(2Cu-Ni)/α-ZrP催化剂催化二氧化碳和甲醇直接合成碳酸二甲酯

The Direct Synthesis of Dimethyl Carbonate from Carbon Dioxide and Methanol over (2Cu-Ni)/α-ZrP Catalyst

制备了一种新型催化剂(2Cu-Ni)/α-ZrP,可催化CO_2和CH_3OH直接合成碳酸二甲酯(DMC)的反应。其中,α-磷酸锆(α-ZrP)载体采用回流法制得,α-ZrP负载2Cu-Ni双金属催化剂用等体积浸渍法制得。采用红外光谱(FTIR)、热重(TG)、X射线衍射(XRD)、程序升温还原(TPR)和程序升温脱附(TPD)考察了催化剂的结构和表面的化学吸附性能。结果表明,负载催化剂表面既有酸性位也有碱性位,有利于CO_2和CH_3OH直接合成碳酸二甲酯的反应。考察了载体煅烧温度和活性组分负载量对(2Cu-Ni)/α-ZrP催化直接合成DMC性能的影响,发现500℃下煅烧,(2Cu-Ni)双金属负载量为7.5%制备的催化剂催化活性最好。在130℃,0.6 MPa的反应条件下,CH_3OH的转化率为5.1%,DMC选择性可达91.7%,而且催化剂的催化活性稳定。

A novel catalyst （2Cu-Ni）/α-ZrP was prepared to catalyze the direct synthesis of dimethyl carbonate （DMC） from CO2 and CH3OH. Among them, α-ZrP was prepared by reflux method and α-ZrP supported （2Cu-Ni） bimetallic catalyst was prepared by the same volume impregnation method. The structure and surface chemisorption properties of the catalysts were investigated by Fourier transform infrared spectroscopy （FTIR）, thermo gravimetric analysis （TG）, X-ray powder diffraction （XRD）, temperature programmed reduction （TPR） and temperature programmed desorption （TPD）. The results showed that both the acidic and the basic sites on the supported catalyst surface were favorable for the direct synthesis of dimethyl carbonate from CO2 and CH3OH. The effects of calcination temperature and the active component loading on the catalytic performance of the direct synthesis of DMC from CH3OH and CO2 were also investigated. It was found that the catalyst prepared by calcination at 500 had the best ℃ catalytic activity when （2Cu-Ni） bimetallic loading was 7.5%. Under the reaction conditions of 130 and ℃ 0.6 MPa, the conversion of CH3OH was 5.1%, the selectivity of DMC reached 91.7% and the catalytic activity was stable.