A series of Fe–Mn catalysts was prepared using different supports(kaolin, diatomite, and alumina) and used for NO abatement via low-temperature NH3-selective catalytic reduction(SCR).The results showed that 12 Fe–10 Mn/Kaolin(with the concentration of Fe and Mn 12 and 10 wt.%, respectively) exhibited the highest activity, and more than 95.8% NO conversion could be obtained within the wide temperature range of 120–300℃.The properties of the catalysts were characterized by inductively coupled plasma-atomic emission spectrometry(ICP-AES), thermogravimetry(TG), Brunner–Emmet–Teller(BET)measurements, X-ray diffraction(XRD), H2-temperature programmed reduction(H2-TPR),NH3-temperature programmed desorption(NH3-TPD), X-ray photoelectron spectroscopy(XPS), scanning electron microprobe(SEM) and energy dispersive spectroscopy(EDS)techniques.The support effects resulted in significant differences in the components and structures of catalysts.The 12 Fe–10 Mn/Kaolin catalyst exhibited better dispersion of active species, optimum low-temperature reduction behavior, the largest amount of normalized Br?nsted acid sites, and the highest Mn4+/Mn and Fe3+/(Fe3++ Fe2+), all of which may be major reasons for its superior catalytic activity.
Iron-based catalysts have been explored for selective catalytic reduction(SCR)of NO due to environmentally benign characters and good SCR activity.Mn-W-Sb modified siderite catalysts were prepared by impregnation method based on siderite ore,and SCR perfor-mance of the catalysts was investigated.The catalysts were analyzed by X-ray diffrac-tion,H_(2)-temperature-programmed reduction,Brunauer-Emmett-Teller,Thermogravimetry-derivative thermogravimetry and in-situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS).The modified siderite catalysts calcined at 450℃ mainly consist of Fe_(2)O_(3),and added Mn,W and Sb species are amorphous.3Mn-5W-1.5Sb-siderite catalyst has a wide temperature window of 180-360℃ and good N_(2) selectivity at low temperatures.In-situ DRIFTS results show NH_(4)^(+),coordinated NH_(3),NH_(2),NO_(3)^(-)species(bidentate),NO_(2)-species(nitro,nitro-nitrito,monodentate),and adsorbed NO_(2) can be discovered on the sur-face of Mn-W-Sb modified siderite catalysts,and doping of Mn will enhance adsorbed NO_(2) formation by synergistic catalysis with Fe^(3+).In addition,the addition of Sb can inhibit sulfates formation on the surface of the catalyst in the presence of SO_(2) and H_(2)O.Time-dependent in-situ DRIFTS studies also indicate that both of Lewis and Br?nsted acid sites play a role in SCR of NO by ammonia at low temperatures.The mechanism of NO removal on the 3Mn-5W-1.5Sb-siderite catalyst can be discovered as a combination of Eley-Rideal and Langmuir-Hinshelwood mechanisms with three reaction pathways.The mechanism of NO,oxidized by synergistic catalysis of Fe^(3+)and Mn^(4+/3+)to form NO_(2) among three pathways,reveals the reason of high NO_(x) conversion of the catalyst at medium and low temperatures.
为了研究纳米γFe2O3催化剂选择性催化还原法（SCR）脱硝反应机理,采用微分反应器测量了纳米γFe2O3催化剂上SCR反应的动力学参数,并构建了SCR反应动力学模型.实验数据分析结果表明,NH3,NO和O2的反应级数分别为0,0.78~0.93和0.09~0.11,反应活化能为57.3 k J/mol.原位红外漫反射光谱（DRIFTS）实验结果表明：NH3能够强吸附到催化剂表面并达到饱和,进一步增加NH3的浓度并不能增加NO的转化速率;NO在有氧条件下能吸附到催化剂表面生成吸附态NO2和亚硝酸盐;在低于270℃的情况下SCR反应遵循Langmuir-Hinshelw ood（L-H）反应机理,在高于270℃的情况下则主要遵循Eley-Rideal（E-R）反应机理.
