxide-poisoning performance,over which the specific reaction rate at 160℃,turnover frequency at 160℃(TOF_(Pd or Pt)),and apparent activation energy were 72.6 mmol/(g_(Pt)·sec)or 124.2 mmol/(g_(Pd)·sec),14.2 sec^(-1)(TOF_(Pt))or 13.1 sec^(-1)(TOF_(Pd)),and 58 k J/mol,respectively.The large EB adsorption capacity,good reducibility,and strong acidity contributed to the good catalytic performance of PdPtVO_(x)/CZO.Catalytic activity of PdPtVO_(x)/CZO decreased when 50 ppm SO_(2)or(1.0 vol.%H_(2)O+50 ppm SO_(2))was added to the feedstock,but was gradually restored to its initial level after the SO_(2)was cut off.The good reversible sulfur dioxide-resistant performance of PdPtVO_(x)/CZO was associated with the facts:(i)the introduction of SO_(2)leads to an increase in surface acidity;(ii)V can adsorb and activate SO_(2),thus accelerating formation of the SO_(x)^(2-)(x=3 or 4)species at the V and CZO sites,weakening the adsorption of sulfur species at the PdPt active sites,and hence protecting the PdPt active sites to be not poisoned by SO_(2).EB oxidation over PdPtVO_(x)/CZO might take place via the route of EB→styrene→phenyl methyl ketone→benzaldehyde→benzoic acid→maleic anhydride→CO_(2)and H_(2)O.展开更多
High-surface-area and well-ordered mesoporous Fe-incorporated SBA-15(xFe-SBA-15)and SBA-15-supported FeOx(yFeOx/SBA-15)with the Fe surface density between 0.09 to 1.11 Fe-atom/nm2have been prepared using the one-step ...High-surface-area and well-ordered mesoporous Fe-incorporated SBA-15(xFe-SBA-15)and SBA-15-supported FeOx(yFeOx/SBA-15)with the Fe surface density between 0.09 to 1.11 Fe-atom/nm2have been prepared using the one-step synthesis and incipient wetness impregnation methods,respectively.Physicochemical properties of these materials were characterized by means of numerous techniques,and their catalytic activities for the combustion of toluene were evaluated.It is found that the xFe-SBA-15 and yFeOx/SBA-15 samples possessed rod-or chain-like morphologies.The Fe species were of high dispersion when the Fe surface density was lower than0.76 Fe-atom/nm2in xFe-SBA-15 and 0.64 Fe-atom/nm2in yFeOx/SBA-15.At a similar Fe surface density and space velocity,the xFe-SBA-15 catalysts showed better activity than the yFeOx/SBA-15 catalysts,in which the xFe-SBA-15 catalyst with Fe surface density 0.59 Fe-atom/nm2performed the best.It is concluded that the good performance of the xFe-SBA-15 sample with Fe surface density0.59 Fe-atom/nm2was associated with its large surface area,high Fe species dispersion,and good low-temperature reducibility.展开更多
Atmospheric pollutants such as nitrogen oxides(NO x),carbon monoxide,and volatile organic compounds(VOCs),chiefly emanating from industrial activities and transportation vehicles,are harmful to human health.Catalysis ...Atmospheric pollutants such as nitrogen oxides(NO x),carbon monoxide,and volatile organic compounds(VOCs),chiefly emanating from industrial activities and transportation vehicles,are harmful to human health.Catalysis is one of the most effective and economic technologies to control serious air pollution problems;however,the key issue is the availability of high-performance catalysts.Great efforts have been made to develop展开更多
Nanoparticles of Ce0.6Zr0.35Y0.05O2 (CZY) solid solution have been prepared by the CTAB (hexadecyl-trimethyl ammonium bromide), CTAB-EG (ethylene glycol) templating, and CTAB-EG-NaCl (in which the pores of the precurs...Nanoparticles of Ce0.6Zr0.35Y0.05O2 (CZY) solid solution have been prepared by the CTAB (hexadecyl-trimethyl ammonium bromide), CTAB-EG (ethylene glycol) templating, and CTAB-EG-NaCl (in which the pores of the precursor synthesized by the CTAB-EG method is filled by a certain amount of NaCl) method, respectively. The physical properties of these materials were characterized by means of tech-niques such as X-ray diffraction (XRD), high resolution scanning electron microscopy (HRSEM), transmission electron microscopy (TEM), selected area electron diffraction (SAED), and N2 adsorp-tion-desorption measurements. The CZY samples synthesized by the above three methods display wormhole-like mesoporous morphology and cubic crystal structures. The materials are narrow in pore size distribution (averaged pore diameter = 5.3―7.1 nm), high in surface areas (95―119 m2/g), and large in pore volumes (0.16―0.18 cm3/g). It has been demonstrated that the introduction of NaCl is capable of retaining the pore structures of solid nanomaterials at high-temperature calcination.展开更多
La1?xSrxCoO3?δ (x=0, 0.4) nanoparticles have been prepared using the citric acid complex-ing-hydrothermal synthesis coupled method and citric acid complexing method. The physico-chemical properties of these materials...La1?xSrxCoO3?δ (x=0, 0.4) nanoparticles have been prepared using the citric acid complex-ing-hydrothermal synthesis coupled method and citric acid complexing method. The physico-chemical properties of these materials were characterized by means of X-ray diffraction (XRD), high resolution scanning electron microscopy (HRSEM), element analysis (EDX), X-ray photoelectron spectroscopic (XPS), oxygen temperature-programmed desorption (O2-TPD), hydrogen temperature-programmed re-duction (H2-TPR) as well as surface area measure-ments and oxidation state titration. Their catalytic performance was examined for the total oxidation of ethylacetate (EA). It is found that the La1?xSrxCoO3?δ (x=0, 0.4) catalysts were single-phase and rhombo-hedrally-structured perovskites and their surface ar-eas ranged from 16 to 26 m2/g. The Sr-doped sample derived from the coupled procedure was uniformly distributed nanoparticles with a short rod-shaped morphology. The doping of Sr (i) enhanced the con-centrations of Co3+ and oxygen vacancies, (ii) in-creased the amount of oxygen adsorbed on the sur-face at low temperatures, (iii) promoted the mobility of lattice oxygen, and (iv) improved the properties of redox. The La0.6Sr0.4CoO2.78 catalyst prepared by the citric acid complexing-hydrothermal synthesis cou-pled strategy performed the best in the oxidation of EA, furthermore no partially oxidized products were formed. Based on the above results, we conclude that in addition to the surface area, the catalytic ac-tivity of the perovskite-type oxide nanoparticles was associated with the structural defect (oxygen vacancy) concentration and redox ability.展开更多
