Controlled Synthesis of Proton-Conductive Porous Organic Polymer Gels via Electrostatically Stabilized Colloidal Formation

Porous organic polymers (POPs) have attracted extensive interest due to their structural diversity and predesigned functionality. However, the majority of POPs are synthesized as insoluble and unprocessable powders, which greatly impede their advanced applications because of limited mass transport and inadaptation for device integration. Herein, we report a controlled synthetic strategy of macroscopic POP gels by a cation-stabilized colloidal formation mechanism, which is widely adaptable to a large variety of tetra-/tri-amino build blocks for the synthesis of Troger's base-linked POP gels, aerogels, and ionic gels. The POP gels combined the integrated advantages of hierarchically porous structures and tailor able mechanical stiffness, whereas they could load substantial amounts of phosphoric acids and construct unimpeded transport pathways for proton conduction, exhibiting unprecedented proton conductivity at subzero temperatures. Our strategy offers a new solution to the intractable processing issues of POPs toward device applications with cutting-edge performances.