中文摘要
本申请针对含低价硫芳硝基化合物催化加氢时易使金属催化剂中毒而无法采用绿色催化还原的问题，基于MPV还原既可酸催化，也可碱催化，合适的酸碱性匹配使催化剂更具有高催化活性，碱中心催化或弱酸中心催化可避免催化剂硫中毒的认识；拟以具有酸、碱性特征的类水滑石为前体制备的多孔复合金属氧化物为催化化体系，根据软硬酸碱相互作用的规律，设计并合成适宜碱性及酸性活性中心匹配的催化体系，获得新的、耐硫、高活性含低价硫芳硝基化合物催化氢转移还原催化体系，用于含低价硫芳硝基化合物的催化氢转移还原。深入研究含低价硫及其他基团芳硝基化合物的结构与催化剂酸碱性对它们之间相互作用影响的规律，为发展含低价硫芳硝基化合物以类水滑石为前体的多孔复合金属氧化物催化清洁还原提供理论依据。
英文摘要
The metal catalysts will get poisoned by the low-valence sulfur, which coexists in aromatic nitro compounds, so that the catalytic reduction using hydrogen in the presence of metal catalysts, such as palladium, platinum, or nickel, cannot be applied to almost all cases of using alkylthio-containing aromatic nitro compounds as substrates. In view of this situation, catalytic transfer hydrogenation was introduced and porous mixed metal oxides prepared from hydrotalcite-like materials were selected as catalyst system. This idea was based on that the Meerwein-Ponndorf-Verley(MPV) reduction could be carried out by either acid catalysis or basic catalysis, the high activity of these catalysts probably comes from the synergetic effect of appropriate basic and acidic sites, and basic catalysis or mildly acidic catalysis can avoid the catalysis getting poisoned. We plan to design and synthesize the appropriate basic and acidic porous mixed metal oxides from hydrotalcite-like materials according to the Principle of Hard and Soft Acids and Bases to obtain the catalysts, which have high activity and are able to resist being poisined, for the catalytic transfer hydrogenation of alkylthio-containing aromatic nitro compound. Furthermore, the effects of the structure of alkylthio-containing aromatic nitro compounds and the acidity and basicity of catalysts on the interactions of them will be studied thorughly.
结题摘要
本申请针对含低价硫芳硝基化合物催化加氢时易使金属催化剂中毒而无法采用绿色催化还原的问题，基于MPV还原既可酸催化，也可碱催化，合适的酸碱性匹配使催化剂更具有高催化活性，碱中心催化或弱酸中心催化可避免催化剂硫中毒的认识；拟以具有酸、碱性特征的类水滑石为前体制备的多孔复合金属氧化物为催化化体系，根据软硬酸碱相互作用的规律，设计并合成适宜碱性及酸性活性中心匹配的催化体系，获得新的、耐硫、高活性含低价硫芳硝基化合物催化氢转移还原催化体系，用于含低价硫芳硝基化合物的催化氢转移还原。深入研究含低价硫及其他基团芳硝基化合物的结构与催化剂酸碱性对它们之间相互作用影响的规律，为发展含低价硫芳硝基化合物以类水滑石为前体的多孔复合金属氧化物催化清洁还原提供理论依据。