A new method called ultrasonic-assisted membrane reaction(UAMR)was reported for the fabrication of ceria-zirconia solid solution.A series of ceria-zirconia solid solutions with different Ce/Zr molar ratios were prepar...A new method called ultrasonic-assisted membrane reaction(UAMR)was reported for the fabrication of ceria-zirconia solid solution.A series of ceria-zirconia solid solutions with different Ce/Zr molar ratios were prepared by the UAMR method and characterized by Xray diffraction(XRD),N2 adsorption,hydrogen temperature-programmed reduction(H2-TPR),scanning electron microscope(SEM),and transmission electron microscopy(TEM)techniques.The UAMR method proved to be superior,especially when the Ce/Zr molar ratio was lower than 1,in fabricating ceria-zirconia solid solutions with large BET surface area,high oxygen storage capacity(OSC),and low reduction temperature.展开更多
Flower-, wire-, and sheet-like MnO2-deposited diatomites have been prepared using a hydrothermal method with Mn(Ac)2, KMnO4 and/or MnSO4 as Mn source and diatomite as support. Physical properties of the materials we...Flower-, wire-, and sheet-like MnO2-deposited diatomites have been prepared using a hydrothermal method with Mn(Ac)2, KMnO4 and/or MnSO4 as Mn source and diatomite as support. Physical properties of the materials were characterized by means of numerous analytical techniques, and their behaviors in the adsorption of chromium(VI) were evaluated. It is shown that the IvinO2-deposited diatomite samples with different morphologies possessed high surface areas and abundant surface hydroxyl groups (especially the wire-like MnO2/diatomite sample). The wire-like MnO2/diatomite sample showed the best performance in the removal of Cr(VI), giving the maximum Cr(VI) adsorption capacity of 101 mg/g.展开更多
CMK-3 and C-FDU-15 samples were synthesized using hard-templating and evaporationinduced self-assembly(EISA)methods,respectively.The pore structures of CMK-3 and CFDU-15 as well as commercial activated carbon were cha...CMK-3 and C-FDU-15 samples were synthesized using hard-templating and evaporationinduced self-assembly(EISA)methods,respectively.The pore structures of CMK-3 and CFDU-15 as well as commercial activated carbon were characterized by means of X-ray diffraction,field emission scanning electron microscopy,transmission electron microscopy,and N2 adsorption–desorption.Adsorption of NO was investigated by means of thermogravimetric analysis,temperature-programmed desorption of NO+O2,and in situ diffuse reflectance Fourier transform infrared spectroscopy.The results show that the CMK-3 and C-FDU-15 materials possessed ordered and uniform structures.The coadsorption capacity of NO and O2 decreased in the sequence CMK-3(88.6 mg/g)>C-FDU-15(71.7 mg/g)>AC(25.3 mg/g).There were two main adsorption species on CMK-3 and CFDU-15:nitrite and nitrate.Nitrite is converted to nitrate easily.However,the adsorption species were more complex on AC,with nitrite being the main species.Moreover,CMK-3 and C-FDU-15 exhibit excellent regeneration efficiency compared with AC.The excellent NO adsorption performance of CMK-3 and C-FDU-15 was associated with their ordered mesoporous structures and high surface areas.The research provides more options for NO adsorption in the future.展开更多
Monoclinic BiVO4 with multiple morphologies and/or porous structures were fabricated using the hydrothermal strategy. The materials were characterized by means of the XRD, Raman, TGA/DSC, SEM, XPS, and UV-Vis techniqu...Monoclinic BiVO4 with multiple morphologies and/or porous structures were fabricated using the hydrothermal strategy. The materials were characterized by means of the XRD, Raman, TGA/DSC, SEM, XPS, and UV-Vis techniques. The photocatalytic activities of the BiVO4 materials were evaluated for the degradation of Methyl Orange under visible-light irradiation. It is observed that pH value and surfactant exerted a great effect on the morphology and pore structure of the BiVO4 product. Spherical BiVO4 with porous structures, flower-cluster-like BiVO4, and flower-bundle-like BiVO4 were generated hydrothermally at 100°C with poly(vinyl pyrrolidone) (PVP) and urea (pH = 2) and at 160°C with NaHCO3 (pH = 7 and 8), respectively. The PVP-derived BiVO4 showed much higher surface areas (5.0-8.4 m2/g) and narrower bandgap energies (2.45-2.49 eV). The best photocatalytic performance of the spherical BiVO4 material with a surface area of 8.4 m2/g was associated with its higher surface area, narrower bandgap energy, higher surface oxygen vacancy density, and unique porous architecture.展开更多
