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作 者:周蒙[1] 邓莹[1] 袁霞[1] 吴剑[1] 罗和安[1]
出 处:《化学反应工程与工艺》2014年第2期182-187,共6页Chemical Reaction Engineering and Technology
基 金:国家自然科学基金(21006080);湖南省自然科学基金(14JJ2065);湖南省高校创新平台开放基金(13K044)
摘 要:为了开发甲苯液相氧化的新催化体系,寻求合适的反应条件提高甲苯选择性氧化生成苯甲醛、苯甲醇的选择性。以分子氧为氧源,在无溶剂条件下,采用N-羟基邻苯二甲酰亚胺(NHPI)与双水杨醛缩乙二胺合钴配合物(Co(Salen))复合催化甲苯液相氧化反应。详细考察了NHPI单独催化以及NHPI与Co(Salen)复合催化过程中NHPI用量、Co(Salen)用量、反应温度、反应时间和氧压对甲苯选择性氧化反应的影响。结果表明:在甲苯0.22 mol,NHPI的摩尔分数2%,Co(Salen)的摩尔分数0.02%,氧压1.60 MPa,110℃的条件下反应2 h,甲苯转化率达到13.6%,苯甲醛选择性32.7%,苯甲醇选择性10.8%,苯甲醛、醇、酸总选择性达97.7%,该反应条件为较佳的工艺条件。For development of a new catalysis system for liquid phase oxidation of toluene to improve the selectivity of intermediate products benzaldehyde and benzyl alcohol at appropriate reaction conditions, N-hydroxylphthalimide (NHPI) and N,N′-bis(salicylidene) ethylenediiminocobalt (Co(Salen)) composite were adopted to catalyze the liquid-phase oxidation of toluene with oxygen molecular without any solvent. The effects of the amount of NHPI catalyst and NHPI/Co(Salen) composite catalyst, reaction temperature, reaction time and O2 pressure on the selectivity oxidation of toluene were investigated carefully. The results showed that the conversion of toluene was 13.6%, the selectivity of benzaldehyde and benzyl alcohol were 32.7%and 10.8%respectively, the total selectivity to benzaldehyde, benzyl alcohol and benzoic acid was up to 97.7%, under the optimum conditions of toluene 0.22 mol, NHPI molar fraction 2%, Co(Salen) molar fraction 0.02%, oxygen pressure 1.60 MPa and temperature of 110 ℃ for 2 h.
关 键 词:甲苯液相氧化 苯甲醛 N-羟基邻苯二甲酰亚胺 双水杨醛缩乙二胺合钴配合物
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