双金属Co/Pd纳米催化剂催化乙炔双羰化反应的性能研究

Access to Highly Active Co/Pd Bimetallic Nanoparticle Catalysts for Acetylene Dicarbonylation Reactions

采用一步还原法制备了一系列双金属纳米Pd基合金催化剂,以获得优秀的乙炔双羰化反应催化剂。利用透射电子显微镜(TEM)、X-射线光电子能谱(XPS)、X-射线衍射(XRD)、原位红外光谱(In-situ IR)等手段对催化剂的性质进行了研究。考察了掺杂金属、溶剂、助剂种类及用量、一氧化碳压力、温度对反应产率的影响。结果表明:以乙腈为溶剂,乙炔、一氧化碳和甲醇为原料合成丁烯二酸二甲酯,Co/Pd双金属纳米催化剂的活性最高,在低温低压条件下丁烯二酸二甲酯的总产率可达97.99%。Co元素的引入,有助于降低Pd对一氧化碳吸附强度,使更多的吸附于催化剂表面的CO分子能参与反应,提高了Pd基纳米双金属催化剂催化乙炔双羰化反应的活性。

A series of bimetallic nano Pd-based alloy catalysts were prepared by one-step reduction method and used to obtain excellent catalysts for acetylene dicarbonylation reactions.The transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD),and in situ infrared spectroscopy(In-situ IR)were used to investigate the composition and structure of Co/Pd catalysts.The effects of doping metal,solvent,type and dosage of promoter,carbon monoxide pressure and temperature on the reaction yield were investigated.The results show that the Co/Pd bimetallic nano-catalysts have excellent catalytic activity in the reaction of acetonitrile,acetylene,carbon monoxide,and methanol,and the total yield of acetylene dicarbonylation can reach 97.99%at low temperature and low pressure.The introduction of Co reduces the chemisorption strength of CO chemisorption on Pd,so that more CO molecules adsorbed on the catalyst surface can participate in the reaction,and the Pd-based nano-catalysts catalytic activity for acetylene dicarbonylation are improved.