The octahedral molecular sieve(OMS-2)-supported Fe( xFe/OMS-2: x = 1, 3, 5, and 10) catalysts were prepared using the pre-incorporation method. Physicochemical properties of the as-synthesized materials were character...The octahedral molecular sieve(OMS-2)-supported Fe( xFe/OMS-2: x = 1, 3, 5, and 10) catalysts were prepared using the pre-incorporation method. Physicochemical properties of the as-synthesized materials were characterized by means of various techniques, and their catalytic activities for CO, ethyl acetate, and toluene oxidation were evaluated. Among all of the samples, performed the best, with the reaction temperature required to achieve 90% conversion( T 90%) being 160 ℃ for CO oxidation, 210 ℃ for ethyl acetate oxidation, and 285 ℃ for toluene oxidation. Such a good catalytic performance of 5Fe/OMS-2 was associated with its high(Mn^(3+) + Mn^(2+)) content and adsorbed oxygen species concentration, and good lowtemperature reducibility and lattice oxygen mobility as well as strong interaction between Fe and OMS-2. In addition, catalytic mechanisms of the oxidation of three pollutants over the 5Fe/OMS-2 catalyst were also studied. It was found that CO, ethyl acetate or toluene was first adsorbed, then the related intermediates were formed, and finally the formed intermediates were completely converted into CO_(2) and H_(2)O.展开更多
The cryptomelane-type manganese oxide (OMS-2)-supported Co (x Co/OMS-2;x=5,10,and15 wt.%) catalysts were prepared via a pre-incorporation route.The as-prepared materials were used as catalysts for catalytic oxidation ...The cryptomelane-type manganese oxide (OMS-2)-supported Co (x Co/OMS-2;x=5,10,and15 wt.%) catalysts were prepared via a pre-incorporation route.The as-prepared materials were used as catalysts for catalytic oxidation of toluene (2000 ppmV).Physical and chemical properties of the catalysts were measured using the X-ray diffraction (XRD),Fourier transform infrared spectroscopic (FT-IR),scanning electron microscopic (SEM),X-ray photoelectron spectroscopy (XPS),and hydrogen temperature-programmed reduction (H_(2)-TPR)techniques.Among all of the catalysts,10Co/OMS-2 performed the best,with the T90%,specific reaction rate at 245℃,and turnover frequency at 245℃ (TOFCo) being 245℃,1.23×10^(-3)moltoluene/(gcat·sec),and 11.58×10^(-3)sec-1for toluene oxidation at a space velocity of 60,000mL/(g·hr),respectively.The excellent catalytic performance of 10Co/OMS-2 were due to more oxygen vacancies,enhanced redox ability and oxygen mobility,and strong synergistic effect between Co species and OMS-2 support.Moreover,in the presence of poisoning gases CO_(2),SO_(2)or NH_(3),the activity of 10Co/OMS-2 decreased for the carbonate,sulfate and ammonia species covered the active sites and oxygen vacancies,respectively.After the activation treatment,the catalytic activity was partly recovered.The good low-temperature reducibility of 10Co/OMS-2 could also facilitate the redox process accompanied by the consecutive electron transfer between the adsorbed O_(2)and the cobalt or manganese ions.In the oxidation process of toluene,the benzoic and aldehydic intermediates werefirst generated,which were further oxidized to the benzoate intermediate that were eventually converted into H_(2)O and CO_(2).展开更多
Porous S-doped bismuth vanadate with an olive-like morphology and its supported iron oxide (y wt.% FeOx/BiVO4-δS0.08, y = 0.06, 0.76, and 1.40) photocatalysts were fabricated using the dodecylamine-assisted alcohol...Porous S-doped bismuth vanadate with an olive-like morphology and its supported iron oxide (y wt.% FeOx/BiVO4-δS0.08, y = 0.06, 0.76, and 1.40) photocatalysts were fabricated using the dodecylamine-assisted alcohol-hydrothermal and incipient wetness impregnation methods, respectively. It is shown that the y wt.% FeOx/BiVO4-δS0.08 photocatalysts contained a monoclinic scheetlite BiVO4 phase with a porous olive-like morphology, a surface area of 8.8-9.2 m^2/g, and a bandgap energy of 2.38-2.42 eV. There was co-presence of surface Bi^5+, Bi^3+, V^5+, V^3+, Fe^3+, and Fe^2+ species in y wt.% FeOx/BiVO4-δS0.08. The 1.40 wt.% FeOx/BiVO4-δS0.08 sample performed the best for Methylene Blue degradation under visible-light illumination. The photocatalytic mechanism was also discussed. We believe that the sulfur and FeOx co-doping, higher oxygen adspecies concentration, and lower baudgap energy were responsible for the excellent visible-light-driven catalytic activity of 1.40 wt.% FeOx/BiVO4-δS0.08.展开更多
Three-dimensionally ordered mesoporous Fe2O3(meso-Fe2O3) and its supported Au, Pd,and Au-Pd alloy(xA uP dy/meso-Fe2O3; x = 0.08–0.72 wt.%; Pd/Au molar ratio(y) = 1.48–1.85)photocatalysts have been prepared via...Three-dimensionally ordered mesoporous Fe2O3(meso-Fe2O3) and its supported Au, Pd,and Au-Pd alloy(xA uP dy/meso-Fe2O3; x = 0.08–0.72 wt.%; Pd/Au molar ratio(y) = 1.48–1.85)photocatalysts have been prepared via the KIT-6-templating and polyvinyl alcohol-protected reduction routes, respectively. Physical properties of the samples were characterized, and their photocatalytic activities were evaluated for the photocatalytic oxidation of acetone in the presence of a small amount of H2O2 under visible-light illumination. It was found that the meso-Fe2O3 was rhombohedral in crystal structure. The as-obtained samples displayed a high surface area of 111.0–140.8 m^2/g and a bandgap energy of 1.98–2.12 eV. The Au, Pd and/or Au–Pd alloy nanoparticles(NPs) with a size of 3–4 nm were uniformly dispersed on the surface of the meso-Fe2O3 support. The 0.72 wt.% AuP d1.48/meso-Fe2O3 sample performed the best in the presence of 0.06 mol/L H2O2 aqueous solution, showing a 100% acetone conversion within4 hr of visible-light illumination. It was concluded that the good performance of 0.72 wt.%AuPd(1.48)/meso-Fe2O3 for photocatalytic acetone oxidation was associated with its ordered mesoporous structure, high adsorbed oxygen species concentration, plasmonic resonance effect between AuPd(1.48) NPs and meso-Fe2O3, and effective separation of the photogenerated charge carriers. In addition, the introduction of H2O2 and the involvement of the photo-Fenton process also played important roles in enhancing the photocatalytic activity of 0.72 wt.%AuPd(1.48)/meso-Fe2O3.展开更多
