液相羰基法合成碳酸二甲酯的铜络合催化剂

Cu-Based Catalysts for Synthesis of Dimethyl Carbonate by Liquid-Phase Oxidative Carbonylation

用溴化铜和季铵盐制备了络合催化剂,并考察了几种无机盐助剂对催化剂性能的影响。结果表明,络合催化剂 Cu_xBr_nL_m 对甲醇液相氧化羰化合成碳酸二甲酯(DMC)具有良好的催化活性,以碳酸钾为助剂时,甲醇转化率达到了26.9%,DMC 选择性达到97.8%。采用傅立叶红外光谱(FT-IR)、X 射线衍射(XRD)、元素分析(EA)和电感耦合等离子发射光谱(ICP-AES)对合成的催化剂进行表征,结果表明,络合催化剂的分子式为 Cu_2Br_6L_2,配位剂和无机盐助剂有助于形成甲醇选择性氧化羰基合成 DMC 的活性物种 Cu(I),而 Cu(I)是催化剂活性中心。

The complex catalysts CuxBrnLn were prepared by combination of quaternary ammonium salt and CuBr2 and effects of several inorganic additives on catalytic performance of CuxBrnLm were investigated. The results showed that the catalytic performance of the complex catalyst for oxidative carbonylation of methanol was excellent. The conversion of methanol reached 26. 9% and the selectivity of DMC reached 97.80% while K2CO3 was added. The complex catalysts were characterized by methods of fourier transform infrared （FT-IR）, X-ray diffraction （XRD）, element analysis （EA） and inductively couple plasma （ICP）. The results indicated that the complex catalyst was Cu2Br6L2, the complexing agent and inorganic additives could promote formation of Cu（Ⅰ） active species for DMC synthesis and Cu（Ⅰ） was main active center of the catalyst.