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Cobalt oxide decorated porous silica particles: Structure and activity relationship in the catalytic oxidation of carbon monoxide
Applied Surface Science ( IF 6.3 ) Pub Date : 2021-12-05 , DOI: 10.1016/j.apsusc.2021.152121
Daniil A. Eurov 1 , Tatiana N. Rostovshchikova 2 , Marina I. Shilina 2 , Demid A. Kirilenko 1 , Maria V. Tomkovich 1 , Maria A. Yagovkina 1 , Olga V. Udalova 3 , Igor Yu. Kaplin 2 , Igor A. Ivanin 2 , Dmitry A. Kurdyukov 1
Affiliation  

Porous (0.6–30 nm) and non-porous spherical silica nanoparticles are synthesized. These silicas with different morphologies are decorated with cobalt (2.9 wt%) using Co(NO3)2·6H2O as precursor. Co-SiO2 particles are studied by N2 sorption, TEM, XRD, XPS, FTIR and TPR-H2 methods. Specific surface area (SSA) of the prepared materials is 10–1200 m2/g. The main crystalline phase is identified as Co3O4. The activity of Co-SiO2 composites in the CO oxidation and preferential oxidation of CO (PROX) in a H2-rich gas mixture improves with increasing atomic ratios of Co/Si and Co3+/Co2+ on the silica surface. Catalysts with the large mesopores containing mainly Co2+ are the least active. Co-SiO2 composites based on synthetic opal grown by sedimentation of non-porous silica particles with the lowest SSA demonstrate the highest catalytic activity. The CO conversion reaches 100% at 150 °C in the absence of hydrogen, while in PROX the 90% conversion of CO is achieved at 170 °C. The large Co3O4 aggregates between non-porous spherical silica particles of opal are the most active and stable during CO-PROX reaction. The lower interaction of Co3O4 nanoparticles with this support promotes the stabilization of the oxidized state Co3+ and provides a higher yield of CO2 in CO-PROX reaction.



中文翻译:

氧化钴修饰的多孔二氧化硅颗粒:一氧化碳催化氧化中的结构和活性关系

合成了多孔(0.6-30 nm)和无孔球形二氧化硅纳米粒子。使用Co(NO 3 ) 2 ·6H 2 O作为前体,这些具有不同形态的二氧化硅用钴(2.9wt%)装饰。通过N 2吸附、TEM、XRD、XPS、FTIR和TPR-H 2方法研究Co-SiO 2颗粒。所制备材料的比表面积 (SSA) 为 10–1200 m 2 /g。主晶相被确定为 Co 3 O 4。Co-SiO 2复合材料在H 2 中CO氧化和CO优先氧化(PROX)的活性富气体混合物随着二氧化硅表面上Co/Si 和 Co 3+ /Co 2+原子比的增加而改善。具有主要包含 Co 2+的大中孔的催化剂活性最低。基于合成蛋白石的Co-SiO 2复合材料通过无孔二氧化硅颗粒的沉降生长,SSA 最低,表现出最高的催化活性。在没有氢气的情况下,CO 转化率在 150 °C 时达到 100%,而在 PROX 中,CO 转化率在 170 °C 时达到 90%。蛋白石的无孔球形二氧化硅颗粒之间的大 Co 3 O 4聚集体在 CO-PROX 反应过程中是最活跃和最稳定的。Co 3 O 4的低相互作用具有这种支持的纳米颗粒促进了氧化态 Co 3+的稳定,并在 CO-PROX 反应中提供了更高的 CO 2产率。

更新日期:2021-12-13
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