Zeolite P was synthesized for the first time via a novel water-bathing route at 90℃ using scrubbed diatomite, sodium hydroxide, and aluminum hydroxide as precursor, with SiO2/Al2O3, SiO2/Na2O, and H2O/Na2O molar rati...Zeolite P was synthesized for the first time via a novel water-bathing route at 90℃ using scrubbed diatomite, sodium hydroxide, and aluminum hydroxide as precursor, with SiO2/Al2O3, SiO2/Na2O, and H2O/Na2O molar ratios of 7.43, 3.81, and 80.00, respectively. The as-fabricated samples were characterized by means of scanning electron microscopy, X-ray diffraction, and nitrogen adsorption measurements. This study showed that (i) treating the diatomite raw material with sodium hexametaphosphate could open the pores in the diatomite via removal of the clay clogged in its pores; (ii) tetragonal mesoporous zeolite P samples with a surface area of 56-60 m2/g could be generated after 6-24 h of water-bathing reaction at 90℃; (iii) extension of water-bathing reaction time could improve the mesoporous structure of zeolite P; and (iv) Ca2+ adsorption capacity of the zeolite P sample was about 300 cmol/kg. Such high-surface-area porous zeolite P could be used as an effective adsorbent for the treatment of water containing calcium and magnesium ions.展开更多
Mesoporous Co3 O4(meso-Co3 O4)-supported Pt(0.53 wt.%Pt/meso-Co304)was synthesized via the KIT-6-templating and polyvinyl alcohol(PVA)-assisted reduction routes.Mesoporous CoO(meso-CoO)was fabricated through in situ r...Mesoporous Co3 O4(meso-Co3 O4)-supported Pt(0.53 wt.%Pt/meso-Co304)was synthesized via the KIT-6-templating and polyvinyl alcohol(PVA)-assisted reduction routes.Mesoporous CoO(meso-CoO)was fabricated through in situ reduction of meso-Co304 with glycerol,and the 0.18-0.69 wt.%Pt/meso-CoO samples were generated by the PVA-assisted reduction method.Meso-Co3 O4 and meso-CoO were of cubic crystal structure and the Pt nanoparticles(NPs)with a uniform size of ca.2 nm were well distributed on the mesoCo3 O4 or meso-CoO surface.The 0.56 wt%Pt/meso-CoO(0.56 Pt/meso-CoO)sample performed the best in benzene combustion(T50%=156℃and T90%=186℃at a space velocity of 80,000 mL/(g h)).Introducing water vapor or C02 with a certain concentration led to partial deactivation of 0.56 Pt/meso-CoO and such a deactivation was reversible.We think that the superior catalytic activity of 0.56 Pt/meso-CoO was intimately related to its good oxygen activation and benzene adsorption ability.展开更多
基金supported by the National Natural Science Foundation of China (No. 20973017 and 21077007)the Creative Research Foundation of Beijing University Technology (No. 00500054R4003)the Creative Research Team of Beijing Municipality (No. PHR201007105)
文摘Perovskite-like oxide La2-xSrxCuO4 (x = 0, 1) single crystallites with microrod-like morphologies and tetragonal crystal structures were prepared hydrothermally at 240 ℃ with poly(ethylene glycol) (PEG) or hexadecyltrimethyl ammonium bromide (CTAB) as a surfactant and after calcination at 850 ℃. The physicochemical properties of the materials were characterized by means of XRD, BET, SEM, TEM/SAED (selected-area electron diffraction), XPS and H2-TPR techniques. It is found that doping Sr2+ to La2CuO4 lattice enhanced the catalytic activity for methane combustion and the LaSrCuO4 catalyst derived from PEG is the best among the tested ones. It is concluded that factors, such as adsorbed oxygen species concentration, reducibility and surface area, determined the catalytic performance of such single-crystalline materials.
基金supported by the Natural Science Foundation of Beijing Municipality Key Class B Project (No.KZ200610005004)the Beijing Municipal Commission of Education (No. PHR200907105)the Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of Beijing Municipality(PHR (IHLB))
文摘A series of single-phase T-structured NdSrCu 1-x Co x O 4-δ with oxygen vacancies and T -structured Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ (x: 0–0.4) with oxygen excess were prepared using ultrasound-assisted citric acid complexing method, and characterized by means of techniques such as thermogravimetric analysis and NO temperature-programmed desorption (NO-TPD). The catalytic activities of these materials were evaluated for the decomposition of NO. It was found that the NdSrCu 1-x Co x O 4-δ catalysts were of oxygen vacancies whereas the Sm 1.8 Ce 0.2 Cu 1?x Co x O 4-δ ones possessed excessive oxygen (i.e., over-stoichiometric oxygen); with a rise in Co doping level, the oxygen vacancy density of NdSrCu 1-x Co x O 4-δ decreased while the over-stoichiometric oxygen amount of Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ increased. The NO-TPD results revealed that NO could be activated much easier over the oxygen-deficient perovskite-like oxides than over the oxygen-excessive perovskite-like oxides, with the NdSrCuO 3.702 catalyst showing the best efficiency in activating NO molecules. Under the conditions of 1.0% NO/helium, 2800 hr -1 , and 600–900°C, the catalytic activity of NO decomposition followed the order of NdSrCuO 3.702 〉 NdSrCu 0.8 Co 0.2 O 3.736 〉 NdSrCu 0.6 Co 0.4 O 3.789 〉 Sm 1.8 Ce 0.2 Cu 0.6 Co 0.4 O 4.187 〉 Sm 1.8 Ce 0.2 Cu 0.8 Co 0.2 O 4.104 〉 Sm 1.8 Ce 0.2 CuO 4.045 , in concord with the sequence of decreasing oxygen vacancy or oxygen excess density. Based on the results, we concluded that the higher oxygen vacancy density and the stronger Cu 3+ /Cu 2+ redox ability of NdSrCu 1-x Co x O 4-δ account for the easier activation of NO and consequently improve the catalytic activity of NO decomposition over the catalysts.
