CuCr_(2)O_(4)催化剂形貌特征与其SCR脱硝性能的关系  

Relationship between morphology characteristics of CuCr_(2)O_(4) catalyst and its SCR denitrification activity

作　　者：高尔豪 寿恬雨 黄蓓 王伟 施耀[2] GAO Er-hao;SHOU Tian-yu;HUANG Bei;WANG Wei;SHI Yao(School of Environmental and Safety Engineering,Changzhou University,Changzhou 213164,China;College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310027,China;Zhejiang Feida Environmental Protection Technology Limited Company,Zhuji 311800,China)

机构地区：[1]常州大学环境与安全工程学院,江苏常州213164 [2]浙江大学化学工程与生物工程学院,浙江杭州310027 [3]浙江菲达环保科技股份有限公司,浙江诸暨311800

出　　处：《浙江大学学报（工学版）》2022年第6期1199-1205,共7页Journal of Zhejiang University：Engineering Science

基　　金：江苏省自然科学基金资助项目(BK20210857);江苏省普通高校自然科学研究资助项目(21KJB610006);常州大学科研启动基金资助项目(ZMF21020016)。

摘　　要：分别制备形貌为多面体状、颗粒状、球状的尖晶石型CuCr_(2)O_(4)催化剂,测试对比不同形貌CuCr_(2)O_(4)催化剂的SCR脱硝性能.结果表明,多面体状CuCr_(2)O_(4)的催化活性最好,且在157℃时脱硝效率达到50%,在225~320℃脱硝效率超过99%,具有良好的抗硫、抗水性能.脱硝活性由大到小依次为多面体状CuCr_(2)O_(4)、颗粒状CuCr_(2)O_(4)、球状CuCr_(2)O_(4).采用表征技术分析微观形貌对CuCr_(2)O_(4)脱硝性能的影响.N_(2)吸附-脱附结果显示,多面体状CuCr_(2)O_(4)具有最大的比表面积(25.5 m^(2)/g)和最大的孔容积(0.154 cm^(3)/g);X射线光电子能谱(XPS)结果显示,多面体状CuCr_(2)O_(4)相较于其他形貌拥有更高比例的表面活性氧(49.5%)和Cu^(+)(16.2%);NH_(3)-程序升温脱附(NH_(3)-TPD)结果显示,多面体状CuCr_(2)O_(4)拥有最高表面酸浓度(0.12 mmol/g)及酸强度;H_(2)-程序升温还原(H_(2)-TPR)结果显示,多面体状CuCr_(2)O_(4)表面活性物种最易还原且数量最多(3.69 mmol/g),使得SCR反应在低温段更易进行.多面体状CuCr_(2)O_(4)的高表面酸性与氧化还原性,使其具有良好的脱硝性能.The SCR denitrification activities of CuCr_(2)O_(4)catalysts with various morphologies were tested and compared.The spinel-type CuCr_(2)O_(4)catalysts with polyhedral,granular and spherical shapes were prepared,respectively.The results showed that polyhedral CuCr_(2)O_(4)showed the best catalytic activity,with the de-NOx activity reaching 50%at 157℃and maintaining above 99%at 225-320℃,and it exhibited good resistance against water vapor and SO_(2).The de-NOx activities follow the sequence of polyhedral CuCr_(2)O_(4)>granular CuCr_(2)O_(4)>spherical CuCr_(2)O_(4).The effects of morphology on the denitrification performance of CuCr_(2)O_(4)were analyzed by a series of characterization techniques.N_(2)sorption-desorption results showed that polyhedral CuCr_(2)O_(4)had the highest specific surface area(25.5 m^(2)/g)and the largest pore volume(0.154 cm^(3)/g);X-ray photoelectron spectroscopy(XPS)results showed that polyhedral CuCr_(2)O_(4)possessed the highest ratio of surface reactive oxygen species(49.5%)and Cu^(+)(16.2%);NH_(3)-programmed temperature desorption(NH_(3)-TPD)showed that polyhedral CuCr_(2)O_(4)had the highest surface acid concentration(0.12 mmol/g)and intensity;H_(2)-programmed temperature reduction(H_(2)-TPR)showed that polyhedral CuCr_(2)O_(4)had the most reducible and abundant surface active species(3.69 mmol/g),which facilitated the SCR reaction in the low-temperature range.The enhanced surface acidity and redox properties of polyhedral CuCr_(2)O_(4)makes it exhibit better de-NOx performance.

关 键 词：CuCr_(2)O_(4) 尖晶石 形貌 SCR 脱硝性能 催化剂 

分 类 号：X511[环境科学与工程—环境工程]