低碳烷烃均相转化研究进展

Homogeneous functionalization of light alkanes

低碳烷烃广泛存在于天然气和石油伴生气中,其资源丰富、价格低廉,有望在未来取代石油成为更加绿色、经济的新型能源和化工原料.但由于C–H键相对惰性和反应选择性差,低碳烷烃的高效转化一直是化学家们面临的重大挑战.本文从C–H键活化机制出发总结了低碳烷烃在均相催化领域中的研究进展,包括水和酸性体系及一些特殊溶剂,通过亲电活化、氧化加成、卡宾插入和自由基活化等多种不同活化机制,实现了低碳烷烃的高附加值转化.

Light alkanes are the most abundantly available carbon-based feedstocks on earth and as major constituents of natural gas and oil-associated gas. Compared with oil, natural gas is considered a greener fuel and promising alternative for energy and chemical production. However, the grand challenge in the chemistry of light alkanes utilization is the development of an efficient method for the selective activation C–H bond. The transportation issue comes from the low boiling point. On the other hand, these unactivated molecules are hard to be activated under mild conditions because of their high bond dissociation energy and low acidity. Moreover, the functionalized products, such as ethylene or methanol, have higher reactivity than light alkanes. Due to these challenges, it is vital that develop efficient processes to achieve value-added convert under economic and green reaction conditions. In this review, we summarized the recent progress in the field of homogeneous functionalizations of light alkanes and was subtitled to four different aspects according to the mechanism, including electrophilic substitution, oxidative addition, carbene insertion,and free radical substitution. However, developing a new, lower temperature, economic, and green direct light alkanes conversion process is still needed to address.