插层水滑石构筑镍基纳米催化剂及其在二苯乙炔选择性加氢反应中的性能  

Intercalated structured nickel-based hydrotalcite nanocatalyst for diphenylacetylene semihydrogenation

作　　者：孙豪飞 秦静茹 兰兴旺 温昕[1] 白国义[1] Hao-Fei Sun;Jing-Ru Qin;Xing-Wang Lan;Xin Wen;Guo-Yi Bai(College of Chemistry and Environmental Science,Hebei University,Baoding 071002,China)

机构地区：[1]河北大学化学与环境科学学院,保定071002

出　　处：《中国科学：化学》2021年第9期1303-1310,共8页SCIENTIA SINICA Chimica

基　　金：国家自然科学基金(编号:22078080,21676068,21706049)资助项目。

摘　　要：本文利用吡啶-2,3-二羧酸与镍离子形成的配合物(Ni-PDA)插入镁铝水滑石层间,制备新型Ni/Mg3Al1O-PDA镍基纳米催化剂.与传统浸渍法、共沉淀法所制备的镍基纳米催化剂相比,该催化剂在1,2-二苯乙炔选择性加氢反应中表现出更高的活性与稳定性.通过X射线粉末衍射、红外光谱、透射电子显微镜和X射线光电子能谱等表征手段发现,Ni-PDA的插层作用有效地促进了镍前驱体均匀分散在水滑石层板间,并将水滑石层间距从0.76 nm增加到1.55 nm.这一过程不仅有利于镍纳米粒子在层板间的高度分散,还提高了催化剂的比表面积和孔体积,从而暴露更多的镍活性位点.此外,催化剂前驱体中MgNiO_(2)尖晶石结构明显促进了活性组分与载体的相互作用,进一步提升了镍纳米粒子的分散程度,从而提高了催化剂活性和稳定性.A novel nickel-based hydrotalcite catalyst Ni/Mg3Al1O-PDA was fabricated by intercalating the complex formed by pyridine-2,3-dicarboxylic acid(PDA)and nickel ions into the layers of Mg-Al hydrotalcite.Compared with nickel-based nanocatalysts prepared by traditional impregnation method and co-precipitation method,this catalyst showed superior catalytic performance in the semi-hydrogenation of 1,2-diphenylacetylene.Results of X-ray powder diffraction,infrared spectrum,transmission electron microscopy and X-ray photoelectron spectroscopy showed that the intercalation effect of Ni-PDA effectively promoted the uniform dispersion of Ni precursors between hydrotalcite laminates,and increased the intercalation distance of hydrotalcite laminates from 0.76 to 1.55 nm.This process not only facilitated the high dispersion of Ni nanoparticles,but also increased the specific surface area and pore volume of the catalyst,thus exposing more Ni active sites.Moreover,the formation of MgNiO_(2)spinel structure in the catalyst precursors significantly improved the interaction between the active species and the support,promoted the dispersion of Ni nanoparticles,and improved the activity and stability of the obtained catalyst.

关 键 词：镍基纳米催化剂 二苯乙炔选择性加氢 水滑石 插层作用 

分 类 号：O643.36[理学—物理化学] TB383.1[理学—化学]