Organic Radical-Linked Covalent Triazine Framework with Paramagnetic Behavior

The production of multifunctional pure organic materials that combine different sizes of pores and a large number of electron spins is highly desirable due to their potential applications as polarizers for dynamic nuclear polarization-nuclear magnetic resonance and as catalysts and magnetic separation media. Here, we report a polychlorotriphenylmethyl radical-linked covalent triazine framework (PTMR-CTF). Two different sizes of micropores were established by N₂ sorption and the presence of unpaired electrons (carbon radicals) by electron spin resonance and superconducting quantum interference device-vibrating sample magnetometer analyses. Magnetization measurements demonstrate that this material exhibits spin-half paramagnetism with a spin concentration of ∼2.63 × 10²³ spins/mol. We also determined the microscopic origin of the magnetic moments in PTMR-CTF by investigating its spin density and electronic structure using density functional theory calculations.