用于硝基苯选择性加氢催化的钯镍合金/氮化镍界面构筑  

Design of a palladium-nickel alloy/nickel nitride interface for selective hydrogenation of nitrobenzene catalysis

作　　者：吴静波 高亚男 段万春 杜先婷 余志鹏 徐坤 Jingbo Wu;Yanan Gao;Wanchun Duan;Xianting Du;Zhi-Peng Yu;Kun Xu(School of Chemistry and Chemical Engineering,Institutes of Physical Science and Information Technology,Key Laboratory of Functional Inorganic Material Chemistry of Anhui Province,Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials,Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education,Anhui University,Hefei 230601,China;School of Chemistry and Materials Science,University of Science and Technology of China,Hefei 230026,China)

机构地区：[1]School of Chemistry and Chemical Engineering,Institutes of Physical Science and Information Technology,Key Laboratory of Functional Inorganic Material Chemistry of Anhui Province,Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials,Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education,Anhui University,Hefei 230601,China [2]School of Chemistry and Materials Science,University of Science and Technology of China,Hefei 230026,China

出　　处：《Science China Materials》2023年第9期3565-3572,共8页中国科学（材料科学（英文版）

基　　金：financially supported by the National Natural Science Foundation of China (22005002);the Natural Science Foundation of Anhui Province (2208085Y03);Anhui University Scientific Research Start-up Fund;supported by the advanced computing resources provided by the Supercomputing Center of the University of Science and Technology of China。

摘　　要：金属负载型催化剂的界面结构设计一直是实现高效、高选择性催化反应的核心研究.本文表明,异质结结构PdNi&Ni_(3)N的界面电荷重新分布可以催化硝基苯选择性加氢成为偶氮类化合物.相比之下,独立的PdNi合金催化硝基苯转化为苯胺,而Ni_(3)N载体在相同条件下对硝基苯加氢的催化几乎没有效果. X射线光电子能谱和理论计算表明,PdNi&Ni_(3)N界面电荷重新分布导致有机反应中间体的吸附能发生变化,从而改变加氢反应途径,实现偶氮化合物的高选择性生成.本研究进一步表明了界面结构设计在有机催化加氢反应中的重要性,而且可能会引起研究者对于异质结构金属(合金)/过渡金属氮化物更多的科学兴趣,以应用于催化领域的不断发展.Designing the interface structure in metalsupported catalysts has been a central challenge in realizing the high efficiency of selective catalysis.Herein,we demonstrate that interfacial charge redistribution at the interface of heterostructured PdNi&Ni_(3)N enables selective catalytic hydrogenation of nitrobenzene into azo compounds.Contrarily,the PdNi alloy alone catalyzes the conversion of nitrobenzene into aniline,and the Ni_(3)N support was almost powerless to catalyze the hydrogenation of nitrobenzene under the same conditions.Interfacial charge redistribution at the interface of PdNi&Ni_(3)N,as evidenced by the X-ray photon spectroscopy results and theoretical calculations,results in a change in the adsorption energy of the organic reaction intermediates,thus altering the hydrogenation reaction pathway to achieve selective production of azo compounds.We believe that this study not only highlights the importance of interface structure in selective catalytic hydrogenation reactions but also inspires more scientific interest in heterostructured metal(alloy)/transition metal nitrides catering to the field of catalysis.

关 键 词：负载型催化剂 偶氮化合物 X射线光电子能谱 加氢反应 选择性加氢 过渡金属氮化物 吸附能 界面结构 

分 类 号：TQ426[化学工程]