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双金属催化剂Fe-Co/Al-PILC的CH4-SCR脱硝性能
CH4-SCR performance of bimetallic Fe-Co catalysts supported on Al-PILC
【摘要】 为了提高甲烷的选择性催化还原NO(CH4-SCR)的效率及其抗烟气中的SO2和H2O的能力,以铝离子柱撑黏土为载体,制备铁-钴双金属催化剂(Fe-Co/Al-PILC)。采用X射线衍射(XRD)、N2吸附-脱附、H2程序升温还原(H2-TPR)、吡啶吸附红外光谱(Py-FTIR)、X射线光电子能谱(XPS)等方法表征催化剂的物化性质,在固定床微型反应器上对其CH4-SCR特性进行系统评估。结果表明,Fe-Co/Al-PILC具有较好的脱硝反应活性,其中0.27Fe-Co/Al-PILC(0.27为Fe与Co的质量分数比)在600℃时达到63.5%的脱硝效率和100%的N2选择性,其抗水抗硫性能也大大提高。催化剂物化性质的表征结果表明,适量的Fe-Co负载量有利于催化剂中形成Co2+和游离态Fe3+,它们是影响催化剂活性的主要因素。H2-TPR结果表明,Fe离子使催化剂的还原温度降低,还原性能增强。吡啶吸附-红外光谱结果表明,催化剂表面同时存在Lewis酸和Br?nsted酸,Lewis酸是催化反应的活性酸性位,Fe离子增加了Lewis酸含量。
【Abstract】 In order to improve efficiency of selective catalytic reduction of NO by methane (CH4-SCR),Al-pillared clays were used as the supports to prepare Fe-Co/Al-PILCs bimetallic catalysts.The physical-chemical properties were characterized by X-ray diffraction (XRD),N2-adsorption-desorption,temperature-programmed reduction of hydrogen (H2-TPR),pyridine adsorption-Fourier transform,infrared spectroscopy (Py-FTIR) and X-ray photoelectron spectroscopy (XPS),and CH4-SCR reactivity was evaluated in a fixed bed micro-reactor.The results show that Fe-Co/Al-PILCs are active to reduce NO.63.5%NO reduction and 100%N2 selectivity at 600℃were achieved with 0.27Fe-Co/Al-PILC,and the resistance to SO2 and H2O was obviously improved.The characterization results show that a suitable load of Fe-Co promotes the formation of Co2+and isolated Fe3+,which are the dominant factors to affect catalyst activity.H2-TPR results show that Fe lowers reduction temperature and improves reduction performance.Py-FTIR results show that both Lewis and Br?nsted acids exist on the catalyst surface and Lewis acid is the active acid site for the catalytic reaction.Fe increases the content of Lewis acid.
【Key words】 air pollutant emission control; selective catalytic reduction; CH4-SCR; bimetallic catalysts; Fe-Co/Al-PILC;
- 【文献出处】 高校化学工程学报 ,Journal of Chemical Engineering of Chinese Universities , 编辑部邮箱 ,2021年06期
- 【分类号】TQ426;X701
- 【被引频次】1
- 【下载频次】231