Cao Yuehan, Huang Zeai, Han Chunqiu, Zhou Ying
National Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu, 610500, China.
School of New Energy and Materials, Southwest Petroleum University, Chengdu, 610500, China.
Adv Sci (Weinh). 2024 Mar;11(12):e2306891. doi: 10.1002/advs.202306891. Epub 2024 Jan 17.
Methane photooxidation into methanol offers a practical approach for the generation of high-value chemicals and the efficient storage of solar energy. However, the propensity for C─H bonds in the desired products to cleave more easily than those in methane molecules results in a continuous dehydrogenation process, inevitably leading to methanol peroxidation. Consequently, inhibiting methanol peroxidation is perceived as one of the most formidable challenges in the field of direct conversion of methane to methanol. This review offers a thorough overview of the typical mechanisms involved radical mechanism and active site mechanism and the regulatory methods employed to inhibit product peroxidation in methane photooxidation. Additionally, several perspectives on the future research direction of this crucial field are proposed.
甲烷光氧化生成甲醇为高价值化学品的生产和太阳能的高效储存提供了一种切实可行的方法。然而,目标产物中的C─H键比甲烷分子中的C─H键更容易断裂,这导致了一个连续的脱氢过程,不可避免地会导致甲醇过氧化。因此,抑制甲醇过氧化被认为是甲烷直接转化为甲醇领域最严峻的挑战之一。本综述全面概述了甲烷光氧化中涉及的典型机理(自由基机理和活性位点机理)以及用于抑制产物过氧化的调控方法。此外,还对这一关键领域未来的研究方向提出了一些观点。