活性炭负载Au-Cu二元催化剂用于多相甲醇羰基化反应

Activated carbon supported Au-Cu binary catalyst for heterogeneous methanol carbonylation

通过浸渍法制备了一系列活性炭(AC)负载的Au-M/AC二元催化剂(M为金属元素),采用ICP-OES、XRD、TEM、XPS、H2-TPR和N2吸附-脱附等分析手段对制备的催化剂进行表征,考察了多种金属组分对催化剂甲醇羰基化催化性能的影响。实验结果表明,与单一组分的Au/AC催化剂相比,Au-M/AC催化剂催化甲醇羰基化的活性均有不同程度的提高,其中,Au-Cu/AC催化剂表现最佳,在240℃、1.7 MPa、n(CH3I)∶n(MeOH)∶n(CO)=1∶24∶25、GHSV=3600 h-1的条件下,Au-Cu/AC催化剂对乙酰基产物的选择性和时空收率分别98.5%和499.5 g/(kg h)。表征结果显示,制备的1Au1Cu/AC催化剂中,Au主要以纳米颗粒分散在载体表面上,Cu以高价氧化态高度分散在催化剂的表面。

A series of activated carbon(AC)supported Au-M/AC binary catalysts(M represents metal element)were prepared by impregnation method,and characterized by ICP-OES,XRD,TEM,XPS,H2-TPR and N2 adsorption-desorption and other analysis methods.The effects of various metal components on the catalytic performance of catalysts in methanol carbonylation were investigated.The experimental results show that the activity of Au-M/AC catalysts in methanol carbonylation is improved to different extents compared with the single-component Au/AC catalyst,wherein,the performance of Au-Cu/AC catalysts is the best.The selectivity and time space yield to acetyl of Au-Cu/AC catalysts achieved 98.5%and 499.5 g/(kg h),respectively at 240℃,1.7 MPa,n(CH3I)∶n(MeOH)∶n(CO)1∶24∶25,GHSV 3600 h-1.The characterization results of the prepared 1Au1Cu/AC catalyst show that Au was mainly dispersed on the surface of the carrier by nanoparticles,while Cu was highly dispersed on the surface of the catalyst in a high-valence oxidation state.