预处理条件对金属有机框架衍生的负载钴催化剂的结构和催化性能的影响  

Influence of pretreatment conditions on the structure and catalytic performance of supported cobalt catalysts derived from metal-organic frameworks

作　　者：孙甲强[1,2] 郑申棵 陈建刚 SUN Jia-qiang;ZHENG Shen-ke;CHEN Jian-gang(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;Hubei Key Laboratory for Processing and Application of Catalytic Materials,College of Chemistry and Chemical Engineering,Huanggang Normal University,Huanggang 438000,China)

机构地区：[1]中国科学院山西煤炭化学研究所煤转化国家重点实验室,山西太原030001 [2]中国科学院大学,北京100049 [3]黄冈师范学院化学化工学院催化材料制备及应用湖北省重点实验室,湖北黄冈438000

出　　处：《燃料化学学报（中英文）》2023年第9期1291-1297,共7页Journal of Fuel Chemistry and Technology

基　　金：supported by the National Natural Science Foundation of China (21503256, 22072175);“Strategic Priority Research Program” of the Chinese Academy of Sciences (XDA21021000);Sanju Environmental Protection New Material Company and the Research Foundation of Huanggang Normal University (2042020026)。

摘　　要：通过金属有机框架材料介导的合成策略制备了负载钴催化剂(Co@C-ZnZrO_(2)和Co/ZnZrO_(2))并进行费托合成性能评价,重点研究了金属有机框架材料热解对负载钴催化剂结构和费托合成性能的影响。采用粉末X射线衍射、透射电镜、高分辨率透射电镜、N_(2)吸附-脱附和X射线光电子能谱对负载钴催化剂的晶相和微观结构进行了表征。费托合成性能研究显示,Co/ZnZrO_(2)的CO转化率为18.1%,C_(5+)选择性为77.4%,而Co@C-ZnZrO_(2)的CO转化率为8.5%,C_(5+)选择性为35.2%。Co/ZnZrO_(2)较高的CO转化率是由于暴露了较多的活性钴位点。而在Co@C-ZnZrO_(2)催化剂上活性Co位点的作用受到碳层的限制,抑制了合成气在Co位点上的吸附和活化。Supported cobalt catalysts(Co@C-ZnZrO_(2) and Co/ZnZrO_(2))were prepared through a metal-organic frameworks(MOFs)-mediated synthesis strategy.The influence of MOFs pyrolysis on the structure and Fischer-Tropsch synthesis performance of supported cobalt catalysts was investigated.The crystalline phase and microstructure of supported cobalt catalysts were characterized by powder X-ray diffraction(XRD),transmission electron microscopy(TEM),high-resolution TEM(HRTEM),N_(2) adsorption-desorption and X-ray photoelectron spectroscopy(XPS).The Co/ZnZrO_(2) showed the CO conversion of 18.1%and the C_(5+)selectivity of 77.4%,whereas the Co@C-ZnZrO_(2) exhibited the CO conversion of 8.5%and the C_(5+)selectivity of 35.2%.The excellent CO conversion for Co/ZnZrO_(2) was attributed to the more exposure of active Co sites.Meanwhile,the activity of Co sites on Co@C-ZnZrO_(2) catalyst was restricted by the carbon layer,suppressing the adsorption and activation of syngas on Co sites.

关 键 词：热解 金属有机框架 负载钴催化剂 费托合成 

分 类 号：O643[理学—物理化学]