基金Supported by the National Natural Science Foundation of China(21277008,20777005)the Natural Science Foundation of Beijing(8082008)
文摘The Fe-modi fied sepiolite-supported Mn–Cu mixed oxide(Cux Mny/Fe-Sep) catalysts were prepared using the co-precipitation method.These materials were characterized by means of the XRD,N_2 adsorption–desorption,XPS,H_2-TPR,and O_2-TPD techniques,and their catalytic activities for CO and ethyl acetate oxidation were evaluated.The results show that catalytic activities of the Cux Mny/Fe-Sep samples were higher than those of the Cu1/Fe-Sep and Mn2/Fe-Sep samples,and the Mn/Cu molar ratio had a distinct in fluence on catalytic activity of the sample.Among the Cux Mny/Fe-Sep and Cu1Mn2/Sep samples,Cu1Mn2/Fe-Sep performed the best for CO and ethyl acetate oxidation,showing the highest reaction rate and the lowest T50 and T90 of 4.4×10^(-6) mmol·g-1·s-1,110,and 140 °C for CO oxidation,and 1.9×10^(-6) mmol·g-1·s-1,170,and210 °C for ethyl acetate oxidation,respectively.Moreover,the Cu1Mn2/Fe-Sep sample possessed the best lowtemperature reducibility and the lowest temperature of oxygen desorption as well as the highest surface Mn^(4+)/Mn^(3+) and Cu^(2+)/CuO atomic ratios.It is concluded that factors,such as the strong interaction between the Cu or Mn and the Fe-Sep support,good low-temperature reducibility,and good mobility of chemisorbed oxygen species,might account for the excellent catalytic activity of Cu1Mn2/Fe-Sep.
基金supported by the Natural Science Foundation of Anhui Province (No. 1908085ME165)the Anhui Provincial Natural Science Key Foundation (No. 2008085UD07)the Special Funds for the Development of Local Science and Technology from the Central Government in Anhui Province (No. 803214271050)
文摘Semiconductor photocatalytic technology has shown great prospects in converting solar energy into chemical energy to mitigate energy crisis and solve environmental pollution problems.The key issue is the development of high-efficiency photocatalysts.Various strategies in the state-of-the-art advancements,such as heterostructure construction,heteroatom doping,metal/single atom loading,and defect engineering,have been presented for the graphitic carbon nitride(g-C3N4)-based nanocomposite catalysts to design their surface chemical environments and internal electronic structures to make them more suitable for different photocatalytic applications.In this review,nanoarchitecture design,synthesis methods,photochemical properties,potential photocatalytic applications,and related reaction mechanisms of the modified high-efficiency carbon nitride-based photocatalysts were briefly summarized.The superior photocatalytic performance was identified to be associated with the enhanced visible-light response,fast photoinduced electron-hole separation,efficient charge migration,and increased unsaturated active sites.Moreover,the further advance of the visible-light harvesting and solar-to-energy conversions are proposed.
基金Project supported by National Natural Science Foundation of China(21677004,21876006,21622701)National Natural Science Committee of China-Liaoning Provincial People’s Government Joint Fund(U1908204)Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions(IDHT20190503)。
文摘Volatile organic compounds(VOCs),methane,carbon monoxide,soot,automotive exhaust,and nitrogen oxides are harmful to the atmosphere and human health.It is urgent to strictly control their emissions.Heterogeneous catalysis is an effective pathway for the removal of these pollutants,and the critical issue is the development of novel and high-performance catalysts.In this review,we briefly summarize the preparation methods,physicochemical properties,catalytic activities,and related reaction mechanisms for the above pollutants removal of the rare earth oxides,mixed rare earth oxide,rare earth oxidesupported noble metal,and mixed rare earth oxide-supported noble metal catalysts that have been investigated by our group and other researchers.It was found that catalytic performance was associated with the factors,such as specific surface area,pore structure,particle size and dispersion,adsorbed oxygen species concentration,reducibility,reactant activation ability or interaction between metal nanoparticles and support.Furthermore,we also envision the development trend of such a topic in future work.
基金supported by the National Natural Science Foundation Committee of China-Liaoning Provincial People’s Government Joint Fund(No.U1908204)the National Natural Science Foundation of China(21976009)+2 种基金the National Key R&D Program of China(Nos.2022YFB3506200 and 2022YFB3504100)the Beijing Natural Science Foundation(J210006)the R&D Program of Beijing Municipal Education Commisson(No.KZ202210005011)。
文摘The PdPtVO_(x)/CeO_(2)-ZrO_(2)(PdPtVO_(x)/CZO)catalysts were obtained by using different approaches,and their physical and chemical properties were determined by various techniques.Catalytic activities of these materials in the presence of H_(2)O or SO_(2)were evaluated for the oxidation of ethylbenzene(EB).The PdPtVO_(x)/CZO sample exhibited high catalytic activity,good hydrothermal stability,and reversible sulfur dioxide-poisoning performance,over which the specific reaction rate at 160℃,turnover frequency at 160℃(TOF_(Pd or Pt)),and apparent activation energy were 72.6 mmol/(g_(Pt)·sec)or 124.2 mmol/(g_(Pd)·sec),14.2 sec^(-1)(TOF_(Pt))or 13.1 sec^(-1)(TOF_(Pd)),and 58 k J/mol,respectively.The large EB adsorption capacity,good reducibility,and strong acidity contributed to the good catalytic performance of PdPtVO_(x)/CZO.Catalytic activity of PdPtVO_(x)/CZO decreased when 50 ppm SO_(2)or(1.0 vol.%H_(2)O+50 ppm SO_(2))was added to the feedstock,but was gradually restored to its initial level after the SO_(2)was cut off.The good reversible sulfur dioxide-resistant performance of PdPtVO_(x)/CZO was associated with the facts:(i)the introduction of SO_(2)leads to an increase in surface acidity;(ii)V can adsorb and activate SO_(2),thus accelerating formation of the SO_(x)^(2-)(x=3 or 4)species at the V and CZO sites,weakening the adsorption of sulfur species at the PdPt active sites,and hence protecting the PdPt active sites to be not poisoned by SO_(2).EB oxidation over PdPtVO_(x)/CZO might take place via the route of EB→styrene→phenyl methyl ketone→benzaldehyde→benzoic acid→maleic anhydride→CO_(2)and H_(2)O.
