负载型非晶态Co-B催化剂在1-辛烯氢甲酰化中的应用

以醇凝胶-氮气热处理方法制备的ZrO2、碳纳米管(CNTs)及介孔分子筛SBA-15作为载体,采用化学还原法制备了负载型非晶态Co-B催化剂,利用粉末X射线衍射(XRD)、氮气吸附等温线、透射电子显微镜(TEM)、电感耦合等离子体-原子发射光谱(ICP-AES)以及X射线光电子能谱(XPS)等对催化剂进行了表征.以1-辛烯的氢甲酰化为目标反应,考察了负载型非晶态Co-B催化剂在氢甲酰化反应中的性能及循环使用效果.表征结果显示,以NaBH4为还原剂制备的负载型Co-B催化剂上的Co-B为非晶态,负载Co-B组分对载体的晶相结构没有影响.反应结果表明,在1-辛烯的氢甲酰化反应中,负载型非晶态Co-B催化剂都显示较高的初始活性.随着循环次数的增加,三种催化剂的活性下降,但下降幅度有所不同,Co-B/CNTs和Co-B/SBA-15的循环使用稳定性高于Co-B/ZrO2.

1-Octene Hydroformylation Using Supported Amorphous Co-B Catalysts

Co-B catalysts supported on ZrO₂ (prepared by alcogel nitrogen thermo-treatment method), carbon nanotubes (CNTs), and mesoporous SBA-15 as supports were prepared by chemical reduction method and characterized by X-ray diffraction (XRD), nitrogen physisorption, transmission electron microscopy (TEM), inductively coupled plasma -atomic emission spectrometry (ICP-AES) and X-ray photoelectron spectroscopy (XPS). Hydroformylation of 1-octene was used as a probe reaction to investigate the catalytic performance and stability of the catalysts in recycles. The as-prepared Co-B catalysts showed amorphous characteristics and the support structures were unchanged. The reaction results reveal that the catalytic activities of Co-B/CNTs, Co-B/ZrO₂ and Co-B/SBA-15 in the hydroformylation of 1-octene were comparatively high. However, the catalytic activities decreased upon recycling. Nevertheless, the Co-B/ CNTs and Co-B/SBA-15 were relatively stable compared with Co-B/ZrO₂.