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A photomediated approach allows a one-pot fabrication of stable coatings of polyelectrolyte complexes with a reversible crosslinking. 

Polymerization-induced self-assembly (PISA) is leveraged for the synthesis of ultra-high molecular weight polymers in concentrated but free-flowing dispersions. 

Wavelength-dependent photoreactions present an opportunity to achieve chemoselectivity of functional groups that otherwise demonstrate similar reactivity under traditional thermal conditions. 

Abstract We describe a methodology of post‐polymerization functionalization to enable subsequent bulk depolymerization to monomer by utilizing mechanochemical macro‐radical generation. By harnessing ultrasonic chain‐scission in the presence ofN‐hydroxyphthalimide methacrylate (PhthMA), we successfully chain‐end functionalize polymers to promote subsequent depolymerization in bulk, achieving up to 82 % depolymerization of poly(methyl methacrylate) (PMMA) and poly(α‐methylstyrene) (PAMS) within 30 min. This method of depolymerization yields a high‐purity monomer that can be repolymerized. Moreover, as compared to the most common methods of depolymerization, this work is most efficient with ultra‐high molecular weight (UHMW) polymers, establishing a method with the potential to address highly persistent, non‐degradable all‐carbon backbone plastic materials. Lastly, we demonstrate the expansion of this depolymerization method to commercial cell cast PMMA, achieving high degrees of depolymerization from post‐consumer waste. This work is the first demonstration of applying PhthMA‐promoted depolymerization strategies in homopolymer PMMA and PAMS prepared by conventional polymerization methods.