基金supported by the National Natural Science Foundation of China (21103005)the Natural Science Foundation of Beijing Municipality (2132015)the Discipline and Postgraduate Education Foundation (20111000501,005000542513551)
文摘High-surface-area and well-ordered mesoporous Fe-incorporated SBA-15(xFe-SBA-15)and SBA-15-supported FeOx(yFeOx/SBA-15)with the Fe surface density between 0.09 to 1.11 Fe-atom/nm2have been prepared using the one-step synthesis and incipient wetness impregnation methods,respectively.Physicochemical properties of these materials were characterized by means of numerous techniques,and their catalytic activities for the combustion of toluene were evaluated.It is found that the xFe-SBA-15 and yFeOx/SBA-15 samples possessed rod-or chain-like morphologies.The Fe species were of high dispersion when the Fe surface density was lower than0.76 Fe-atom/nm2in xFe-SBA-15 and 0.64 Fe-atom/nm2in yFeOx/SBA-15.At a similar Fe surface density and space velocity,the xFe-SBA-15 catalysts showed better activity than the yFeOx/SBA-15 catalysts,in which the xFe-SBA-15 catalyst with Fe surface density 0.59 Fe-atom/nm2performed the best.It is concluded that the good performance of the xFe-SBA-15 sample with Fe surface density0.59 Fe-atom/nm2was associated with its large surface area,high Fe species dispersion,and good low-temperature reducibility.
文摘Atmospheric pollutants such as nitrogen oxides(NO x),carbon monoxide,and volatile organic compounds(VOCs),chiefly emanating from industrial activities and transportation vehicles,are harmful to human health.Catalysis is one of the most effective and economic technologies to control serious air pollution problems;however,the key issue is the availability of high-performance catalysts.Great efforts have been made to develop
基金the National Natural Science Foundation of China (Grant No. 20473006) and PHR (IHLB)
文摘Nanoparticles of Ce0.6Zr0.35Y0.05O2 (CZY) solid solution have been prepared by the CTAB (hexadecyl-trimethyl ammonium bromide), CTAB-EG (ethylene glycol) templating, and CTAB-EG-NaCl (in which the pores of the precursor synthesized by the CTAB-EG method is filled by a certain amount of NaCl) method, respectively. The physical properties of these materials were characterized by means of tech-niques such as X-ray diffraction (XRD), high resolution scanning electron microscopy (HRSEM), transmission electron microscopy (TEM), selected area electron diffraction (SAED), and N2 adsorp-tion-desorption measurements. The CZY samples synthesized by the above three methods display wormhole-like mesoporous morphology and cubic crystal structures. The materials are narrow in pore size distribution (averaged pore diameter = 5.3―7.1 nm), high in surface areas (95―119 m2/g), and large in pore volumes (0.16―0.18 cm3/g). It has been demonstrated that the introduction of NaCl is capable of retaining the pore structures of solid nanomaterials at high-temperature calcination.
基金This work was supported by the Key Project of Science and Technology Development Plan of the Education Committee of Beijing and the Key Project (Class B) of Natural Science Foundation of Beijing (Grant No. KZ200610005004).
文摘La1?xSrxCoO3?δ (x=0, 0.4) nanoparticles have been prepared using the citric acid complex-ing-hydrothermal synthesis coupled method and citric acid complexing method. The physico-chemical properties of these materials were characterized by means of X-ray diffraction (XRD), high resolution scanning electron microscopy (HRSEM), element analysis (EDX), X-ray photoelectron spectroscopic (XPS), oxygen temperature-programmed desorption (O2-TPD), hydrogen temperature-programmed re-duction (H2-TPR) as well as surface area measure-ments and oxidation state titration. Their catalytic performance was examined for the total oxidation of ethylacetate (EA). It is found that the La1?xSrxCoO3?δ (x=0, 0.4) catalysts were single-phase and rhombo-hedrally-structured perovskites and their surface ar-eas ranged from 16 to 26 m2/g. The Sr-doped sample derived from the coupled procedure was uniformly distributed nanoparticles with a short rod-shaped morphology. The doping of Sr (i) enhanced the con-centrations of Co3+ and oxygen vacancies, (ii) in-creased the amount of oxygen adsorbed on the sur-face at low temperatures, (iii) promoted the mobility of lattice oxygen, and (iv) improved the properties of redox. The La0.6Sr0.4CoO2.78 catalyst prepared by the citric acid complexing-hydrothermal synthesis cou-pled strategy performed the best in the oxidation of EA, furthermore no partially oxidized products were formed. Based on the above results, we conclude that in addition to the surface area, the catalytic ac-tivity of the perovskite-type oxide nanoparticles was associated with the structural defect (oxygen vacancy) concentration and redox ability.
基金the National High-Tech Research and Development Program of China(Grant No.2006AA06Z347)the National Natural Science Foundation of China(Grant Nos.20877006 and 20833011).
文摘A new method called ultrasonic-assisted membrane reaction(UAMR)was reported for the fabrication of ceria-zirconia solid solution.A series of ceria-zirconia solid solutions with different Ce/Zr molar ratios were prepared by the UAMR method and characterized by Xray diffraction(XRD),N2 adsorption,hydrogen temperature-programmed reduction(H2-TPR),scanning electron microscope(SEM),and transmission electron microscopy(TEM)techniques.The UAMR method proved to be superior,especially when the Ce/Zr molar ratio was lower than 1,in fabricating ceria-zirconia solid solutions with large BET surface area,high oxygen storage capacity(OSC),and low reduction temperature.
基金financially supported by the Science and Technology Program of Jilin Province (Nos. 20130305015GX, 2014204037SF)the Beijing Natural Science Foundation (No. 2142008)the National Natural Science Foundation of China (No. 51225402)
文摘Flower-, wire-, and sheet-like MnO2-deposited diatomites have been prepared using a hydrothermal method with Mn(Ac)2, KMnO4 and/or MnSO4 as Mn source and diatomite as support. Physical properties of the materials were characterized by means of numerous analytical techniques, and their behaviors in the adsorption of chromium(VI) were evaluated. It is shown that the IvinO2-deposited diatomite samples with different morphologies possessed high surface areas and abundant surface hydroxyl groups (especially the wire-like MnO2/diatomite sample). The wire-like MnO2/diatomite sample showed the best performance in the removal of Cr(VI), giving the maximum Cr(VI) adsorption capacity of 101 mg/g.
