keggin型杂多化合物合成及其催化氧化苯的研究.pdf

硕士学位论文摘要杂多化合物是一种兼有酸性和氧化还原性的双功能性催化剂。与传统催化剂相比,它具有确定的内部结构、独特的假液相反应场、在极性溶液中良好的溶解性等优点。在有机催化反应中,杂多化合物显示出较高催化活性和选择性。由于其在反应中对设备的腐蚀性低、反应条件温和,因此,近年来受到广泛关注。。在此基础上以(C4H9)4N+为阳离子,合成磷钼钒杂多化合物。利用FT-IR、、 ,分析结果表明该类杂多化合物具有Keggin型结构。为研究探索所制备的杂多化合物的催化活性,考察了该类催化剂在苯羟化制苯酚和苯氨化制苯胺反应中的催化活性。一、催化苯羟化制苯酚在苯氧化羟化制苯酚反应中,选用30%H202为氧化剂,在乙酸作溶剂的条件下,考察了反应温度、反应时间、氧化剂用量、催化剂用量等因素对反应的影响。最佳条件反应下,%、%。二、催化苯氨化制苯胺以苯为原料,盐酸羟胺为氨源,10%次氯酸钠为氧化剂,在乙酸作溶剂的条件下, 考察反应温度、反应时间、氧化剂用量、催化剂用量等因素对反应的影响。%。实验结果表明,钒取代的磷钼钒杂多季铵盐显示出优秀的催化氧化能力。在杂多化合物中,引入钒元素可以提高催化剂的氧化性,钒引入量越多,催化剂的氧化能力越强,但同时会降低催化剂的选择性。以有机阳离子为抗衡离子可以改变杂多化合物在有机溶剂中的溶解性,同时提高催化剂的催化氧化活性。关键词:杂多化合物;Keggin结构;苯酚;苯胺 Abstract pounds have great utilitiesincatalysis because oftheiracidity and oxidation’reduction pared with the traditional has the determination internal structure,a unique phase,in polar solution,such as the advantages of good anic catalytic reaction,the pounds show high catalytic activity and itis 10w inthe response toequipment’S corrosiveness,the response condition 。 itreceived thewidespread attention in recent years. In our work,three vanadium substituted heteropoly acid have been synthesized by acidification— on thiswork,we take(C4H9)4N-t-as thepositive ion' and synthesized phosphorus molybdenum vanadium internal structure was analyzed by FT-IR,XRD,” analysis resuIt indicated thatthiskind pound has structure. Inorder tostudy pound catalytic activity which we prepare,We inspected thiskind ofcatalyst inthebenzene tophenol and benzene toaniline reaction. hydroxylation ofbenzene tophenol Inthebenzene hydroxylation ofphenol reaction,we choice of30%H202 as oxidant in acetic acid as solvent,inspected theeffects ofreaction temperature,reaction time, oxidant dosage,the amount ofcatalyst on theoptimum condition, thephenol y