Au催化劑論文：負載型Au催化劑的制備及其在肉桂醛選擇性加氫反應中的應用研究

1、Au催化劑論文：負載型Au催化劑的制備及其在肉桂醛選擇性加氫反應中的應用研究【中文摘要】負載型納米Au催化劑在許多化合物的【英文摘要】Supported gold catalysts are a kind of promising catalysts for selective hydrogenation based on their good activity and selectivity for the reduction of many compounds.In this paper, using several metal oxides doped TiO2 as supports,

2、 which were prepared by the sol-gel method, a series of gold catalysts were prepared by the deposition-precipitation （DP） method. Additionally, a series of Au/La（OH）3 catalysts were prepared by cocipitation （CP） method. All the catalyst were tested in cinnamaldehyde hydrogenation. Their phisico-chem

3、ical properties were investigated by XRD, TEM, XPS, BET and TPR techniques. The reaction conditions of cinnamaldehyde selective hydrogenation were optimized.The results show that the performance of Au/TiO2 catalyst is influenced by the type and the content of additives. Among the metal oxide promote

4、rs tested, La2O3 modified Au/TiO2 shows the best selectivity for the reduction of carbon-carbon double bond in cinnamaldehyde. The moderate amount of La2O3（10 wt%） can obviously improve the catalytic activity and selectivity of Au/TiO2 for cinnamaldehyde hydrogenation. The presence of La2O3 in TiO2

5、restrains the growth of TiO2 crystallites, increases the surface area of catalysts and makes the particle size distribution of Au crystallites more evenly. The gold on the surface of Au/TiO2 exists mainly as Au0, but on the La2O3 doped catalyst there is a small portion of Au3+ species besides Au0, w

6、hich may benefit the activation of the C=O bond of cinnamaldehyde.The results show that La（OH）3 supported gold catalyst shows high selectivity for the reduction of carbon-carbon double bond. With the characterization results, the reason of the high selectivity is that the supporter La（OH）3 and Au in

7、teract to form a unique structure. The preparation conditions of Au/La（OH）3 catalyst are optimized as follows: 2 wt% of gold content, calcination temperature 100°C and reduction temperature 150°C.The reaction conditions of cinnamaldehyde selective hydrogenation over Au/La（OH）3 catalyst are

8、 optimized as follows: reaction temperature 180°C, reaction pressure 2.0 MPa, catalyst dosage 0.25 g, solvent isopropanol. Under the optimal conditions, the conversion of cinnamaldehyde and the selectivity to cinnamyl alcohol can reach 100% and 75.7%, respectively, after reaction 22 h.【關鍵詞】Au催化

9、劑 助劑 La（OH）3 選擇性加氫 肉桂醛 肉桂醇【英文關鍵詞】gold catalyst promoter La（OH）3 selective hydrogenation cinnamaldethyde cinnamyl alcohol【目錄】負載型Au催化劑的制備及其在肉桂醛選擇性加氫反應中的應用研究摘要4-6ABSTRACT6-7第一章 文獻綜述11-301.1 肉桂醛催化加氫合成肉桂醇的研究進展11-201.1.1 肉桂醇的用途111.1.2 肉桂醇的合成方法11-131.1.3 非貴金屬催化劑在肉桂醛選擇性加氫中的應用進展13-161.1.4 貴金屬催化劑在肉桂醛選擇性加氫中的應用

10、進展16-201.2 納米Au 催化劑的研究進展20-281.2.1 負載型Au 催化劑的制備20-221.2.2 負載型納米Au 催化劑性能的影響因素22-251.2.3 Au 催化劑在液相加氫中的應用25-281.3 立題依據及主要研究內容28-301.3.1 論文立題依據和意義28-291.3.2 論文主要研究內容29-30第二章 實驗部分30-362.1 試劑與主要儀器30-312.1.1 主要試劑30-312.1.2 主要儀器及設備312.2 實驗方案與步驟31-322.2.1 實驗方案312.2.2 實驗步驟31-322.3 催化劑的制備32-332.3.1 Au/M_xO_yTi

11、0_2 催化劑的制備32-332.3.2 Au/La(OH_3 催化劑的制備332.4 催化劑的活性評價33-342.4.1 實驗方法332.4.2 產物分析33-342.5 催化劑的表征34-362.5.1 X 射線衍射(XRD342.5.2 比表面和孔結構的測定(BET342.5.3 元素分析(STEM-EDX342.5.4 高分辨透射電鏡(HRTEM34-352.5.5 X 射線光電子能譜儀(XPS352.5.6 程序升溫還原(H_2-TPR35-36第三章 助劑對Au/Ti0_2催化劑加氫性能的影響研究36-533.1 前言363.2 助劑對Au/Ti0_2 催化性能的影響36-393

12、.2.1 助劑種類的影響36-373.2.2 助劑添加方式的影響37-383.2.3 助劑添加量的影響38-393.3 助劑La_20_3 對Au/Ti0_2 催化性能的影響39-513.3.1 助劑La_20_3 添加量對Au/Ti0_2 性能的影響39-483.3.2 焙燒溫度對Au/10%La_20_3-Ti0_2 催化劑加氫性能的影響48-493.3.3 還原溫度對Au/10%La_20_3-Ti0_2 催化劑加氫性能的影響49-503.3.4 還原時間對Au/10%La_20_3-Ti0_2 催化劑加氫性能的影響50-513.4 本章小結51-53第四章 納米Au/La(OH_3催化劑加氫性能的研究53-684.1 前言534.2 載體種類對Au 催化劑性能的影響53-564.2.1 載體種類對Au 催化劑加氫性能的影響53-544.2.2 不同載體負載的Au 催化劑的表征54-564.3 Au/La(OH_3 催化劑上肉桂醛選擇性加氫反應研究56-674.3.1 Au 負載量對Au/La(OH_3 催化劑加氫性能的影響56-574.3.2 焙燒溫度對Au/La(OH_3 催化劑加氫性能的影響57-634.3.3 還原溫度對A