Temperature- and Voltage-Induced Ligand Rearrangement of a Dynamic Electroluminescent Metallopolymer

A dynamic‐covalent metal‐containing polymer was synthesized by the condensation of linear diamine and dialdehyde subcomponents around copper(I) templates in the presence of bidentate phosphine ligands. In solution, the red polymers undergo a sol–gel transition upon heating to form a yellow gel, a process that can be either reversible or irreversible depending on the solvent used. When fabricated into a light‐emitting electrochemical cell (LEC), the polymer emits infrared light at low voltage. As the voltage is increased, a blue shift in the emission wavelength is observed until yellow light is emitted, a process which is gradually reversed over time upon lowering the voltage. The mechanism underlying these apparently disparate responses is deduced to be due to loss of the copper phosphine complex from the polymer. Tunable LECs: A dynamic‐covalent metal‐containing polymer which can reversibly rearrange its structure in response to high temperature or electric field is reported. In solution, the polymers form heat‐set gels at high temperatures. When incorporated into light‐emitting electrochemical cells (LECs), the wavelength of emission depends on the applied voltage.