通过二维沸石调节铂的氢化选择性  

Regulating the hydrogenation selectivity of platinum using a twodimensional zeolite

作　　者：翟玉慧 马悦 崔凤超 田宇阳 朱广山 Yuhui Zhai;Yue Ma;Fengchao Cui;Yuyang Tian;Guangshan Zhu(Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education,Faculty of Chemistry,Northeast Normal University,Changchun 130024,China)

机构地区：[1]Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education,Faculty of Chemistry,Northeast Normal University,Changchun 130024,China

出　　处：《Science China Materials》2024年第7期2135-2141,共7页中国科学（材料科学）（英文版）

基　　金：supported by the National Natural Science Foundation of China(22075040,22131004 and U21A20330)and the“111”Project(B18012).

摘　　要：不饱和醇是一类重要的医药中间体,然而C=C加氢比C=O加氢反应更具有热力学优势,因此由不饱和醛合成不饱和醇具有挑战性.为解决这一问题,需要寻求一种具有可调控选择性的氢化催化剂.二维沸石的高长径比和大量的末端基团作为锚定位点,使其不仅能作为催化剂载体,还可以有效地调节催化剂性能.本研究利用二维沸石IPC-1P作为铂纳米颗粒的载体,成功制备出异相催化剂Pt@IPC-1P.铂纳米颗粒的尺寸小于2 nm且均匀地分布在IPC-1P上.令人惊喜的是,Pt@IPC-1P催化剂对不饱和醇的选择性超过了90%,并实现了接近100%的催化转化率,远超其他铂基催化剂.理论计算证实,二维沸石IPC-1P在肉桂醛向肉桂醇的转化过程中起到了积极作用,其放热效应能量高于苯丙醛.这项工作展现了二维沸石在催化有机物转化领域具有广阔的应用前景.Unsaturated alcohols are important pharmaceutical intermediates;however,their synthesis from unsaturated aldehydes is challenging because the C=C hydrogenation is more thermodynamically preferential than the transformation of C=O.Suitable catalysts with regulated catalytic selectivity to hydrogenation are required.Two-dimensional(2D)zeolites possess high aspect ratios and many terminal bonds as anchoring sites,rendering them not only candidates as catalyst supports but also promising for adjusting the performance of the catalysts.In this study,we exploited a 2D zeolite,IPC-1P,as the support for Pt nanoparticles(NPs)to produce a heterogeneous catalyst,[e-mail] Pt NPs were uniformly distributed on the IPC-1P with a size of less than 2 nm.Unexpectedly,Pt@IPC-1P exhibited over 90%selectivity to unsaturated alcohols and nearly 100%catalytic conversion,exceeding the catalytic performance of other Pt-based catalysts.Theoretical calculations showed that the 2D zeolite facilitated the formation of the cinnamyl alcohol from cinnamaldehyde,as evidenced by the more energetically preferential exothermic effect than that of phenylpropylaldehyde.The 2D zeolite has an unfolded prospect for catalytic usages in organic transformation.

关 键 词：heterogeneous catalysis 2D zeolite hydrogenation selectivity CINNAMALDEHYDE top-down approach 

分 类 号：TQ426[化学工程]