This report studied the changes in the slow dynamics of polyacrylate by adding a hindered phenol (CA) capable of forming three intermolecular hydrogen bonds (inter-HBs) per molecule with the polymer chain. The CA molecule apparently diminishes the slow modes (with lower peak temperatures and peak heights) of the polyacrylate, although it has a higher glass transition temperature () than the acrylic matrix, and the rigid CA-bridged HB network significantly amplifies the α-relaxation near (with higher peak temperatures and peak heights). Consequently, the mixtures exhibit a diminishing slow mode that gradually merges with the prominent -peak with increasing CA loadings. The anomalous dynamics concerning the opposite behaviors of the slow mode and α-relaxation was further rationalized in terms of dissociation of inter-HBs when the temperature is higher than , together with the small molecule-alleviated macromolecular connectivity. This work provides essential insights into the slow dynamics of such HB-driven hybrids, and paves the way for tailoring the viscous flow properties of the hybrid material from a molecular level perspective.
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