γ-丁內酯氫化觸媒之研究

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题名:	γ-丁內酯氫化觸媒之研究
其它题名:	Catalyst study for γ-butyrolactone hydrogenation
作者:	黃世昕 HUANG,SHI-XIN
贡献者:	李國禎 LI,KUO-TSENG 化學工程與材料工程學系
关键词:	氫化反應;γ-丁內酯 hydrogenation;γ-butyrolactone
日期:	2019
上传时间:	2019-12-16T02:19:48Z (UTC)
摘要:	1,4-丁二醇(BDO)是一種重要的化工原料，可用於生產四氫呋喃(THF)及聚對苯二甲酸二丁酯(PBT)等，其下游產品廣泛應用於工程塑膠、有機溶劑、農藥、增塑劑、皮革、纖維等民生用品。本論文使用圓柱型銅鋅觸媒(Cu/ZnO/Al2O3)在固定床反應器中催化γ-丁內酯(GBL)之氫化反應以同時生成1,4-丁二醇(BDO)、四氫呋喃(THF)及正丁醇，藉由改變進料流量、反應溫度、反應壓力、觸媒顆粒尺寸(包括原倍數、1/2、1/4)及Pd之添加，尋求出最適當的1,4-丁二醇(BDO)生產條件。在相同之實驗條件下，GBL之轉化率與BDO產率會隨著觸媒顆粒之減小而明顯的提升，顯示此反應有很強的internal diffusion resistance。隨溫度降低及壓力上升，GBL轉化率會增加。在原倍數觸媒中添加Pd，會明顯提升GBL轉化率且有很高之BDO選擇率，但在1/4觸媒(未添加Pd之情況)之轉化率已很接近平衡轉化率，所以可減少觸媒尺寸來取代Pd之添加。使用1/4倍數的Cu/ZnO/Al2O3觸媒催化γ-丁內酯之氫化反應，有很高的BDO選擇率(>90%)。在180℃及1000psi下，得到最高之BDO產率為87.32%。以1/4觸媒進行動力學分析，結果顯示γ-丁內酯在Cu/ZnO/Al2O3觸媒上之氫化反應可以視為一級反應，其活化能為29.5 kJ/mol。 1,4-Butanediol (BDO) is an industrially important chemical. It can be used to produce tetrahydrofuran (THF), polybutylene terephthalate (PBT). This thesis used a Cu/ZnO/Al2O3 catalyst with cylindrical shape to catalyse γ-butyrolactone hydrogenation in a packed bed reactor for producing BDO, tetrahydrofuran (THF) and n-butanol. We changed feed flow rate, reaction temperature, reaction pressure, catalyst particle size, and Pd addition, in order to find the optimum conditions for producing 1,4- butanediol (BDO) were found. GBL conversion and BDO yield increased significantly with the decrease of catalyst particle size, indicating that the reaction affected strongly by internal diffusion resistance. GBL conversion increased with decreasing temperature and with increasing pressure. The addition of Pd to the catalyst with the orginal size increased GBL conversion significantly. The conversion of the catalyst with 1/4 size (without Pd addition) was very close to the equilibrium conversion, therefore, catalyst particle size reduction can be used instead of Pd addition. Maximum BDO yield of 87.32% was obtained at 180℃ and 1000psig. The catalyst with 1/4 size had high BDO selectivity (>90%). Reaction kinetics analysis of the catalyst with 1/4 size indicated that the γ-butyrolactone hydrogenation on Cu/ZnO/Al2O3 catalyst can be regarded as a first-order reaction with an activation energy of 29.5 kJ/mol. The catalyst was examined with FE-SEM, EDS, BET, XRD and ICP-AES.
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