Al-Catam

A family of aluminium catecholate-amine catalysts for fast, controlled, and highly selective ring-opening polymerisation

The Al-catam catalysts are our family of aluminium complexes built on catecholate-amine (catam) ligands, developed for the ring-opening polymerisation (ROP) of cyclic esters, such as lactide and ε-caprolactone.

Across three studies, this project has progressively built up a mechanistic picture of this catalyst family: from first demonstrating exceptional room-temperature activity for lactide ROP, to uncovering the role of non-covalent interactions in the catalytic pocket, to using chirality itself as a design handle to control catalyst aggregation and unlock even higher rates.

The group has a broad interest in catalyst design. We adopt a complementary experimental and computational approach to gain a better understanding of these systems and to guide the development of the next generation of polymerisation catalysts. Our holistic approach involves organic ligand and metal complex synthesis and characterisation, mechanistic studies (including structure–activity and kinetic studies), polymer synthesis and characterisation, and overarching computational studies.

Publications

  1. Gesslbauer, S.; Cheek, H.; White, A. J. P.; Romain, C. Highly active aluminium catalysts for room temperature ring-opening polymerisation of rac-lactide. Dalton Trans. 2018, 47, 10410–10414. 10.1039/C8DT01526K
  2. Gesslbauer, S.; Savela, R.; Chen, Y.; White, A. J. P.; Romain, C. Exploiting Noncovalent Interactions for Room-Temperature Heteroselective rac-Lactide Polymerization Using Aluminum Catalysts. ACS Catal. 2019, 9, 7912–7920. 10.1021/acscatal.9b00875
  3. Gesslbauer, S.; Hutchinson, G.; White, A. J. P.; Burés, J.; Romain, C. Chirality-Induced Catalyst Aggregation: Insights into Catalyst Speciation and Activity Using Chiral Aluminum Catalysts in Cyclic Ester Ring-Opening Polymerization. ACS Catal. 2021, 11, 4084–4093. 10.1021/acscatal.0c05245