Well-defined ultrahigh molecular weight (UHMW) polymers exhibit great potential as high-performance materials such as durable lubrication and thick coating. However, undertaking reversible deactivation radical polymerizations (RDRPs) for the synthesis of UHMW polymers remains a formidable challenge because irreversible chain termination and initiators decay occur. Most of the UHMW polymers synthesized so far have been limited to conjugated monomers, such as acrylamide, acrylate, and styrene, while the synthesis of UHMW polymers using unconjugated monomers, such as N-vinyl pyrrolidone (NVP) and N-vinylcaprolactam (NVCL), has rarely been reported arising from the high reactivity of the propagating radicals. We report a new strategy for obtaining UHMW polymers from unconjugated monomers via photoenzymatic RAFT polymerization. Low dispersion UHMW linear and star polymers from unconjugated monomers have been achieved at 10 <sup>o</sup>C for the first time. Advantages of this method include mild conditions, oxygen-tolerant operation, scalable synthesis, etc.

Achieving ultrahigh molecular weight polymers from unconjugated monomers via photoenzymatic RAFT polymerization

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