Microporous organic polymers (MOPs) have been prepared via one-pot polycondensation reactions between aldehydes and amines. Primary amines were reacted with imines to produce porous polymers from A₂ + B₂ monomer combinations. The resulting networks exhibit BET surface areas in the range 500–600 m² g⁻¹. This approach opens up the possibility of synthesising MOPs using readily-available and inexpensive precursors.

• Produced starch hydrogels through high temperature-pressure gelatinisation. • Employed a range of NMR methods to probe the molecular mobility and water dynamics. • Reported for the first time highly dynamic starch chains in the solvent phase of gels. • Correlated the degree of chain structural mobility with bulk properties. • Revealed a previously unknown level of molecular organisation in starch gels.

Supramolecular hydrogels are composed of self‐assembled solid networks that restrict the flow of water. l‐Phenylalanine is the smallest molecule reported to date to form gel networks in water, and it is of particular interest due to its crystalline gel state. Single and multi‐component hydrogels of l‐phenylalanine are used herein as model materials to develop an NMR‐based analytical approach to gain insight into the mechanisms of supramolecular gelation. Structure and composition of the gel fibres were probed using PXRD, solid‐state NMR experiments and microscopic techniques. Solution‐state NMR studies probed the properties of free gelator molecules in an equilibrium with bound molecules. The dynamics of exchange at the gel/solution interfaces was investigated further using high‐resolution magic angle spinning (HR‐MAS) and saturation transfer difference (STD) NMR experiments. This approach allowed the identification of which additive molecules contributed in modifying the material properties.