DFT study of mechanisms possible for the ring-opening of L-Lactide catalysed by a Zirconium-based liquid formulation and initiated by benzyl alcohol

Data to support article: A Highly Active and Selective Zirconium-based Catalyst System for the Industrial Production of Poly(lactic acid) Journal: ACS Catalysis, 2023, 13, 4, 2681–2695 DOI: 10.1021/acscatal.2c05690 Authors: Antoine Buchard,1,2 Christopher J. Chuck,1,3 Matthew G. Davidson,1,2* Gerrit Gobius du Sart,4 Matthew D. Jones,1,2 Strachan N. McCormick1,2* and Andrew D. Russell2 1 Centre for Sustainable and Circular Technologies, University of Bath, Bath BA2 7AY, UK. 2 Department of Chemistry, University of Bath. 3 Department of Chemical Engineering, University of Bath. 4 TotalEnergies Corbion PLA, Arkelsedijk 46, 4206 AC Gorinchem, The Netherlands *Email: [e-mail]; [e-mail] For DFT inquiries: [e-mail] Description: DFT optimised geometries and computed free enthalpies of local minima (intermediates) and local maxima (transition states) were used to investigate the mechanism of the ring-opening of L-Lactide catalysed by a Zirconium-based liquid formulation and initiated by benzyl alcohol Protocols: Gaussian09 (rev D.01) software Functionals tested: PBE0-D3; wB97XD; M06-D3 Solvent model: cpcm=(ethylacetate); temperature=453.15K Basis sets: 6-311+g(d) for N and O atoms, 6-311++g(d,p) for H from NH and OH groups, 6-31g(d) for all C and H atoms, except CH3 groups on aromatic rings (STO-3G)), Zr: SDD ECP and basis set Content: - Gaussian09 rev D.01 output files - DFT Mechanism.pdf, illustrating the calculations made and summarising the free enthalpies computed