一步水热合成Cu⁃SAPO⁃34选择性催化丙烯还原氮氧化物  

Selective Catalytic Reduction of Nitric Oxide with Propylene over One⁃Step Synthesized Cu⁃SAPO⁃34 Catalysts

作　　者：周皞[1] 杨迪 王聪颖 赵辉爽[1] 伍士国[1] 苏亚欣[2] ZHOU Hao;YANG Di;WANG Cong-Ying;ZHAO Hui-Shuang;WU Shi-Guo;SU Ya-Xin(Changzhou Institute of Engineering Technology,Changzhou,Jiangsu 213164,China;School of Environmental Science and Engineering,Donghua University,Shanghai 201620,China)

机构地区：[1]常州工程职业技术学院,常州213164 [2]东华大学环境科学与工程学院,上海201620

出　　处：《无机化学学报》2020年第10期1997-2004,共8页Chinese Journal of Inorganic Chemistry

基　　金：江苏省自然科学基金(No.BK20181161);国家自然科学基金(No.51278095);江苏省高校“青蓝工程”项目(2017);江苏省“333工程”科研项目(2018)资助。

摘　　要：采用一步法水热合成不同Cu/Al比的Cu-SAPO-34催化剂,并对其丙烯选择性催化还原NO(C3H6-SCR)性能进行了研究。通过N2吸附-脱附、X射线衍射(XRD)、X射线光电子能谱(XPS)、程序升温还原(H2-TPR)和原位漫反射傅里叶变换红外光谱(In situ DRIFTS)等研究手段对催化剂进行表征,考察Cu-SAPO-34中Cu物种含量对催化剂的物理化学性质和反应活性的影响。结果表明,当铜负载量为2.76%~4.12%(w/w)时,Cu-SAPO-34催化剂在富氧条件下300~400℃内表现出非常有吸引力的C3H6-SCR活性,可实现~100%的脱硝效率和~100%的N2选择性。原位红外光谱研究表明,Cu-SAPO-34分子筛骨架上孤立的Cu^2+离子是NO吸附和活化形成NO2-/NO3-中间物种的主要活性位,并通过C3H6-SCR反应过程中Cu^2+/Cu^+氧化还原循环来实现Cu^2+离子的持续供给。To investigate the performance of Cu-chabazite for selective catalytic reduction of NO with propylene(C3H6-SCR),a series of Cu-SAPO-34 catalysts with varied Cu/Al ratio have been synthesized by the one-pot hydrothermal method.These catalysts were characterized using N2 adsorption-desorption,X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),temperature programmed reduction by H2(H2-TPR),and in⁃situ diffuse reflectance infrared Fourier transform spectroscopy(in⁃situ DRIFTS)techniques.The effect of Cu component on physicochemical properties and C3H6-SCR activity were investigated.Cu-SAPO-34 catalysts with Cu loading(22.76%~4.12%(w/w))exhibited attractive activities,with nearly 100%NOx conversion and 100%N2 selectivity at the temperatures(300~400℃)in the excess of oxygen.Based on in situ DRIFT studies,the formation of NO2-/NO3-intermediates requires the presence of isolated Cu^2+ions in Cu-SAPO-34,which undergo a periodic Cu^2+/Cu^+redox cycle during C3H6-SCR.

关 键 词：Cu-SAPO-34 选择性催化还原 NO 丙烯 Cu^2+离子 

分 类 号：X511[环境科学与工程—环境工程]