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1.
Spinel cobalt manganese oxide nano-composites were grown on nanosheets using acetate precursors in mono-ethylene glycol. Crystal structures and morphologies of nano-composites were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy and energy dispersive X-ray spectroscopy to characterize the element composition. Fourier transform infrared spectroscopy was used for structural characterization and UV–Vis diffuse reflectance spectra (UV–Vis DRS) for optical properties. XRD results showed tetragonal spinel cobalt manganese oxide (Co,Mn)(Co,Mn)2O4 and cubic spinel cobalt manganese oxide MnCo2O4.5 structural phases. The crystallite size calculated by the Scherrer’s equation was 17 nm. The morphological studies displayed the existence of 40–63 nm nano-powders grown on nanosheets with a good degree of crystallization. Optical properties of cobalt manganese oxide nano-composites exhibit absorbance edge, and the band gap calculated from UV–Vis DRS results was 1.78 eV. FTIR spectra indicated that hydroxyl and oxide groups were major active sites. The absorption bands observed at 656 and 568 cm?1 are related to stretching vibrations of Mn–O and Co–O, respectively. The photocatalytic activities of nano-composites for photocatalytic mineralization of Acid Black 1 textile dye showed an outstanding performance. Photocatalytic process yielded 91% total organic carbon removals within 2.5 h of irradiation. The enhanced photocatalytic activity was attributed to better charge separation of the photo-generated electron–hole pairs in nano-composite.  相似文献   

2.
Pyridine derivative complexes are widely employed as biological active materials especially as antibacterial agents. Five transition metal(II) mpk complexes (mpk = methyl 2-pyridyl ketone) were synthesized and investigated using elemental analysis, spectroscopic techniques (IR and UV–Vis–NIR) and conductometric measurements. The general formulae established from experimental data were found to be [M(mpk)2(NO3)2xH2O (x = 0 for M = Cd(II), Zn(II), x = 2 for M = Cu(II)) and [M(mpk)2(H2O)2](NO3)2 (M = Co(II), Ni(II)). These compositions were further confirmed by thermal analysis and their thermal stability in dynamic air atmosphere investigated.  相似文献   

3.
Manganese–copper bimetal oxide catalysts supported on ZSM5 and acid-treated multi-walled carbon nanotubes (MWCNTs) were produced by incipient wetness impregnation for selective catalytic reduction of NO with dielectric barrier discharge plasma. Plasma can activate molecules even at ambient temperature, generating active oxygen species such as O, O3, and HO2 radicals, which can oxidize NO to NO2 effectively. The SCR activity of Mn–Cu/MWCNTs was studied and compared to that of the Mn–Cu/ZSM5. The obtained samples were characterized by XRD, SEM, TEM, ICP, H2-TPR, Raman spectroscopy, and XPS. The results show that MnCu/MWCNTs catalyst possesses NO removal activity superior to that of the MnCu/ZSM5 catalyst. MWCNTs-based catalyst attains NO removal efficiency of 88% at 480 J/L, while the ZSM5-supported catalyst achieves NO removal efficiency of 82% at the same energy density. The oxygen content increased from 3.33 to 19.07% on the nanotube surface after introducing Mn and Cu, which almost remained unchanged on ZSM5. The oxygen-containing functionalities are important for NOx adsorption and removal. Moreover, the characterization revealed that CuO is the main phase of copper oxide, but copper dispersion decreases on MnCu/ZSM5 surface because of the formation of copper dimer species. The manganese is well-dispersed on the catalysts, MnO2 and Mn2O3 contents of MnCu/MWCNTs are larger than that of MnCu/ZSM5, MnO2 is the predominant phase of manganese oxide.  相似文献   

