Wu Wenjian, Li Wenzhi, Wu Mingwei, Zhang Hao, Zhu Chen, Jiang Yihang
Laboratory of Clean Low-Carbon Energy, University of Science and Technology of China Hefei 230023 PR China
Institute of Energy, Hefei Comprehensive National Science Center Hefei 230031 PR China.
RSC Adv. 2023 Feb 13;13(8):5393-5404. doi: 10.1039/d3ra00058c. eCollection 2023 Feb 6.
Upgrading methane into methanol or other high value-added chemicals is not only beneficial to mitigate the greenhouse effect, but also provides basic raw materials for industrial production. Nowadays, most research is limited to zeolite systems, and it is a considerable challenge to extend the support to metal oxides while achieving a high yield of methanol. In this paper, we take advantage of impregnation methods to synthesise a novel Cu/MoO catalyst, which can convert methane to methanol in the gaseous phase. At 600 °C, the Cu(2)/MoO catalyst can achieve a maximum STY of 47.2 μmol (g h) with a molar ratio CH : O : HO = 5 : 1.4 : 10. Consequences of SEM, TEM, HRTEM and XRD substantiate that Cu is incorporated into the lattice of MoO to form CuMoO. And transmission infrared spectroscopy, Raman spectroscopy together with XPS characterization techniques confirm the generation of CuMoO, which is the main active site provider. This work provides a new support platform for Cu-based catalyst research in the methane-to-methanol system.
将甲烷升级转化为甲醇或其他高附加值化学品,不仅有利于缓解温室效应,还能为工业生产提供基础原料。如今,大多数研究局限于沸石体系,在将载体扩展至金属氧化物的同时实现甲醇的高产率是一项颇具挑战的任务。在本文中,我们利用浸渍法合成了一种新型的Cu/MoO催化剂,该催化剂能够在气相中将甲烷转化为甲醇。在600℃下,当CH∶O∶H₂O的摩尔比为5∶1.4∶10时,Cu(2)/MoO催化剂可实现47.2 μmol/(g h)的最大时空产率。扫描电子显微镜(SEM)、透射电子显微镜(TEM)、高分辨透射电子显微镜(HRTEM)和X射线衍射(XRD)的结果证实,Cu掺入MoO的晶格中形成了CuMoO。此外,傅里叶变换红外光谱(FTIR)、拉曼光谱以及X射线光电子能谱(XPS)表征技术证实了CuMoO的生成,它是主要的活性位点提供者。这项工作为甲烷制甲醇体系中铜基催化剂的研究提供了一个新的载体平台。