Shen Zilong, Li Wenzhi, Jin Jingting, Lu Zhiheng, Wang Liqun, Jiang Yihang, Yuan Liang
Laboratory of Clean Low-Carbon Energy, Department of Thermal Science and Energy Engineering, University of Science and Technology of China Hefei 230023 P. R. China
National & Local Joint Engineering Research Center of Precision Coal Mining, Anhui University of Science and Technology Huainan 232001 P. R. China.
RSC Adv. 2025 Mar 17;15(11):8244-8252. doi: 10.1039/d5ra01115a.
Direct functionalization of methane in natural gas is of paramount importance but faces tremendous challenges. We reported a nickel-modified copper zeolite catalyst for the selective oxidation of methane into methanol. Using HO as an oxidant in the liquid phase at 80 °C, CuNi/ZSM-5 catalyst presented a relatively high methanol yield of 82 162 μmol g h (with a methanol selectivity of ∼74%). Combining series of designed experiments and thorough characterization analysis, including electron microscopy, X-ray photoelectric spectroscopy, Fourier transform infrared reflection as well as diffuse reflectance infrared Fourier transform spectroscopy, abundant Cu active sites were found on Ni-Promoted Cu/ZSM-5, differing from the dominating Cu active sites over Cu/ZSM-5. Cu active sites had an excellent ability to promote CH adsorption, CH activation and CHOH generation compared to Cu active sites. This work elucidates a constellation of insightful and potent perspectives for further improvement of metal-zeolite catalysts for the direct oxidation of methane to methanol.
天然气中甲烷的直接官能团化至关重要，但面临巨大挑战。我们报道了一种用于将甲烷选择性氧化为甲醇的镍改性铜沸石催化剂。在80°C的液相中使用HO作为氧化剂，CuNi/ZSM-5催化剂表现出相对较高的甲醇产率，为82 162 μmol g h（甲醇选择性约为74%）。结合一系列设计实验和全面的表征分析，包括电子显微镜、X射线光电子能谱、傅里叶变换红外反射以及漫反射红外傅里叶变换光谱，在镍促进的Cu/ZSM-5上发现了丰富的铜活性位点，这与Cu/ZSM-5上占主导的铜活性位点不同。与铜活性位点相比，铜活性位点具有促进CH吸附、CH活化和CHOH生成的优异能力。这项工作为进一步改进用于将甲烷直接氧化为甲醇的金属沸石催化剂阐明了一系列有见地和有效的观点。