4.
We present the principles of stoichiography and a reference-free stoichiographic differential (separating) dissolution method used to study the composition and structure of thin films and nanostructured systems: HTS films with 123 different compositions, Al–Au–Sn–Co–Mn, Si/SiO2/Ni(Cr)–Cu–Cu2S, Cr–Cu–S, and Cu–S multilayer films, Bi–Ti–O films on Ru/SiO2/Si, Mn1–xZn x S, and ZnS–EuS supports, and also nanostructured manganese ferrite in borate glass matrices, nanodisperse composite sorbents and the Co–Si–Pt–O/Al2O3 catalyst modified by Pt nanoparticles, and oxide catalyst precursor Fe2Co/Al2O3 for the synthesis of carbon nanotubes.  相似文献   

5.
2-Hydroxy salicylhydrazide isatin hydrazone (L) and its Mn (II), Co (II), Ni (II), Cu (II), and Zn (II), metal complexes were synthesized. 1H NMR, UV–Vis, IR spectroscopy and elemental (CHN/S) analysis techniques were applied for characterization. TG/DTA techniques revealed that all the synthetic compounds are thermally stable up to 300 °C. They were found non-electrolytes in nature. Furthermore, all these complexes were evaluated for antiglycation and DPPH radical scavenging activities. They showed varying degree of activity with IC50 values between 168.23 and 269.0 μM in antiglycation and 29.63–57.71 μM in DPPH radical scavenging activity. Mn (II), Co (II), Ni (II), Cu (II), and Zn (II), metal complexes showed good antiglycation as well as DPPH radical scavenging activity. The IC50 values for antiglycation activity are 168.23 ± 2.37, 234.27 ± 4.33, 257.1 ± 6.43, 267.7 ± 8.43, 269.0 ± 8.56 Ni for Co, Zn, Mn, Cu, and Ni complexes, respectively, while IC50 value were found to be 29.63 ± 2.76, 31.13 ± 1.41, 35.16 ± 2.45, 43.53 ± 3.12, 57.71 ± 2.61 μM for Cu, Zn, Mn, Co and Ni complexes, respectively, for DPPH radical scavenging activity. These synthesized metal complexes were found to be better active than standards Rutin (IC50 = 294.46 μM) for anti-glycation, and tert-butyl-4-hydroxyanisole (IC50 = 44.7 μM) for DPPH radical scavenging activity.  相似文献   

6.
The Cu/ZSM-5 catalysts prepared by different copper precursors were used for the selective catalytic reduction (SCR) of NO x with NH3. The Cu/ZSM-5 catalyst prepared by the copper nitrate (Cu/ZSM-5-N) presented the best performance among the Cu/ZSM-5 catalysts and showed above 90 % NO x conversion at 225–405 °C. The average particle size of CuO was 5.82, 9.20, and 11.01 nm over Cu/ZSM-5-N, Cu/ZSM-5-S (prepared by copper sulfate), and Cu/ZSM-5-C (prepared by copper chloride), respectively. The Cu/ZSM-5-N catalyst showed the highly dispersed copper species, the strong surface acidity, and the excellent redox ability compared with the Cu/ZSM-5-C and Cu/ZSM-5-S catalysts. The Cu+ and Cu2+ existed in the Cu/ZSM-5 catalysts and the abundant Cu+ over Cu/ZSM-5-N might be responsible for the superior SCR activity.  相似文献   

7.
Manganese-based catalysts have attracted much attention due to their excellent performance for NO reduction with NH3 (NH3-SCR) at low temperatures. In the current study, the novel metal Sb was modified into Mn/TiO2 and Fe–Mn/TiO2, and the NO x conversion was compared with those of Mn/TiO2 and Fe–Mn/TiO2 catalysts to investigate the effect of the Sb. The NO x reduction activities of the catalysts were evaluated in the temperature range of 100–250 °C at a space velocity of 60,000 h?1. The physicochemical properties of all the catalysts were characterized by Brunauer–Emmett–Teller surface area, temperature-programmed desorption of ammonia, temperature-programmed reduction, X-ray photoelectron spectroscopy, X-ray diffraction, and high-resolution transmission electron microscopy. Interestingly, the Sb-promoted Mn-based catalysts showed significantly higher NO x conversion than the other catalysts with or without 6 vol% of H2O. The high performance of the Sb-modified catalysts could be related to the increase of acid sites and redox properties.  相似文献   

