化学反应工程与工艺
化學反應工程與工藝
화학반응공정여공예
CHEMICAL REACTION ENGINEERING AND TECHNOLOGY
2014年
2期
182-187
,共6页
周蒙%邓莹%袁霞%吴剑%罗和安
週矇%鄧瑩%袁霞%吳劍%囉和安
주몽%산형%원하%오검%라화안
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
甲苯液相氧化%苯甲醛%N-羥基鄰苯二甲酰亞胺%雙水楊醛縮乙二胺閤鈷配閤物
갑분액상양화%분갑철%N-간기린분이갑선아알%쌍수양철축을이알합고배합물
liquid-phase oxidation of toluene%benzaldehyde%N-hydroxyphthalimide%N,N′-bis(salicylidene) ethylenediiminocobalt
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。
為瞭開髮甲苯液相氧化的新催化體繫,尋求閤適的反應條件提高甲苯選擇性氧化生成苯甲醛、苯甲醇的選擇性。以分子氧為氧源,在無溶劑條件下,採用N-羥基鄰苯二甲酰亞胺(NHPI)與雙水楊醛縮乙二胺閤鈷配閤物(Co(Salen))複閤催化甲苯液相氧化反應。詳細攷察瞭NHPI單獨催化以及NHPI與Co(Salen)複閤催化過程中NHPI用量、Co(Salen)用量、反應溫度、反應時間和氧壓對甲苯選擇性氧化反應的影響。結果錶明:在甲苯0.22 mol,NHPI的摩爾分數2%,Co(Salen)的摩爾分數0.02%,氧壓1.60 MPa,110℃的條件下反應2 h,甲苯轉化率達到13.6%,苯甲醛選擇性32.7%,苯甲醇選擇性10.8%,苯甲醛、醇、痠總選擇性達97.7%,該反應條件為較佳的工藝條件。
위료개발갑분액상양화적신최화체계,심구합괄적반응조건제고갑분선택성양화생성분갑철、분갑순적선택성。이분자양위양원,재무용제조건하,채용N-간기린분이갑선아알(NHPI)여쌍수양철축을이알합고배합물(Co(Salen))복합최화갑분액상양화반응。상세고찰료NHPI단독최화이급NHPI여Co(Salen)복합최화과정중NHPI용량、Co(Salen)용량、반응온도、반응시간화양압대갑분선택성양화반응적영향。결과표명:재갑분0.22 mol,NHPI적마이분수2%,Co(Salen)적마이분수0.02%,양압1.60 MPa,110℃적조건하반응2 h,갑분전화솔체도13.6%,분갑철선택성32.7%,분갑순선택성10.8%,분갑철、순、산총선택성체97.7%,해반응조건위교가적공예조건。
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.