2004-08-012024-05-17https://scholars.lib.ntu.edu.tw/handle/123456789/670663摘要：本計畫擬研究氮化硼(boron nitride, BN)載體在氫化反應具有的特殊選擇性氫化的效果，先前研究BN載體支撐的金屬，顯示具有較高的電子密度。對不飽和醛類的兩種官能基C=C、C=O，在進行氫化反應時，將會有選擇性氫化反應，其中後者(C=O)產生不飽和醇類，在特用化學工業上具有較高的經濟價值。第一年(93年度)在巴豆醛選擇性氫化研究，顯示負載於BN上的雙金屬PtSn對巴豆醇有很高的選擇率，發現PtSn的合金態有重大的影響力，表面Sn2+氧化態扮演親電子(即路易士酸)位置，使C=O得以吸附並活化，優先的氫化成巴豆醇。第二年(94年度)本計畫將探討高正電性的鐵或鈷扮演電子予體(electron donor)，來增加Pt上之電荷密度，因而降低對C=C的束縛能(binding energy)而使C=O優先被氫化。將以初濕含浸法(incipient wetness)製備一系列雙金屬Pt-Fe/BN及Pt-Co/BN觸媒，並與Al2O3、活性碳等載體做一比較。續用巴豆醛為選擇性氫化指標，進行氣相氫化反應，探討氫化反應之操作條件。實驗分析著重於C=C及C=O的氫化產物選擇率，作為BN與傳統載體<br> Abstract: This research proposes to study the specially selective hydrogenation using BN (boron nitride) supported bi-metal catalyst. BN-supported Pt showed near metal state and the electron density was high due to the BN support effect from previous study. The functional groups, C=C and C=O, of an un-saturated aldehyde can be selectively hydrogenated depending on the status of Pt site. The C=O hydrogenation is favorable when a metal cluster has high electron density. An un-saturated alcohol from C=O hydrogenation has high-market value for the special chemicals in industry. The results of the first year (2004) indicated that very high selectivity of crotyl alcohol was found due to the PtSn alloy on BN support. The status of PtSn alloy played an important role The surface Sn2+ served as Lewis acid site so that C=O was activated and preferentially hydrogenated to crotyl alcohol. The project of 2nd year (2005) will study the increase of Pt electron density induced by electron donor, such as Fe and Co. Thus, the binding energy of C=C with Pt can be reduced resulting in the preferential C=O hydrogenation. A series of Pt-Fe/BN and Pt-Co/BN catalysts will be prepared using incipient wetness method. For comparison purpose, Al2O3 and active carbon supported bi-metal catalysts will also be prepared. The hydrogenation of crotonaldehyde is still chosen to be a selective-hydrogenation index. The hydrogenation will be carried out in gas phase, and the various reaction conditions will be investigated. The product selectivities of C=C and C=O hydrogenation will be analyzed in order to compare the difference between BN and the traditional supports. Finally a reaction mechanism will be established, and foster to develop a novel hydrogenation catalyst.選擇性氫化氮化硼雙金屬觸媒巴豆醛鉑鐵鈷Selective hydrogenationBoron nitrideBi-metal catalystCrotonaldehydePtFeCo