8.
The Co–Mn/Ti–Ce catalyst prepared by sol–gel and impregnation method was evaluated for catalytic oxidation of Hg0 in the simulated flue gas compared with Co/TiO2 and Co–Mn/TiO2. The results showed that Co–Mn/Ti–Ce catalyst exhibited higher catalytic activity (around 93% Hg0 removal efficiency in the temperature of 150 °C with 6% O2, 400 ppm NO, 200 ppm SO2 and 3% H2O) than Co/TiO2 and Co–Mn/TiO2. Based on the characterization results of N2 adsorption–desorption, XRD, UV–Vis, XPS, H2-TPR and Hg-TPD, it could be concluded that the lower band gap, better reducibility and mercury adsorption capability and the presence of Co3+/Co2+, Mn4+/Mn3+ and Ce4+/Ce3+ redox couples as well as surface oxygen species contributed to the excellent Hg0 oxidation removal performance. In addition, well dispersion of active components and a synergetic effect among Co, Mn and Ce species might improve the activity further. A Mars–Maessen mechanism is thought to be involved in the Hg0 oxidation. The lattice oxygen derived from MnO x or CoO x would react with adsorbed Hg0 to form HgO and the consumption of lattice oxygen could be replenished by O2. For Co–Mn/Ti–Ce, MnO x?1 could be alternatively reoxidized by the lattice oxygen derived from adjacent CoO x and CeO x which is beneficial to the Hg0 oxidation.  相似文献   

9.
The photo-assisted selective catalytic reduction (SCR) of NO with NH3 (Photo-SCR) was performed over TiO2 modified by supporting 1 wt% of various transition metal (V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Ta or W) oxides aiming at the improvement of the photo-SCR activity. The addition of Nb, Mo or W oxide to TiO2 was found to enhance the photo-SCR activity. We have reported that the amount of acid sites on TiO2 is one of the key factors to the photo-SCR activity. The increase in the activity depends on the enhancement of acidity of catalyst by the addition of Nb, Mo or W oxide. In contrast, the addition of V, Cr, Mn, Fe, Co, Ni or Cu oxide to TiO2 lowered the photo-SCR activity, although addition of metal cations also changed the acidity of TiO2. We guess that the reduction of the activity was caused by two reasons; the first is that the sites newly formed on these transition metal oxides is not photoactive and the second is that TiO2 supporting V, Cr, Mn, Fe, Co, Ni or Cu oxides had low stabilities under the reaction conditions, i.e., the chemical state of the cations changed during the reaction. Therefore, we concluded that the increase in the acid sites that are active sites for photo-SCR and the stability of the catalysts are important for the photo-SCR.  相似文献   

10.
Catalytic properties of MnOx-FeOx complex oxide (hereafter denoted as Mn-Fe) catalysts modified with different loadings of chromium oxide were investigated by using the combination of physico-chemical techniques, such as N2 physisorption, X-ray diffraction (XRD), high-resolution transmission electron microscope (HRTEM), in situ Fourier transform infrared spectroscopy (in situ FT-IR) and temperature-programmed reduction (TPR) and their catalytic activities were evaluated with the selective catalytic reduction (SCR) of NOx by NH3. It was found that with the addition of Cr, more NO could be removed in the low-temperature window (below 120 °C). Among the tested catalysts, Mn-Fe-Cr (2 : 2 : 1) catalyst exhibited the best catalytic performance at 80 °C with the NO conversion higher than 90%. The combination of the reaction and characterization results indicated that (1) the strong interaction among tertiary metal oxides existed in the catalysts when Cr was appropriately added, which made the active components better dispersed with less agglomeration and sintering and the largest BET specific surface area could be obtained; (2) Cr improved the low-temperature reducibility of the catalyst and promoted the formation of the active intermediate (–NH+3), which favored the low-temperature SCR reaction.  相似文献   

