The synthesis of functional and processable polyethylenes from simple vinyl monomers with controlled molecular weights and architectures has been a grand challenge of polymer chemistry. Post-polymerization modification of the homopolymers of ethylene is attractive for this purpose but has been hampered by the lack of efficient methods for the selective functionalization of C–H bonds in polyolefins. We report the selective, catalytic oxidation of C–H bonds in commodity polyethylenes with varying molecular weights and architectures. Remarkably, the functionalized materials, even at low levels of functionalization, exhibit physical properties that are absent in unmodified polyolefins, such as strong adhesion and the ability to be painted with common waterborne latex paint. Such observations indicate that selectively modified polyethylenes as described here may help to transform existing commodity plastics into more valuable and potentially more sustainable materials.

由具有受控分子量和结构的简单乙烯基单体合成功能性和可加工聚乙烯一直是聚合物化学的一大挑战。乙烯均聚物的聚合后改性对此很有吸引力，但由于缺乏对聚烯烃中C–H键进行选择性官能化的有效方法而受到阻碍。我们报道了具有不同分子量和结构的商品聚乙烯中C–H键的选择性催化氧化。引人注目的是，即使在低官能度的情况下，官能化的材料也表现出未改性的聚烯烃所不具备的物理性能，例如强粘合性和可以用普通的水性乳胶漆进行涂漆的能力。