醋酸溶液中Pd(OAc)_2-对苯醌-CO催化甲烷选择氧化制甲醇

Selective oxidation of methane to methanol in acetic acid solvent with Pd(OAc)_2-p-benzoquinone-CO catalyst system

考察了Pd(OAc)2-对苯醌-CO催化剂体系中甲烷有氧选择氧化制甲醇反应的性能。结果表明,在Pd(OAc)2用量为100μmol时,该催化剂体系中对苯醌和CO的最佳用量分别是1 000μmol和0.4 MPa。在讨论反应温度、反应时间及反应溶剂对甲烷选择氧化影响的基础上,得出在原料气组成为2.5 MPa甲烷+0.4 MPa氧气+0.4 MPa氮气及最佳催化剂用量的条件下,该催化剂体系选择性催化氧化甲烷的适宜工艺条件为反应温度130℃、反应时间3 h、溶剂中CH3COOH与H2O的体积比为4∶1。在此工艺条件下,目标产物甲醇的生成量为1 650μmol。

Selective aerobic oxidation of methane to methanol was carried out in an acetic acid solvent with Pd（OAc）2-p-benzoquinone-CO catalyst system;the effects of reaction temperature,time and solvent on the methane oxidation were investigated.The results showed that when the amount of Pd（OAc）2 is 100 μmol,the optimum amounts of p-benzoquinone and CO in the catalyst system are 1 000 μmol and 0.4 MPa,respectively.With a feed of 2.5 MPa CH4 ＋ 0.4 MPa O2 ＋ 0.4 MPa N2,the optimal reaction conditions are 130 ℃,reaction time of 3 h,and volume ratio of CH3COOH to H2O being 4;under such conditions,the yield of methanol reaches 1 650 μmol in a 250 mL reactor.