不同酸碱性的钯基催化剂制备及其在甲基异丁基酮合成中应用无机化学专业论文.docxVIP

摘要 摘要 卜海师范大学硕士学位论文 这说明了酸性载体SBA．15．S更有利于缩合反应的进行，从而使得Pd／SBA一15一S 的催化性能更加优越。同时，Pd／SBA．15．S的丙酮转化率大大的高于SBA．15．S， 说明缩合、加氢相互协同，共同促进反应进行。对比Pd／SBA．15．S与Pd／SBA．15 的催化活性，后者的丙酮转化率极低，并且未发现MIBK的生成，其主要产物 为IPA，而前者具有较高的丙酮转化率和MIBK选择性，表明SBA．15表面的 Si—OH对缩合反应基本无活性，而磺酸基团对丙酮的缩合非常有效。Pd／SBA．1 5．S 体系催化剂的磺酸含量在10m01％时得到最佳的催化活性，酸含量过高会使过度 缩合的副产物增多，并覆盖活性位。在反应200。C时，丙酮转化率高达61．7％， MIBK选择性达85．8％，催化活性优异。将Pd／SBA一15—10％S进行活性套用，循 环反应6次后，MIBK产率仍达23．6％，经酸处理催化剂活性得到有效的恢复， 表明催化剂循环过程中活性降低主要是由于酸含量的流失。 关键词：丙酮；一步法；甲基异丁基酮；钯；氧化物；不同酸碱性；改性SBA一15 II 万方数据 Shanghai Shanghai Normal University Master of Philosophy Abs仃act Abstract Methyl isobutyl ketone(MIBK)is one of the most important chemical products， which is widely used in the field of chemical engineering．The advanced process for producing MIBK is one—step synthesis from acetone．In this process．the key technology is to develop the multi—fuctional catalyst，which has both the ability of hydrogenation and condensation，as well as suitable acid—base sites．In this study the balance of condensation and hydrogenation was explored by adjusting the acidity and alkalinity of the carrier at a fixed amount of Pd． Metal oxides have the rich pore structure，good thermal stability,large specific surface area，and suitable acidity—basicity properties，which were widely used as the cartier of this reaction．In this paper,basic MgO，acid A1203，as well as MgAI mixed oxide derived from HTLc synthesized by coprecipitation．In order to find the most suitable metal—carrier combination，these three oxides with different acidity-basicity properties impregnated Pd or／and Ni，and evaluated by batch reactor．The catalyst samples are characterized by XRD、BET、C02-TPD、H2-TPR and TEM．Some effects such as the load of mental content the structure of oxides，base strength of the derived oxides，metal dispersion，and the reducibility of catalysts are discussed．Then the catalytic acitivities of acetone liquid·phase condensation and hydrogenation over these catalysts are tested．D