Molecularly imprinted materials are man-made mimics of biological receptors. Their polymer network has recognition sites complementary to a substrate in terms of size, shape and chemical functionality. They have diverse applications in various chemical, biomedical and engineering fields such as solid phase extraction, catalysis, drug delivery, pharmaceutical purification, (bio)sensors, water treatment, membrane separations and proteomics. The stability and reusability of molecularly imprinted polymers (IPs) have crucial roles in developing applications that are reliable, economic and sustainable. In the present article the effect of crosslinkers, functional monomers and conditions for template extraction on the long-term stability and reusability of IPs was systematically investigated. Adsorption capacity, selectivity, morphology and thermal decomposition of eleven different L-phenylalanine methyl ester imprinted polymers were studied to reveal performance loss over 100 adsorption–regeneration cycles. Furthermore, crosslinker and functional monomer specific reversible and irreversible decomposition of imprinted polymers as a result of adsorbent regeneration were investigated through adsorption studies, electron microscopy, N₂ adsorption and thermogravimetric analysis. A decomposition mechanism was proposed and revealed using NMR spectroscopy. Solutions to avoid or overcome the limitations of the most common crosslinkers, functional monomers and extraction techniques were proposed and experimentally validated.

Downstream processing is considered to be the bottleneck in pharmaceutical manufacturing because its development has not kept pace with upstream production. In some cases, the lack of efficient downstream processing capacity can seriously affect both the sustainability and profitability of a pharmaceutical product and even result in its failure. Minimising solvent and raw material consumption, as well as utilising waste, can make a significant difference towards environmentally benign and economically viable chemical production. In this work, the authors present the development and modelling of a continuous adsorption process with in situ solvent recovery for the isolation of oleuropein from olive leaves, an agricultural waste. Waste utilisation in agriculture has gained increasing attention because this economic sector is ranked as the 2^nd highest global greenhouse gas emission contributor. Imprinted polymers were developed for the selective scavenging of oleuropein from olive leaf extracts using green solvents. The mild temperature-swing (25–43 °C) process allows the continuous isolation of oleuropein at 1.75 g product per kg of adsorbent per hour with an unprecedented 99.7% purity. In situ solvent recovery was realized with a solvent-resistant nanofiltration membrane allowing 97.5% solvent recycle and 44.5% total carbon footprint reduction, while concentrating both the product stream for crystallisation and the waste stream for disposal.