Atakan Aylin, Keraudy Julien, Mäkie Peter, Hulteberg Christian, Björk Emma M, Odén Magnus
Nanostructured Materials, Department of Physics, Chemistry and Biology, Linköping University, Linköping SE 58183, Sweden.
Plasma and Coatings Physics, Department of Physics, Chemistry and Biology, Linköping University, Linköping SE 58183, Sweden.
J Colloid Interface Sci. 2019 Jun 15;546:163-173. doi: 10.1016/j.jcis.2019.03.046. Epub 2019 Mar 14.
A hybrid catalyst consisting of Zr-doped mesoporous silica (Zr-SBA-15) supports with intergrown Cu nanoparticles was used to study the effects of a catalyst's chemical states on CO hydrogenation. The chemical state of the catalyst was altered by using tetraethyl orthosilicate (TEOS) or sodium metasilicate (SMS) as the silica precursor in the synthesis of the Zr-SBA-15 framework, and infiltration (Inf) or evaporation induced wetness impregnation (EIWI) as the Cu loading method. As a result, the silica precursor mainly affects the activity of the catalyst whereas the Cu loading method alters the selectivity of the products. TEOS materials exhibit a higher catalytic activity compared to SMS materials due to different Zr dispersion and bonding to the silica matrix. EIWI catalysts display selectivity for methanol formation, while the Inf ones enable methanol conversion to DME. This is correlated to a higher Zr content and lower Cu oxidation states of EIWI prepared catalysts.
一种由掺杂锆的介孔二氧化硅（Zr-SBA-15）载体与共生的铜纳米颗粒组成的混合催化剂被用于研究催化剂化学状态对CO加氢的影响。在Zr-SBA-15骨架的合成中，通过使用正硅酸四乙酯（TEOS）或偏硅酸钠（SMS）作为二氧化硅前驱体，以及采用浸润法（Inf）或蒸发诱导浸渍法（EIWI）作为铜负载方法来改变催化剂的化学状态。结果表明，二氧化硅前驱体主要影响催化剂的活性，而铜负载方法则改变产物的选择性。由于Zr在二氧化硅基质中的分散和键合不同，TEOS材料比SMS材料表现出更高的催化活性。EIWI催化剂对甲醇生成具有选择性，而浸润法制备的催化剂则能使甲醇转化为二甲醚。这与EIWI制备的催化剂中较高的Zr含量和较低的铜氧化态相关。
