氮掺杂Pd-Cu/Al_(2)O_(3)催化剂富氢气氛下CO优先氧化性能  

Nitrogen doped Pd-Cu/Al_(2)O_(3)for CO preferential oxidation performance in H_(2)-rich stream

作　　者：岳丽君 马浩程 赵婉君 李晋芳 张成明 Yue Lijun;Ma Haocheng;Zhao Wanjun;Li Jinfang;Zhang Chengming(Engineering Research Center of Ministry of Education for Fine Chemicals,School of Chemistry and Chemical Engineering,Shanxi University,Taiyuan 030006,Shanxi,China;Taiyuan Xiaodian District No.1 Middle School,Taiyuan 030032,Shanxi,China)

机构地区：[1]山西大学化学化工学院,精细化学品教育部工程研究中心,山西太原030006 [2]太原市小店区第一中学,山西太原030032

出　　处：《工业催化》2023年第10期48-54,共7页Industrial Catalysis

基　　金：山西省自然科学基金(201801D121043)。

摘　　要：以Al_(2)O_(3)为载体,采用共浸渍法制备Pd-Cu/Al_(2)O_(3)和Pd-Cu-N/Al_(2)O_(3)催化剂。利用连续流动微反应装置考察氮掺杂对Pd-Cu/Al_(2)O_(3)催化剂低温富氢气氛下CO优先氧化性能的影响,结合XRD、FT-IR、H_(2)-TPR和XPS等手段对催化剂进行表征。结果表明,相较于Pd-Cu/Al_(2)O_(3),Pd-Cu-N/Al_(2)O_(3)具有更好的CO优先氧化性能。氮掺杂促进了表面Cu_(2)Cl(OH)_(3)的分散,增强了Pd和Cu之间的相互作用,提高了Pd和Cu_(2)Cl(OH)_(3)的氧化还原能力。同时,氮掺杂也有利于生成更多的表面活性Cu+物种,并且部分进入Pd晶格,抑制了反应过程中PdHx的形成,从而使催化剂催化性能提高。Pd-Cu/Al_(2)O_(3)and Pd-Cu-N/Al_(2)O_(3)catalysts were prepared by co-impregnation method with Al_(2)O_(3)as supports.The effect of nitrogen doping on the catalytic performance of Pd-Cu/Al_(2)O_(3)catalyst for CO preferential oxidation in H_(2)-rich stream was studied by using a fixed-bed continuous flow reactor.The catalysts were characterized by XRD,FT-IR,H_(2)-TPR and XPS.Compared with Pd-Cu/Al_(2)O_(3),Pd-Cu-N/Al_(2)O_(3)has better CO preferential oxidation performance.The results show that nitrogen doping promotes the dispersion of Cu_(2)Cl(OH)_(3)on the surface,enhances the interaction between Pd and Cu,and improves the redox ability of Pd and Cu_(2)Cl(OH)_(3).At the same time,the addition of nitrogen is also conducive to the formation of more active Cu+on the surface,and the interstitial nitrogen entering the lattice of Pd may inhibit the formation of PdHx in the reaction process,thus improving the catalytic activity of the Pd-Cu/Al_(2)O_(3).

关 键 词：催化化学 Wacker型催化剂 Pd-Cu/Al_(2)O_(3) CO优先氧化 氮掺杂 

分 类 号：TQ426.99[化学工程] O643.36[理学—物理化学]