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.