Over the past two decades, a branch of organic chemistry has emerged that breaks with the paradigm of synthesizing pure compounds and focusses instead on complex (macro)molecular networks akin to those found in nature. In this proposed project, we aim to address unmet challenges in supramolecular chemistry and systems chemistry by developing original dynamic reaction networks whose building blocks are capable of supramolecular (self-)recognition. The first two objectives of SUPRANET focus on the use of dynamic covalent orthoester networks for the discovery of anion, cation and ion pair receptors, whose unique properties may pave the way towards the utilization of inorganic ions as drugs. For instance, we will develop self-assembled ion pair cages for the electro-neutral transport of medicinally relevant anions across phospholipid membranes. Our network approach will also allow us to “imprison” ionic guests for the first time in self-assembled receptors that could be used for the transport and controlled release of ions, even against osmotic pressure. Objectives three and four of SUPRANET go beyond the equilibrium state and, as such, are relevant to the chemistry of life, in which key processes depend on dissipative steady states. The proposed reaction networks will feature biologically relevant ribose building blocks that are continuously assembled and disassembled by two different irreversible reactions, resulting in steady state mixtures of either RNA oligomers or ribose-derived vesicles. It is our hope that these studies will provide insights into open questions regarding the molecular origins of life, such as the non-enzymatic formation of RNA oligomers capable of self-recognition and the simultaneous emergence of compartmentalization and self-replication. SUPRANET thus seeks to break new ground in both equilibrium and far-from-equilibrium dynamic networks and is equally motivated by applied and fundamental challenges.

Next-generation energy storage solutions are needed to satisfy the increasing demand for electrically powered devices. Organic electrode materials (OEMs) are promising candidates, constituted of widely available elements, accessible in processes with low CO2 footprint and easily recycled. However, existing OEMs suffer from a lack of porosity, which inhibits counter ion diffusion to the electroactive sites or renders redox processes irreversible, severely limiting their performance. NanOBatt explores a fundamentally new concept for OEMs in order to significantly improve their intrinsic porosity and provide pathways for efficient counter ion diffusion. In NanOBatt I and my team will investigate redox-active conjugated nanohoops and macrocycles with intrinsic porosity as OEMs in next-generation batteries: Redox-active groups can be installed with the desired properties, their extended conjugation and aromaticity stabilize charges, and their rigid 3D shapes and nanometer-sized cavities lead to nanoporous structures, ideally suited to enable fast counter ion diffusion. In spite of these outstanding properties, conjugated nanohoops have not been explored as OEMs, and even macrocycles have received only little attention as such. The aims of NanOBatt are to develop synthetic strategies and design guidelines for redox-active conjugated nanohoops and macrocycles as OEMs, elucidate the role of conjugation and porosity on charge stabilization and ion diffusion in their charge/discharge processes and investigate their application as OEMs in alternative battery cell configurations, namely Na, Al, Mg and all-organic batteries. NanOBatt uniquely bridges the gap between fundamental research on organic materials and their application in next-generation charge storage devices. With NanOBatt I will initiate a new research field with ground-breaking impact, both in the scientific community as well as for the future direction of my own research.