基金supported by the National Natural Science Foundation of China(Nos.21277008 and 20777005)the National Key Research and Development Program of China(No.2017YFC0209905)
文摘CMK-3 and C-FDU-15 samples were synthesized using hard-templating and evaporationinduced self-assembly(EISA)methods,respectively.The pore structures of CMK-3 and CFDU-15 as well as commercial activated carbon were characterized by means of X-ray diffraction,field emission scanning electron microscopy,transmission electron microscopy,and N2 adsorption–desorption.Adsorption of NO was investigated by means of thermogravimetric analysis,temperature-programmed desorption of NO+O2,and in situ diffuse reflectance Fourier transform infrared spectroscopy.The results show that the CMK-3 and C-FDU-15 materials possessed ordered and uniform structures.The coadsorption capacity of NO and O2 decreased in the sequence CMK-3(88.6 mg/g)>C-FDU-15(71.7 mg/g)>AC(25.3 mg/g).There were two main adsorption species on CMK-3 and CFDU-15:nitrite and nitrate.Nitrite is converted to nitrate easily.However,the adsorption species were more complex on AC,with nitrite being the main species.Moreover,CMK-3 and C-FDU-15 exhibit excellent regeneration efficiency compared with AC.The excellent NO adsorption performance of CMK-3 and C-FDU-15 was associated with their ordered mesoporous structures and high surface areas.The research provides more options for NO adsorption in the future.
基金supported by the National Natural Science Foundation of China (No. 20973017, 21077007)the Creative Research Foundation of Beijing University of Technology (No. 00500054R4003, 005000543111501)+2 种基金the HiTech Research and Development Program (863)of China (No. 2009AA063201)the Funding Projectfor Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of Beijing Municipality (No. PHR200907105, PHR201007105,PHR201107104)the Hong Kong Baptist University (FRG2/09-10/023)
文摘Monoclinic BiVO4 with multiple morphologies and/or porous structures were fabricated using the hydrothermal strategy. The materials were characterized by means of the XRD, Raman, TGA/DSC, SEM, XPS, and UV-Vis techniques. The photocatalytic activities of the BiVO4 materials were evaluated for the degradation of Methyl Orange under visible-light irradiation. It is observed that pH value and surfactant exerted a great effect on the morphology and pore structure of the BiVO4 product. Spherical BiVO4 with porous structures, flower-cluster-like BiVO4, and flower-bundle-like BiVO4 were generated hydrothermally at 100°C with poly(vinyl pyrrolidone) (PVP) and urea (pH = 2) and at 160°C with NaHCO3 (pH = 7 and 8), respectively. The PVP-derived BiVO4 showed much higher surface areas (5.0-8.4 m2/g) and narrower bandgap energies (2.45-2.49 eV). The best photocatalytic performance of the spherical BiVO4 material with a surface area of 8.4 m2/g was associated with its higher surface area, narrower bandgap energy, higher surface oxygen vacancy density, and unique porous architecture.
基金supported by the National Natural Science Foundation of China (Nos. 21277008 and 20777005)National Key Research and Development Program of China (No. 2017YFC0209905)Natural Science Foundation of Beijing (No. 8082008 )。
文摘The octahedral molecular sieve(OMS-2)-supported Fe( xFe/OMS-2: x = 1, 3, 5, and 10) catalysts were prepared using the pre-incorporation method. Physicochemical properties of the as-synthesized materials were characterized by means of various techniques, and their catalytic activities for CO, ethyl acetate, and toluene oxidation were evaluated. Among all of the samples, performed the best, with the reaction temperature required to achieve 90% conversion( T 90%) being 160 ℃ for CO oxidation, 210 ℃ for ethyl acetate oxidation, and 285 ℃ for toluene oxidation. Such a good catalytic performance of 5Fe/OMS-2 was associated with its high(Mn^(3+) + Mn^(2+)) content and adsorbed oxygen species concentration, and good lowtemperature reducibility and lattice oxygen mobility as well as strong interaction between Fe and OMS-2. In addition, catalytic mechanisms of the oxidation of three pollutants over the 5Fe/OMS-2 catalyst were also studied. It was found that CO, ethyl acetate or toluene was first adsorbed, then the related intermediates were formed, and finally the formed intermediates were completely converted into CO_(2) and H_(2)O.
基金supported by the National Natural Science Foundation of China (Nos. 21277008 and 20777005)National Key Research and Development Program of China (No. 2017YFC0209905)。
文摘The cryptomelane-type manganese oxide (OMS-2)-supported Co (x Co/OMS-2;x=5,10,and15 wt.%) catalysts were prepared via a pre-incorporation route.The as-prepared materials were used as catalysts for catalytic oxidation of toluene (2000 ppmV).Physical and chemical properties of the catalysts were measured using the X-ray diffraction (XRD),Fourier transform infrared spectroscopic (FT-IR),scanning electron microscopic (SEM),X-ray photoelectron spectroscopy (XPS),and hydrogen temperature-programmed reduction (H_(2)-TPR)techniques.Among all of the catalysts,10Co/OMS-2 performed the best,with the T90%,specific reaction rate at 245℃,and turnover frequency at 245℃ (TOFCo) being 245℃,1.23×10^(-3)moltoluene/(gcat·sec),and 11.58×10^(-3)sec-1for toluene oxidation at a space velocity of 60,000mL/(g·hr),respectively.The excellent catalytic performance of 10Co/OMS-2 were due to more oxygen vacancies,enhanced redox ability and oxygen mobility,and strong synergistic effect between Co species and OMS-2 support.Moreover,in the presence of poisoning gases CO_(2),SO_(2)or NH_(3),the activity of 10Co/OMS-2 decreased for the carbonate,sulfate and ammonia species covered the active sites and oxygen vacancies,respectively.After the activation treatment,the catalytic activity was partly recovered.The good low-temperature reducibility of 10Co/OMS-2 could also facilitate the redox process accompanied by the consecutive electron transfer between the adsorbed O_(2)and the cobalt or manganese ions.In the oxidation process of toluene,the benzoic and aldehydic intermediates werefirst generated,which were further oxidized to the benzoate intermediate that were eventually converted into H_(2)O and CO_(2).
