Investigation into the roles of interfacial H2O structure in catalytic oxidation of HCHO and CO over CuMnO2 catalysts.
Investigation into the roles of interfacial H2O structure in catalytic oxidation of HCHO and CO over CuMnO2 catalysts.
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DOI：
10.1016/j.jes.2022.10.044
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发表时间：
2022-11
影响因子：
6.9
通讯作者：
Chunyan Ma;Jushuang Pan;Cheng Chen;Yuanyuan Dong;Feng Yao;Fengbang Wang;Maoyong Song
中科院分区：
文献类型：
--
作者：
Chunyan Ma;Jushuang Pan;Cheng Chen;Yuanyuan Dong;Feng Yao;Fengbang Wang;Maoyong Song
高性价比的MnO2基催化剂在潮湿空气中的快速失活限制了其在实际中的应用，而水在氧化过程中的作用的识别对于开发耐水的MnO2基催化剂具有重要意义。在相对湿度为40%的潮湿空气中，CuMnO2在室温下10小时内显示出20.3%的甲醛转化率，但在干燥空气中3小时后失活。湿空气中甲醛氧化具有良好的活性和稳定性，这归功于水通过在CuMnO2表面形成氢键促进甲醛氧化成H2O-HOCH2OH超分子组件。H2O-HOCH2OH超分子组装体容易被氧化成碳酸盐，碳酸盐进一步被氧化成二氧化碳。此外，CuMnO2在潮湿空气中表现出较差的CO氧化活性，但在干燥空气中10小时内CO转化率仍为100%。水在CuMnO2上对CO表现出竞争吸附作用。CuMnO2可用于湿空气中的甲醛脱除和干燥空气中的CO脱除。
The rapid deactivation of cost-effective MnO2-based catalysts in humid air limits their application in practice, and the identification of the role of water in an oxidation process is significant for developing water-resistant MnO2-based catalysts. Here, CuMnO2showed a 20.3% HCHO conversion in 10 hr at room temperature in humid air with relative humidity of 40%, but deactivated in 3 hr in dry air. The excellent activity and stability of HCHO oxidation in humid air were attributed to the positive effect of H2O on HCHO oxidation to the H2O-HOCH2OH supermolecule assemblies via hydrogen bonds formed on CuMnO2. H2O-HOCH2OH supermolecule assemblies tend to be oxidized to carbonate, which is further oxidized to CO2. Furthermore, CuMnO2exhibited a much poorer activity of CO oxidation in humid air, but the CO conversion was still 100% in 10 hr in dry air. H2O showed a competitive adsorption effect to CO on CuMnO2. CuMnO2could be applied in HCHO elimination in humid air and CO elimination in dry air.