Ordered mesoporous carbons (OMCs) have demonstrated great potential in catalysis, and as supercapacitors and adsorbents. Since the introduction of the organic–organic self-assembly approach in 2004/2005 until now, the direct synthesis of OMCs is still limited to the wet processing of phenol-formaldehyde polycondensation, which involves soluble toxic precursors, and acid or alkali catalysts, and requires multiple synthesis steps, thus restricting the widespread application of OMCs. Herein, we report a simple, general, scalable and sustainable solid-state synthesis of OMCs and nickel OMCs with uniform and tunable mesopores (∼4–10 nm), large pore volumes (up to 0.96 cm³ g⁻¹) and high-surface areas exceeding 1,000 m² g⁻¹, based on a mechanochemical assembly between polyphenol-metal complexes and triblock co-polymers. Nickel nanoparticles (∼5.40 nm) confined in the cylindrical nanochannels show great thermal stability at 600 °C. Moreover, the nickel OMCs offer exceptional activity in the hydrogenation of bulky molecules (∼2 nm).

Porous organic materials (POMs) are of growing interest due to their potential uses in gas adsorption, separation, and catalysis. In comparison to porous inorganic materials (e.g., zeolites and metal oxides) or inorganic–organic hybrids (e.g., metal–organic frameworks), POMs possess a number of advantages, such as being composed of only light elements, possessing accessible functionality for organic reactions, having high stability in air and at atmospheric moisture levels, and possessing chemical robustness to acids and bases. Borrowed from the rich library of organic chemistry, various reaction routes like Sonogashira–Hagihara coupling, Yamamoto polymerization, Suzuki couplings, oxidative polymerization, the trimerization reaction of carbonitriles, solvothermal radical polymerization, and the imine condensation reaction, to name just a few, have been used to construct POMs. Not surprisingly, nearly all chemical transformations for POM construction proceed via solution-based synthesis methods. Just recently, much interesting progress on the mechanochemical synthesis (MS) of POMs has been made, highlighting the unique features of this method, such as solvent-free processing and fast reaction rates. In this mini-review, we wish to summarise the recent advances on the design of polymers of intrinsic microporosity, covalent–organic frameworks, covalent triazine-based frameworks, ordered mesoporous polymers, and ordered mesoporous carbons via MS. A brief comment about the MS of POMs in the future will also be discussed.