11.
Coordination polymers were obtained by the reaction of metal acetates, M(CH3COO)2·xH2O {where M = Mn(II), Co(II), Ni(II) and Cu(II)} with AFP ligand (AFP = 5,5'-(piperazine-1,4-diylbis(methylene))bis(2-aminobenzoic acid). The AFP ligand was prepared by the one-pot, two-step reaction of formaldehyde, 2-aminobenzoic acid, and piperazine. Structural and spectroscopic properties have been studied by elemental, spectral (FT-IR, 1H NMR, 13C NMR, and UV–vis), and thermogravimetric analysis. UV–vis spectra and magnetic moment values indicate that Mn(II), Co(II), and Ni(II) polymer–metal complexes are octahedral, while Cu(II) and Zn(II) polymer–metal complexes are distorted octahedral and tetrahedral, respectively. The analytical data confirmed that the coordination polymers of Mn(II), Co(II), Ni(II), and Cu(II) are coordinated with two water molecules, which are further supported by infrared spectra and thermogravimetric analysis data. The prepared polymer–metal complexes showed good antibacterial activities against all tested microorganisms; however, the AFP ligand was also found to be effective, but relatively less than their polymer–metal complexes. Along with antibacterial activity, all the polymer–metal complexes exhibit significant antifungal activity against most of the tested fungal strains. The results of antimicrobial activity reveals that the AFP–Cu(II) showed the highest antibacterial and antifungal activity than other polymer–metal complexes.  相似文献   

12.
A series of NiMnTi mixed metal oxides (Ni/Mn-TiO2, Mn/NiTi-LDO and TiO2/NiMn-LDO, NiMnTi-LDO) were synthesized via different assembling methods and evaluated in the selective catalytic reduction of NOx with NH3(NH3-SCR). As the results presented, catalysts via diverse assembling methods of LDHs templates afforded different catalytic denitrification (DeNOx) performance, which might be related to the exposure degree of active constituents and the interaction intensity between metal components. Noticeably, compared with Ni/Mn-TiO2, Mn/NiTi-LDO and TiO2/NiMn-LDO catalysts, the NiMnTi-LDO catalyst deriving from one step in-situ method NiMnTi-LDH precursor template exhibited the most desirable performance at temperature window of 150–360 °C in NH3-SCR (above 90% NOx conversion with 95% N2 selectivity). The specific structure and property of samples were correlated by means of a series of characterizations, where the results indicated that NiMnTi-LDO possessed the highest surface area, the strongest redox ability, the most abundant acid amount and the best dispersion.  相似文献   

13.
Different amounts of Mn and Ce oxides were loaded onto nitric acid-modified activated carbon (ACN) by wet impregnation. The series of catalysts were employed for the selective catalytic reduction of NO x by NH3 at temperatures between 100 and 250 °C. Cerium-modified catalysts exhibited higher de-NO x performance than those modified with Mn/ACN, even with the same total loadings. The precursor solution with a molar ratio for Ce/(Mn + Ce) of 0.4 exhibited the highest catalytic activity. Enhanced resistance to SO2 and H2O and better stability were observed for 10%Mn–Ce(0.4)/ACN relative to 10%Mn/ACN. The catalysts were further characterized by N2 physisorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), hydrogen temperature-programmed reduction (H2-TPR), and temperature-programmed desorption of ammonia (NH3-TPD). The N2 physisorption and XRD results suggested that co-doping Ce with Mn increased the surface area and promoted the dispersion of Mn–Ce binary metal oxides. H2-TPR the NH3-TPD results demonstrated that the interaction between manganese oxide and cerium oxide species enhanced the redox and surface acidity of 10%Mn–Ce(0.4)/ACN.  相似文献   

