Activity and Sediments Study for the Hydrocarboxylation of Acetylene with Carbon Monoxide to Acrylic Acid on Ni-Cu Homogeneous Catalyst
Activity and Sediments Study for the Hydrocarboxylation of Acetylene with Carbon Monoxide to Acrylic Acid on Ni-Cu Homogeneous Catalyst
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DOI：
10.1021/ie4021446
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发表时间：
2013-10-02
影响因子：
4.2
通讯作者：
Shi, Li
中科院分区：
文献类型：
--
作者：
Lin, Tie-jun;Meng, Xuan;Shi, Li
固体沉淀物是高温高压乙炔羟化法生产丙烯酸工业规模的关键问题。研究了沉积物的活动及其形成因素。实验表明，在一定乙炔初始分压下，沉淀主要是由Cu2+浓度引起的，丙烯酸收率达到80%。两种沉积物的粒径分布和颗粒形态不同，但均含有碳纳米纤维。SEM-EDXS，拉曼光谱，XRD和元素分析表明三种类型的焦炭（i,e，聚合物，丝状和石墨）和三种碳（即非晶碳，碳化物和石墨）。一般认为停留时间、反应温度和催化剂浓度分布对沉积物形成和副反应有影响。
Solid sediment is a key problem in the industrial-scale production of acrylic acid by hydrocarboxylation of acetylene under high temperature and pressure. The activity and factors for the formation of sediments have been studied. Experiments demonstrate that 80% yield of acrylic acid was achieved, and the sediments were mainly caused by the concentration of Cu2+ under a certain amount of acetylene initial partial pressure. The two kinds of sediments have different particle size distribution and different particle morphology, but both contain carbon nanofibers. SEM-EDXS, Raman spectra, XRD, and elemental analysis indicate three types of coke (i,e, polymeric, filamentous, and graphitic) and three carbon species (i.e., amorphous carbon, carbide, and graphite). It is generally accepted that residence time, reaction temperature, and distribution of catalyst concentration have an impact on sediment formation and side reactions.