Correlations between adhesion and molecular interactions at buried interfaces of model polymer systems and in commercial multilayer barrier films

Daniel Rossi; Yuchen Wu; Yifan Dong; Rajesh Paradkar; Xiaoyun Chen; Tzu-Chi Kuo; Zhan Chen

doi:10.1063/5.0232449

Correlations between adhesion and molecular interactions at buried interfaces of model polymer systems and in commercial multilayer barrier films

J Chem Phys. 2024 Sep 28;161(12):124710. doi: 10.1063/5.0232449.

Authors

Daniel Rossi¹, Yuchen Wu^{1

2}, Yifan Dong³, Rajesh Paradkar³, Xiaoyun Chen⁴, Tzu-Chi Kuo⁴, Zhan Chen^{1

2}

Affiliations

¹ Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, USA.
² Department of Macromolecular Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109, USA.
³ Packaging and Specialty Plastics, The Dow Chemical Company, Lake Jackson, Texas 77566, USA.
⁴ Core R&D, The Dow Chemical Company, Midland, Michigan 48674, USA.

PMID: 39324534
DOI: 10.1063/5.0232449

Abstract

Sum frequency generation vibrational spectroscopy (SFG) was applied to characterize the interfacial adhesion chemistry at several buried polymer interfaces in both model systems and blown multilayer films. Anhydride/acid modified polyolefins are used as tie layers to bond dissimilar polymers in multilayer barrier structures. In these films, the interfacial reactions between the barrier polymers, such as ethylene vinyl alcohol (EVOH) or nylon, and the grafted anhydrides/acids provide covalent linkages that enhance adhesion. However, the bonding strengths vary for different polymer-tie layer combinations. Here, using SFG, we aim to provide a systematic study on four common polymer-tie interfaces, including EVOH/polypropylene-tie, EVOH/polyethylene-tie, nylon/polypropylene-tie, and nylon/polyethylene-tie, to understand how the adhesion chemistry varies and its impact on the measured adhesion. Our SFG studies suggest that adhesion enhancement is driven by a combination of reaction kinetics and the interfacial enrichment of the anhydride/acid, resulting in stronger adhesion in the case of nylon. This observation matches well with the higher adhesion observed in the nylon/tie systems in both lap shear and peel test measurements. In addition, in the polypropylene-tie systems, grafted oligomers due to chain scission may migrate to the interface, affecting the adhesion. These by-products can react or interfere with the barrier-tie chemistry, resulting in reduced adhesion strength in the polypropylene-tie system.