14.
New seven metal complexes of tioconazole drug with the general formulae [MCl2(L)2(H2O)x].yH2O (where, x = 0 and y = 1 for M = Mn(II) or x = 2, y = 2 for M = Co(II)), and x = 0, y = 3 for M = Cu(II), Ni(II), Zn(II)) and [MCl2(L)2(H2O)2]Cl.3H2O (where M = Cr(III) and Fe(III)) have been prepared and characterized based on elemental analyses, IR, magnetic moment, molar conductance, and thermal analyses techniques. From molar conductance data bivalent metal chelates are non-electrolytes while Cr(III) and Fe(III) chelates are electrolytes and of 1:1 type. According to the IR spectral data, TCNZ is coordinated to the metal ions in a neutral unidentate manner with N donor site of the imidazole–N. All the complexes are octahedral except Mn(II) complex has tetrahedral structure. TCNZ drug and its metal complexes were also screened for their biological activity.  相似文献   

15.
Manganese–cobalt–cerium oxide (Mn–Co–Ce–Ox) catalysts were synthesized by the co-precipitation method and tested for activity in low-temperature catalytic oxidation of NO in the presence of excess O2. With the best Mn–Co–Ce mixed-oxide catalyst, approximately 80 % NO conversion was achieved at 150 °C and a space velocity of 35,000 h?1. The effect of reaction conditions (reaction temperature, volume fractions of NO and O2, gas hourly space velocity (GHSV), and catalyst stability) was investigated. The optimum reaction temperature was 150 °C. Increasing the O2 content above 3 % results in almost no improvement of NO oxidation. This catalyst enables highly effective removal of NO within a wide range of GHSV. Furthermore, the stability of the Me–Co–Ce–Ox catalyst was excellent; no noticeable decrease of NO conversion was observed in 40 h.  相似文献   

16.
Co-M(M=La,Ce, Fe,Mn, Cu,Cr)复合金属氧化物催化分解N2O   总被引:1,自引:0,他引:1  
薛莉  贺泓 《物理化学学报》2007,23(5):664-670
通过共沉淀法制备了一系列Co-M(M= La, Ce, Fe, Mn, Cu, Cr)复合金属氧化物及纯Co3O4催化剂, 考察了其催化分解N2O 的活性. 结果表明在研究的系列催化剂中, Co-Ce 复合氧化物催化剂具有最好的催化分解N2O的活性; 其活性与Ce/Co 摩尔比有直接的关系, 当Ce/Co 摩尔比为0.05 时(CoCe0.05 催化剂)催化活性最佳; 当有NO 和O2共存时, 可能在催化剂活性中心上形成表面硝酸盐或亚硝酸盐吸附物种而使其活性受到较大影响. 通过对Co-M 催化剂的XRD、BET、O2-TPD及H2-TPR 等表征结果的分析, 发现作为主要活性位的Co2+的氧化还原能力是影响催化剂活性的主要原因. 这是因为根据反应机理, N2O 的表面分解步骤与Co2+氧化成Co3+的能力相关, 而吸附氧的脱附与Co3+还原成Co2+的能力相关. 在所研究的催化剂中, 添加除CeO2之外的其它过渡金属氧化物时, 催化剂中Co3+/Co2+的氧化还原能力降低, 因此其催化性能降低. 另外, 添加不同过渡金属氧化物也改变了N2O 催化分解反应的速控步骤.  相似文献   

17.
Cu–Mn bimetal catalysts were prepared to remove nitrogen oxides (NOx) from diesel engine exhaust at low temperatures. At a Cu/Mn ratio of 3:2, the NOx conversions at 200 °C reached 65% and 90% on Cu–Mn/ZSM-5 and Cu–Mn/SAPO-34, respectively. After a hydrothermal treatment and reaction in the presence of C3H6, the activity of Cu–Mn/SAPO-34 was more stable than that of Cu–Mn/ZSM-5. No obvious variations in the crystal structure or dealumination were observed, whereas the physical structure was best maintained in Cu–Mn/SAPO-34. The atomic concentration of Cu on the surface of Cu–Mn/SAPO-34 was quite stable, and the consumption of octahedrally coordinated Cu2+ could be recovered. Conversely, the proportion of octahedrally coordinated Cu2+ on the surface of Cu–Mn/ZSM-5 significantly decreased. Therefore, besides the structure, the redox cycle between Cu+ and octahedrally coordinated Cu2+ played an important role in the stability of the catalysts.  相似文献   

