Solvent‐Free Self‐Assembly to the Synthesis of Nitrogen‐Doped Ordered Mesoporous Polymers for Highly Selective Capture and Conversion of CO₂

Abstract

A solvent-free induced self-assembly technology for the synthesis of nitrogen-doped ordered mesoporous polymers (N-OMPs) is developed, which is realized by mixing polymer precursors with block copolymer templates, curing at 140-180 °C, and calcination to remove the templates. This synthetic strategy represents a significant advancement in the preparation of functional porous polymers through a fast and scalable yet environmentally friendly route, since no solvents or catalysts are used. The synthesized N-OMPs and their derived catalysts are found to exhibit competitive CO₂ capacities (0.67-0.91 mmol g^-1 at 25 °C and 0.15 bar), extraordinary CO₂ /N₂ selectivities (98-205 at 25 °C), and excellent activities for catalyzing conversion of CO₂ into cyclic carbonate (conversion >95% at 100 °C and 1.2 MPa for 1.5 h). The solvent-free technology developed in this work can also be extended to the synthesis of N-OMP/SiO₂ nanocomposites, mesoporous SiO₂ , crystalline mesoporous TiO₂ , and TiPO, demonstrating its wide applicability in porous material synthesis.