研究界面 HO 结构在 CuMnO 催化剂上催化氧化 HCHO 和 CO 中的作用。
Investigation into the roles of interfacial HO structure in catalytic oxidation of HCHO and CO over CuMnO catalysts.
机构信息
Key Laboratory of Environmental Nanotechnology and Health Effects, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China; University of Chinese Academy of Sciences, Beijing 100049, China.
No. 52 Institute of China North Industries Group Yantai Branch Co. Ltd., Yantai 264000, China.
出版信息
J Environ Sci (China). 2024 Mar;137:310-320. doi: 10.1016/j.jes.2022.10.044. Epub 2022 Nov 8.
The rapid deactivation of cost-effective MnO-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 MnO-based catalysts. Here, CuMnO showed 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 HO on HCHO oxidation to the HO-HOCHOH supermolecule assemblies via hydrogen bonds formed on CuMnO. HO-HOCHOH supermolecule assemblies tend to be oxidized to carbonate, which is further oxidized to CO. Furthermore, CuMnO exhibited a much poorer activity of CO oxidation in humid air, but the CO conversion was still 100% in 10 hr in dry air. HO showed a competitive adsorption effect to CO on CuMnO. CuMnO could be applied in HCHO elimination in humid air and CO elimination in dry air.
在潮湿空气中，成本效益高的 MnO 基催化剂会迅速失活，这限制了它们在实际中的应用，因此，确定水在氧化过程中的作用对于开发耐水 MnO 基催化剂具有重要意义。在这里，CuMnO 在相对湿度为 40%的潮湿空气中，在室温下 10 小时内甲醛的转化率达到了 20.3%，但在干燥空气中 3 小时后就失活了。CuMnO 在潮湿空气中具有出色的甲醛氧化活性和稳定性，这归因于 HO 通过在 CuMnO 上形成氢键，对甲醛氧化为 HO-HOCHOH 超分子组装体产生积极影响。HO-HOCHOH 超分子组装体容易被氧化为碳酸盐，碳酸盐进一步被氧化为 CO。此外，CuMnO 在潮湿空气中的 CO 氧化活性较差，但在干燥空气中仍能在 10 小时内实现 100%的 CO 转化率。HO 在 CuMnO 上对 CO 表现出竞争性吸附作用。CuMnO 可用于潮湿空气中的甲醛消除和干燥空气中的 CO 消除。
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