双金属催化剂Fe-Co/Al-PILC的CH_(4)-SCR脱硝性能  

CH_(4)-SCR performance of bimetallic Fe-Co catalysts supported on Al-PILC

作　　者：黄莎莎 苏亚欣[1] 周夏 杨迪 王聪颖 温妮妮 邓文义[1] 周皞 田凤国 HUANG Sha-sha;SU Ya-xin;ZHOU Xia;YANG Di;WANG Cong-ying;WEN Ni-ni;DENG Wen-yi;ZHOU Hao;TIAN Feng-guo(School of Environmental Science and Engineering,Donghua University,Shanghai 201620,China;School of Intelligent Equipment,Changzhou Vocational Institute of Engineering,Changzhou 203164,China)

机构地区：[1]东华大学环境科学与工程学院,上海201620 [2]常州工程技术学院智能装备学院,江苏常州213164

出　　处：《高校化学工程学报》2021年第6期1073-1081,共9页Journal of Chemical Engineering of Chinese Universities

基　　金：上海市自然科学基金(19ZR1400700,19ZR1401800);江苏省自然科学基金(BK20181161);中央高校基本科研业务费(2232019D3-24)。

摘　　要：为了提高甲烷的选择性催化还原NO(CH_(4)-SCR)的效率及其抗烟气中的SO_(2)和H_(2)O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)、N_(2)吸附-脱附、H_(2)程序升温还原(H_(2)-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CH_(4)-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N_(2)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Co^(2+)和游离态Fe^(3+),它们是影响催化剂活性的主要因素。H_(2)-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Brønsted酸,Lewis酸是催化反应的活性酸性位,Fe离子增加了Lewis酸含量。In order to improve efficiency of selective catalytic reduction of NO by methane(CH_(4)-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),N_(2)-adsorption-desorption,temperature-programmed reduction of hydrogen(H_(2)-TPR),pyridine adsorption-Fourier transform,infrared spectroscopy(Py-FTIR)and X-ray photoelectron spectroscopy(XPS),and CH_(4)-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% N_(2) selectivity at 600℃ were achieved with 0.27Fe-Co/Al-PILC,and the resistance to SO_(2) and H_(2)O was obviously improved.The characterization results show that a suitable load of Fe-Co promotes the formation of Co^(2+) and isolated Fe^(3+),which are the dominant factors to affect catalyst activity.H_(2)-TPR results show that Fe lowers reduction temperature and improves reduction performance.Py-FTIR results show that both Lewis and Bronsted 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.

关 键 词：大气污染控制 选择性催化还原 CH_(4)-SCR 双金属催化剂 Fe-Co/Al-PILC 

分 类 号：X511[环境科学与工程—环境工程]