泡沫硅负载钴锰催化剂的制备及其合成气制低碳醇反应性能研究  

Preparation of silicon foam supported CoMn catalysts and their catalytic performances in higher alcohol synthesis via syngas

作　　者：杜鑫 张明伟[1] 房克功[1] DU Xin;ZHANG Mingwei;FANG Kegong(State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院山西煤炭化学研究所煤炭高效低碳利用全国重点实验室,山西太原030001 [2]中国科学院大学,北京100049

出　　处：《燃料化学学报（中英文）》2024年第9期1224-1234,共11页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(22179137)资助。

摘　　要：本研究采用浸渍法、沉淀法和水热合成法制备了一系列泡沫硅负载CoMn基催化剂,并结合XRD、H_(2)-TPR、N_(2)物理吸附-脱附、TEM和XPS等表征技术考察了制备方法对催化剂在合成气制低碳醇反应中的性能影响。研究表明,催化剂表面存在Co_(2+)(CO_(2)C)、Co^(0)物种,水热合成法制备的催化剂表面CO_(2)C-Co^(0)活性位点存在良好的协同作用有利于醇的生成,较高比例的CO_(2)C也促进了CO的非解离吸附和插入,从而呈现最高的醇选择性。在t=260℃,p=5.0 MPa,GHSV=4500 h^(-1),H_(2)/CO(体积比)=2∶1的反应条件下,该泡沫催化剂可实现CO转化率11.1%,总醇选择性34.7%,C_(2)+OH选择性34.5%的反应性能。A series of silicon foam supported CoMn catalysts were prepared using impregnation,precipitation,and hydrothermal methods.Combining the characterization techniques such as XRD,H_(2)-TPR,N_(2) physical adsorption,TEM,and XPS,the effect of different catalyst preparation methods on the catalytic performance in the synthesis of higher alcohols from syngas was investigated.Research has shown that there are Co^(2)+(Co_(2)C)and Co^(0) species on the surface of the catalyst.The active sites of Co_(2)C-Co^(0) on the surface of the catalyst prepared by hydrothermal synthesis have a good synergistic effect,which is conducive to the generation of alcohols.A higher proportion of Co_(2)C also promotes the associative adsorption and insertion of CO,resulting in the highest alcohol selectivity.Under the reaction conditions:t=260℃,p=5.0 MPa,GHSV=4500 h−1,H_(2)/CO(volume ratio)=2∶1,the catalyst exhibited the best reaction performance to achieve CO conversion of 11.1%,total alcohol selectivity of 34.7%,and C_(2)+OH selectivity of 34.5%.

关 键 词：合成气 低碳醇 泡沫硅 钴锰催化剂 

分 类 号：O643[理学—物理化学]