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Slurry methanol synthesis from CO2 hydrogenation over micro-spherical SiO2 support Cu/ZnO catalysts
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2018-07-03 , DOI: 10.1016/j.jcou.2018.06.023
Ying Jiang , Haiyan Yang , Peng Gao , Xiaopeng Li , Jianming Zhang , Hongjiang Liu , Hui Wang , Wei Wei , Yuhan Sun

The micro-spherical SiO2 support is prepared by the spray-drying method, and then a series of SiO2 supported Cu/ZnO-based catalysts with different percentage of Cu and ZnO are synthesized by ammonia-evaporation method. The Cu and ZnO loadings play a critical role on the physicochemical properties and catalytic performance of catalysts. The results show that Cu and Zn cations can be deposited into the pores of the micro-spherical SiO2 with well-distributed when the metal loadings are below 47.91 wt%. In addition, the specific surface area of catalysts increases with increasing loadings due to the formation of porous structure inside SiO2 support, while it decreases when the metal loading is above 47.91 wt%. According to XRD, XPS, XAES and CO adsorption in situ FTIR analysis, both Cu+ and Cu° species exist on the reduced surface of Cu/ZnO/SiO2 catalysts. The catalytic performance for slurry methanol synthesis from CO2 hydrogenation is examined. The Cu/ZnO/SiO2 catalyst exhibits an optimum catalytic activity when the metal loading reaches to 28.23 wt%. However, the CO2 conversion changes slightly with a further increase of metal loadings, because the pore of support is blocked and the reducibility of catalysts is decreased significantly with incorporation of excess metal compounds into SiO2. In addition, the methanol selectivity enhances with increasing metal loadings due to the decrease of the proportion of Cu+ species.



中文翻译:

微球SiO 2载体Cu / ZnO催化剂上CO 2加氢制浆甲醇

采用喷雾干燥法制备了微球形SiO 2载体,然后通过氨蒸发法合成了一系列Cu和ZnO含量不同的SiO 2负载的Cu / ZnO基催化剂。铜和锌的负载量对催化剂的物理化学性质和催化性能起着至关重要的作用。结果表明,当金属负载量低于47.91 wt%时,Cu和Zn阳离子可以均匀分布在微球形SiO 2的孔中。另外,由于在SiO 2内部形成多孔结构,催化剂的比表面积随负载增加而增加。支持,而当金属负载量高于47.91 wt%时,它会降低。根据XRD,XPS,XAES和CO吸附原位FTIR分析,Cu / ZnO / SiO 2催化剂的还原表面上都存在Cu +和Cu°物种。考察了由CO 2加氢合成淤浆甲醇的催化性能。当金属负载量达到28.23 wt%时,Cu / ZnO / SiO 2催化剂表现出最佳的催化活性。但是,随着金属负载量的进一步增加,CO 2的转化率会略有变化,这是因为载体的孔被堵塞,并且由于将过量的金属化合物掺入SiO 2中,催化剂的还原性大大降低了。。另外,由于Cu +种类比例的降低,甲醇选择性随金属负载量的增加而提高。

更新日期:2018-07-03
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