Cu-Ni@S-1催化剂的制备及其脱硝性能  

Preparation and Denitration Performance of Cu-Ni@S-1 Catalyst

作　　者：白雄伟 张嘉兴 闫秘 赵玉 张莉民 王琪 李炳辉 张安峰[1] 郭新闻[1] BAI Xiongwei;ZHANG Jiaxing;YAN Mi;ZHAO Yu;ZHANG Limin;WANG Qi;LI Binghui;ZHANG Anfeng;GUO Xinwen(State Key Laboratory of Fine Chemicals,School of Chemical Engineering,Dalian University of Technology,Dalian 116024,China;Shandong Junfei Environmental Protection Technology Co.,Ltd.,Zibo 255400,China)

机构地区：[1]大连理工大学化工学院精细化工国家重点实验室,辽宁大连116024 [2]山东骏飞环保科技有限公司,山东淄博255400

出　　处：《石油学报（石油加工）》2024年第4期965-973,共9页Acta Petrolei Sinica(Petroleum Processing Section)

摘　　要：采用溶解-再晶化法将金属Cu和Ni封装到不同粒径的中空Silicalite-1(S-1)分子筛空腔内部,制备了不同金属掺杂量的中空封装型催化剂。采用X射线粉末衍射(XRD)、扫描电子显微镜(SEM)、X射线光电子能谱分析(XPS)等手段对催化剂样品进行了表征,并采用固定床反应器模拟实际工况考察催化剂对催化裂化再生烟气(n(CO)/n(NO)=13/3)中氮氧化物(NO x)的脱除性能。结果表明:在催化剂用量0.15 g、压力0.1 MPa、温度680℃、混合气体积空速60000 mL/(g·h)的条件下,3%Cu@S-1-380的脱硝效率仅为63%,而2%Cu-0.5%Ni@S-1-380的脱硝效率为100%;Ni和Cu之间形成Cu_(x) Ni_(y) O共熔体,促进了Cu^(+)与Cu^(2+)之间快速循环,提高了氧化还原反应速率;催化剂的中空空腔结构有效防止了金属的流失和烧结,极大地提高了反应物的扩散性能和催化剂的催化活性。相同反应条件下,随着分子筛粒径的减小、金属含量的增加,催化剂的脱硝率提高,双金属共同封装对催化活性的提高非常显著。Cu and Ni were encapsulated into Silicalite-1(S-1)molecular sieve with different particle sizes by dissolvation-recrystallization method,based on which the hollow encapsulated catalysts with different metal doping amounts were prepared.The catalysts were characterized by X-ray powder diffraction(XRD),scanning electron microscopy(SEM),and X-ray photoelectron spectroscopy(XPS).The fixed bed reactor was used to simulate the removal of nitrogen oxides(NO_(x))in flue gas(n(CO)/n(NO)=13/3)from fluid catalytic cracking regeneration process under operating conditions.The results show that under the conditions of catalyst dosage 0.15 g,pressure 0.1 MPa,temperature 680℃and space velocity 60000 mL/(g·h),the denitration efficiency of 3%Cu@S-1-380 is only 63%,and that of 2%Cu-0.5%Ni@S-1-380 is 100%.The formation of Cu_(x) Ni_(y) O eutectic between Ni and Cu promotes the rapid cycling between Cu^(+)and Cu^(2+),and increases the redox reaction rate.The hollow cavity structure of catalyst effectively prevents metal loss and sintering,greatly improving the diffusion performance of reactants and the catalytic activity of catalyst.Under the same reaction conditions,as the particle size of molecular sieve decreases and the metal content increases,the denitrification efficiency of catalyst increases.The bimetallic co-encapsulation can significantly improve the catalytic activity.

关 键 词：中空沸石 脱硝助剂 流化催化裂化(FCC) 双金属催化剂 再生烟气 氮氧化物(NO_(x)) 

分 类 号：TQ241.1[化学工程—有机化工]