Abstract
Surface-initiated Cu(0)-mediated controlled radical polymerization (Si-CuCRP) can be successfully applied to fabricate poly[(oligoethylene glycol)methyl ether methacrylate] (POEGMA) brushes in one pot, presenting a grafting-density gradient across the surface. This is achieved by continuously varying the distance (d) between a copper plate, used as a source of Cu species, and the initiator-functionalized substrate. X-ray photoelectron spectroscopy (XPS) analysis of monolayers of CuI-selective ligands demonstrates that a higher concentration of activator species diffuses to the initiating substrate in areas closer to the copper plate, a progressive decrease in activator concentration being observed upon increasing the distance between the two surfaces. As confirmed by the SI-CuCRP kinetics measured at different positions along the gradient, radical-termination reactions between propagating chains limit the grafting density of POEGMA grafts where the diffusion of activators is favored (i.e., at d → 0). This...
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