May Yu Aung, Wei Shuai, Yu Wen-Zhu, Wang Wei-Wei, Jia Chun-Jiang
Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, China.
Langmuir. 2020 Sep 29;36(38):11196-11206. doi: 10.1021/acs.langmuir.0c00692. Epub 2020 Sep 17.
Copper manganese composite (hopcalite) catalyst has been widely explored for low-temperature CO oxidation reactions. However, the previous reports on the stabilization of such composite catalysts have shown that they deactivated severely under moist conditions. Herein, we developed an α-MnO nanorod-supported copper oxide catalyst that is very active and stable for the conditions with or without moisture by the deposition precipitation (DP) method. Incredibly, the CuO/MnO DP catalyst (with 5 wt % copper loading) achieves superior activity with a reaction rate of 9.472 μmol·g·s even at ambient temperatures, which is at least double times of that for the reported copper-based catalyst. Additionally, the CuO/MnO DP catalyst is significantly more stable than the copper manganese composite catalysts reported in the literature under the presence of 3% water vapor as well as without moisture. A correlation between the catalytic CO oxidation activity and textural characteristics was derived multitechnique analyses. The results imply that the superior activity of the CuO/MnO DP catalyst is associated with the proper adsorption of CO on partially reduced copper oxide as Cu(I)-CO and more surface oxygen species at the interfacial site of the catalyst.
铜锰复合(霍加拉特)催化剂已被广泛用于低温CO氧化反应的研究。然而,先前关于此类复合催化剂稳定性的报道表明,它们在潮湿条件下会严重失活。在此,我们通过沉积沉淀(DP)法制备了一种α-MnO纳米棒负载的氧化铜催化剂,该催化剂在有无水分的条件下都具有很高的活性和稳定性。令人惊讶的是,即使在环境温度下,CuO/MnO DP催化剂(铜负载量为5 wt%)也具有优异的活性,反应速率为9.472 μmol·g·s,这至少是已报道的铜基催化剂的两倍。此外,在3%水蒸气存在以及无水分的情况下,CuO/MnO DP催化剂比文献报道的铜锰复合催化剂显著更稳定。通过多种技术分析得出了催化CO氧化活性与结构特征之间的相关性。结果表明,CuO/MnO DP催化剂的优异活性与CO在部分还原的氧化铜上以Cu(I)-CO形式的适当吸附以及催化剂界面处更多的表面氧物种有关。