基金supported by the National Natural Science Foundation of China(No.21077007)the Natural Science Foundation of Beijing Municipality(No.2102008)+3 种基金the Discipline and Postgraduate Education Foundation(No.PXM2013 014204 07 000261,005000542513551)the Creative Research Foundation of Beijing University of Technology(No.00500054R4003,005000543111501)the Funding Project for Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of Beijing Municipality(No.PHR201007105,PHR201107104)the Hong Kong Baptist University for financial support(No.FRG2/09-10/023)
文摘Porous S-doped bismuth vanadate with an olive-like morphology and its supported iron oxide (y wt.% FeOx/BiVO4-δS0.08, y = 0.06, 0.76, and 1.40) photocatalysts were fabricated using the dodecylamine-assisted alcohol-hydrothermal and incipient wetness impregnation methods, respectively. It is shown that the y wt.% FeOx/BiVO4-δS0.08 photocatalysts contained a monoclinic scheetlite BiVO4 phase with a porous olive-like morphology, a surface area of 8.8-9.2 m^2/g, and a bandgap energy of 2.38-2.42 eV. There was co-presence of surface Bi^5+, Bi^3+, V^5+, V^3+, Fe^3+, and Fe^2+ species in y wt.% FeOx/BiVO4-δS0.08. The 1.40 wt.% FeOx/BiVO4-δS0.08 sample performed the best for Methylene Blue degradation under visible-light illumination. The photocatalytic mechanism was also discussed. We believe that the sulfur and FeOx co-doping, higher oxygen adspecies concentration, and lower baudgap energy were responsible for the excellent visible-light-driven catalytic activity of 1.40 wt.% FeOx/BiVO4-δS0.08.
基金supported by the National Natural Science Foundation of China (No. 21377008)the National High Technology Research and Development Program of China ("863"Program)(No. 2015AA034603)the Foundation of the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions
文摘Three-dimensionally ordered mesoporous Fe2O3(meso-Fe2O3) and its supported Au, Pd,and Au-Pd alloy(xA uP dy/meso-Fe2O3; x = 0.08–0.72 wt.%; Pd/Au molar ratio(y) = 1.48–1.85)photocatalysts have been prepared via the KIT-6-templating and polyvinyl alcohol-protected reduction routes, respectively. Physical properties of the samples were characterized, and their photocatalytic activities were evaluated for the photocatalytic oxidation of acetone in the presence of a small amount of H2O2 under visible-light illumination. It was found that the meso-Fe2O3 was rhombohedral in crystal structure. The as-obtained samples displayed a high surface area of 111.0–140.8 m^2/g and a bandgap energy of 1.98–2.12 eV. The Au, Pd and/or Au–Pd alloy nanoparticles(NPs) with a size of 3–4 nm were uniformly dispersed on the surface of the meso-Fe2O3 support. The 0.72 wt.% AuP d1.48/meso-Fe2O3 sample performed the best in the presence of 0.06 mol/L H2O2 aqueous solution, showing a 100% acetone conversion within4 hr of visible-light illumination. It was concluded that the good performance of 0.72 wt.%AuPd(1.48)/meso-Fe2O3 for photocatalytic acetone oxidation was associated with its ordered mesoporous structure, high adsorbed oxygen species concentration, plasmonic resonance effect between AuPd(1.48) NPs and meso-Fe2O3, and effective separation of the photogenerated charge carriers. In addition, the introduction of H2O2 and the involvement of the photo-Fenton process also played important roles in enhancing the photocatalytic activity of 0.72 wt.%AuPd(1.48)/meso-Fe2O3.
基金supported as a Project of National Natural Science Foundation (No.20973017)
文摘Zeolite P was synthesized for the first time via a novel water-bathing route at 90℃ using scrubbed diatomite, sodium hydroxide, and aluminum hydroxide as precursor, with SiO2/Al2O3, SiO2/Na2O, and H2O/Na2O molar ratios of 7.43, 3.81, and 80.00, respectively. The as-fabricated samples were characterized by means of scanning electron microscopy, X-ray diffraction, and nitrogen adsorption measurements. This study showed that (i) treating the diatomite raw material with sodium hexametaphosphate could open the pores in the diatomite via removal of the clay clogged in its pores; (ii) tetragonal mesoporous zeolite P samples with a surface area of 56-60 m2/g could be generated after 6-24 h of water-bathing reaction at 90℃; (iii) extension of water-bathing reaction time could improve the mesoporous structure of zeolite P; and (iv) Ca2+ adsorption capacity of the zeolite P sample was about 300 cmol/kg. Such high-surface-area porous zeolite P could be used as an effective adsorbent for the treatment of water containing calcium and magnesium ions.
基金supported by the National Natural Science Foundation of China(Nos.21677004,21876006,21607005,21622701,21477005,and U1507108)National Natural Science Foundation of China-Liaoning Provincial People’s Government Joint Fund(U1908204)Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions(IDHT20190503)
文摘Mesoporous Co3 O4(meso-Co3 O4)-supported Pt(0.53 wt.%Pt/meso-Co304)was synthesized via the KIT-6-templating and polyvinyl alcohol(PVA)-assisted reduction routes.Mesoporous CoO(meso-CoO)was fabricated through in situ reduction of meso-Co304 with glycerol,and the 0.18-0.69 wt.%Pt/meso-CoO samples were generated by the PVA-assisted reduction method.Meso-Co3 O4 and meso-CoO were of cubic crystal structure and the Pt nanoparticles(NPs)with a uniform size of ca.2 nm were well distributed on the mesoCo3 O4 or meso-CoO surface.The 0.56 wt%Pt/meso-CoO(0.56 Pt/meso-CoO)sample performed the best in benzene combustion(T50%=156℃and T90%=186℃at a space velocity of 80,000 mL/(g h)).Introducing water vapor or C02 with a certain concentration led to partial deactivation of 0.56 Pt/meso-CoO and such a deactivation was reversible.We think that the superior catalytic activity of 0.56 Pt/meso-CoO was intimately related to its good oxygen activation and benzene adsorption ability.