PMID- 35921684
OWN - NLM
STAT- PubMed-not-MEDLINE
LR  - 20220818
IS  - 1520-5207 (Electronic)
IS  - 1520-5207 (Linking)
VI  - 126
IP  - 32
DP  - 2022 Aug 18
TI  - Atomistic Modeling of Hydrogen and Oxygen Solubility in Semicrystalline PA-6 and 
      HDPE Materials.
PG  - 6102-6111
LID - 10.1021/acs.jpcb.2c02854 [doi]
AB  - Hydrogen is a clean and sustainable energy carrier which plays a major role in 
      the transition of the global energy market to a less fossil fuel dependent 
      future. Polymer-based materials are crucial in the production, storage, 
      transportation, and energy extraction of hydrogen. More insights in the 
      hydrogen-polymers interactions are required to guide material design and product 
      development, especially for hydrogen solubility in polymers, which is crucial in 
      many applications. The current study aims at rationalizing the determining 
      factors of hydrogen solubility in two relevant polymers: polyamide-6 (PA-6) and 
      high density polyethylene (HDPE). Based on atomistic molecular dynamics 
      simulations and experimental data, we have reached several conclusions related to 
      hydrogen and oxygen solubility in these two polymers. The crystal phases of PA-6 
      and HDPE are impenetrable to hydrogen and oxygen at elevated pressures, despite 
      the small molecular size of hydrogen and oxygen. The practical implication for 
      gas barrier applications is that polymer crystals act as impermeable obstacles 
      and gas migration takes place primarily in the amorphous phase. Experimental 
      hydrogen and oxygen solubilities in PA-6 and HDPE at elevated pressures can be 
      predicted in a semiquantitative manner by molecular simulations. The 
      discrepancies between experimental and predicted values could be attributed to 
      neglect of the effect of crystal regions on the amorphous polymer domains. 
      Although hydrogen is smaller than oxygen, it has been experimentally observed 
      that hydrogen has a lower solubility in PA-6 and HDPE than oxygen. This 
      observation has been confirmed by molecular simulations and attributed to the 
      more favorable energetic interactions of oxygen with PA-6 and PE than of 
      hydrogen. These interactions dominate the solubility behavior over the 
      distribution of the accessible volume in the polymers.
FAU - Voyiatzis, Evangelos
AU  - Voyiatzis E
AUID- ORCID: 0000-0001-8753-8134
AD  - DSM Applied Science Center, P.O. Box 1066, 6160 BB Geleen, The Netherlands.
FAU - Stroeks, Alexander
AU  - Stroeks A
AUID- ORCID: 0000-0002-2167-4245
AD  - DSM Engineering Materials, Urmonderbaan 22, 6167 RD Geleen, The Netherlands.
LA  - eng
PT  - Journal Article
DEP - 20220803
PL  - United States
TA  - J Phys Chem B
JT  - The journal of physical chemistry. B
JID - 101157530
SB  - IM
EDAT- 2022/08/04 06:00
MHDA- 2022/08/04 06:01
CRDT- 2022/08/03 17:52
PHST- 2022/08/04 06:00 [pubmed]
PHST- 2022/08/04 06:01 [medline]
PHST- 2022/08/03 17:52 [entrez]
AID - 10.1021/acs.jpcb.2c02854 [doi]
PST - ppublish
SO  - J Phys Chem B. 2022 Aug 18;126(32):6102-6111. doi: 10.1021/acs.jpcb.2c02854. Epub 
      2022 Aug 3.