Jurca Bogdan, Peng Lu, Primo Ana, Gordillo Alvaro, Dhakshinamoorthy Amarajothi, Parvulescu Vasile I, García Hermenegildo
Department of Organic Chemistry and Biochemistry and Catalysis, Faculty of Chemistry, University of Bucharest, Bdul Regina Elisabeta 4-12, 030016 Bucharest, Romania.
Instituto Universitario de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas, Av. De los Naranjos s/n, 46022 Valencia, Spain.
Nanomaterials (Basel). 2022 Sep 16;12(18):3220. doi: 10.3390/nano12183220.
Starting from the reported activity of Co-Fe nanoparticles wrapped onto graphitic carbon (Co-Fe@C) as CO hydrogenation catalysts, the present article studies the influence of a series of metallic (Pd, Ce, Ca, Ca, and Ce) and non-metallic (S in various percentages and S and alkali metals) elements as Co-Fe@C promoters. Pd at 0.5 wt % somewhat enhances CO conversion and CH selectivity, probably due to H activation and spillover on Co-Fe. At similar concentrations, Ce does not influence CO conversion but does diminish CO selectivity. A 25 wt % Fe excess increases the Fe-Co particle size and has a detrimental effect due to this large particle size. The presence of 25 wt % of Ca increases the CO conversion and CH selectivity remarkably, the effect being attributable to the CO adsorption capacity and basicity of Ca. Sulfur at a concentration of 2.1% or higher acts as a strong poison, decreasing CO conversion and shifting selectivity to CO. The combination of S and alkali metals as promoters maintain the CO selectivity of S but notably increase the CO conversion. Overall, this study shows how promoters and poisons can alter the catalytic activity of Co/Fe@C catalysts, changing from CH to CO. It is expected that further modulation of the activity of Co/Fe@C catalysts can serve to drive the activity and selectivity of these materials to any CO hydrogenation products that are wanted.
从报道的负载在石墨碳上的钴铁纳米颗粒(Co-Fe@C)作为一氧化碳加氢催化剂的活性出发,本文研究了一系列金属(钯、铈、钙、钙和铈)和非金属(不同百分比的硫以及硫与碱金属)元素作为Co-Fe@C促进剂的影响。0.5 wt%的钯在一定程度上提高了一氧化碳转化率和甲烷选择性,这可能是由于氢在钴铁上的活化和溢流。在相似浓度下,铈不影响一氧化碳转化率,但会降低一氧化碳选择性。25 wt%的过量铁会增加铁钴颗粒尺寸,由于颗粒尺寸较大而产生不利影响。25 wt%的钙的存在显著提高了一氧化碳转化率和甲烷选择性,这种效果归因于钙的一氧化碳吸附能力和碱性。浓度为2.1%或更高的硫起到强毒物的作用,降低一氧化碳转化率并使选择性转向一氧化碳。硫与碱金属作为促进剂的组合保持了硫的一氧化碳选择性,但显著提高了一氧化碳转化率。总体而言,这项研究表明促进剂和毒物如何改变Co/Fe@C催化剂的催化活性,使其从生成甲烷转变为生成一氧化碳。预计对Co/Fe@C催化剂活性的进一步调控可用于将这些材料的活性和选择性导向任何所需的一氧化碳加氢产物。