18.
Crystalline NO[Mn(NO3)3] ( I ) and (NO)2[Co(NO3)4] ( II ) were synthesized by reaction of the corresponding metal and a liquid N2O4/ethylacetate mixture. I is orthorhombic, Pca21, a = 9.414(2), b = 15.929(3), c = 10.180(2) Å, Z = 4, R1 = 0.0286. II is monoclinic, C2/c, a = 14.463(3), b = 19.154(4), c = 13.724(3) Å, β = 120.90(3), Z = 12, R1 = 0.0890. Structure I consists of [Mn(NO3)3] sheets with NO+ cations between them. Two types of Mn atoms have CNMn = 7 and 8. Structure II is ionic containing isolated [Co(NO3)4]‐anions and NO+ cations with CNCo = 8. Crystals of Mn(NO3)2 ( III ) and Co(NO3)2 ( IV ) were obtained by concentration of metal nitrate hydrate solutions in 100% HNO3 in a desiccator with P2O5. III is cubic, Pa 3, a = 7.527(2) Å, Z = 4, R1 = 0.0987. IV is trigonal, R 3, a = 10.500(2), c = 12.837(3) Å, Z = 12, R1 = 0.0354. The three dimensional structure III is isotypic to the strontium and barium dinitrates. Structure IV contains a three dimensional network of interconnected Co(NO3)6/3 units with a distorted octahedral coordination environment of Co atoms. General correlations between central atom coordination and coordination modes of NO3 groups are discussed.  相似文献   

19.
The Co–Mg–Al mixed metal oxides were prepared by calcination of co-precipitated hydrotalcite-like precursors at various temperatures (600–800 °C), characterised with respect to chemical (AAS) and phase (XRD) composition, textural parameters (BET), form and aggregation of cobalt species (UV–vis-DRS) and their redox properties (H2-TPR, cyclic voltammetry). Moreover, the process of thermal decomposition of hydrotalcite-like materials to mixed metal oxide systems was studied by thermogravimetric method combined with the analysis of gaseous decomposition products by mass spectrometry. Calcined hydrotalcite-like materials were tested as catalysts for methanol incineration. Catalytic performance of the oxides depended on cobalt content, Mg/Al ratio and calcination temperature. The catalysts with lower cobalt content, higher Mg/Al ratio and calcined at lower temperatures (600 or 700 °C) were less effective in the process of methanol incineration. In a series of the studied catalysts, the best results, with respect to high catalytic activity and selectivity to CO2, were obtained for the mixed oxide with Co:Mg:Al molar ratio of 10:57:33 calcined at 800 °C. High activity of this catalyst was likely connected with the presence of a Co–Mg–Al spinel-type phases, containing easy reducible Co3+ cations, formed during high-temperature treatment of the hydrotalcite-like precursor.  相似文献   

20.
Catalysts active in ammonia oxidation have been obtained by the substitution of transition metal (Mn, Fe, Co, Ni, and Cu) ions for Mg ions in the cordierite structure 2MgO · 2Al2O3 · 5SiO2 at 1100°C. Their phase composition, texture, and activity depend on the type and amount of introduced transition metal oxide. The Mn- and Cu-containing catalysts, which consist of substituted cordierites 2(Mg1 ? x M x )O · 2Al2O3 · 5SiO2 and Mn2O3 or CuO crystallites located on their surface, are most active in ammonia oxidation. The catalysts are characterized by a small specific surface area and have large pores, whose total volume is small. The Fe-containing catalysts consist of the Fe-substituted cordierite phase and particles of an iron oxide phase. These particles are mostly located in internal pores of the catalysts and are, therefore, hardly accessible to ammonia molecules. The introduction of Co or Ni oxide leads to the formation of a low-active spinel phase rather than the cordierite phase.  相似文献   

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