Nanoscale Stabilization Mechanism of Sodium Sulfate Decahydrate at Polyelectrolyte Interfaces

Damilola O. Akamo; Bernadette Cladek; Monojoy Goswami; Kyle R. Gluesenkamp; Orlando Rios; David J. Keffer

doi:10.1021/acsomega.3c09796

Nanoscale Stabilization Mechanism of Sodium Sulfate Decahydrate at Polyelectrolyte Interfaces

Damilola O. Akamo
, Bernadette Cladek
, Monojoy Goswami
, Kyle R. Gluesenkamp
, Orlando Rios
, David J. Keffer

Research output: Contribution to journal › Article › peer-review

2 Scopus citations

Abstract

Sodium sulfate decahydrate (SSD) is a low-cost phase-change material (PCM) for thermal energy storage applications that offers substantial melting enthalpy and a suitable temperature range for near-ambient applications. However, SSD’s consistent phase separation with decreased melting enthalpy over repeated thermal cycles limits its application as a PCM. Sulfonated polyelectrolytes, such as dextran sulfate sodium (DSS), have shown great effectiveness in preventing phase separation in SSD. However, there is limited understanding of the stabilization mechanism of SSD by DSS at the atomic length and time scales. In this work, we investigate SSD stabilization via DSS using neutron scattering and molecular dynamics (MD) simulations. Neutron scattering and pair distribution function analysis revealed the structural evolution of the PCM samples below and above the phase change temperatures. MD simulations revealed that water from the hydrate structure migrates from the hydrate crystal to the SSD-DSS interfacial region upon melting. The water is stabilized at this interface by aggregation around the hydrophilic sulfonic acid groups attached to the backbone of the polyelectrolyte. This architecture retains water near the dehydrated sodium sulfate, preventing phase separation and, consequently, stabilizing SSD rehydration. This work provides atomistic insight into selecting and designing stable and high-performance PCMs for heating and cooling applications in building technologies.

Original language	English
Pages (from-to)	18051-18061
Number of pages	11
Journal	ACS Omega
Volume	9
Issue number	16
DOIs	https://doi.org/10.1021/acsomega.3c09796
State	Published - Apr 23 2024

Funding

This work was sponsored by the U.S. Department of Energy’s (DOE) Building Technologies Office under contract no. DE-AC05-00OR22725 with UT-Battelle, LLC. The authors would like to acknowledge Sven Mumme from the U.S. Department of Energy Building Technologies Office. This research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The computational resources for this research were provided by the Infrastructure for Scientific Applications and Advanced Computing (ISAAC) at the University of Tennessee, Knoxville. Part of the MD simulations used resources of the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Scientific User Facility supported by the DOE Office of Science under contract no. DE-AC02- 05CH11231.

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title = "Nanoscale Stabilization Mechanism of Sodium Sulfate Decahydrate at Polyelectrolyte Interfaces",

abstract = "Sodium sulfate decahydrate (SSD) is a low-cost phase-change material (PCM) for thermal energy storage applications that offers substantial melting enthalpy and a suitable temperature range for near-ambient applications. However, SSD{\textquoteright}s consistent phase separation with decreased melting enthalpy over repeated thermal cycles limits its application as a PCM. Sulfonated polyelectrolytes, such as dextran sulfate sodium (DSS), have shown great effectiveness in preventing phase separation in SSD. However, there is limited understanding of the stabilization mechanism of SSD by DSS at the atomic length and time scales. In this work, we investigate SSD stabilization via DSS using neutron scattering and molecular dynamics (MD) simulations. Neutron scattering and pair distribution function analysis revealed the structural evolution of the PCM samples below and above the phase change temperatures. MD simulations revealed that water from the hydrate structure migrates from the hydrate crystal to the SSD-DSS interfacial region upon melting. The water is stabilized at this interface by aggregation around the hydrophilic sulfonic acid groups attached to the backbone of the polyelectrolyte. This architecture retains water near the dehydrated sodium sulfate, preventing phase separation and, consequently, stabilizing SSD rehydration. This work provides atomistic insight into selecting and designing stable and high-performance PCMs for heating and cooling applications in building technologies.",

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AU - Gluesenkamp, Kyle R.

AU - Rios, Orlando

AU - Keffer, David J.

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N2 - Sodium sulfate decahydrate (SSD) is a low-cost phase-change material (PCM) for thermal energy storage applications that offers substantial melting enthalpy and a suitable temperature range for near-ambient applications. However, SSD’s consistent phase separation with decreased melting enthalpy over repeated thermal cycles limits its application as a PCM. Sulfonated polyelectrolytes, such as dextran sulfate sodium (DSS), have shown great effectiveness in preventing phase separation in SSD. However, there is limited understanding of the stabilization mechanism of SSD by DSS at the atomic length and time scales. In this work, we investigate SSD stabilization via DSS using neutron scattering and molecular dynamics (MD) simulations. Neutron scattering and pair distribution function analysis revealed the structural evolution of the PCM samples below and above the phase change temperatures. MD simulations revealed that water from the hydrate structure migrates from the hydrate crystal to the SSD-DSS interfacial region upon melting. The water is stabilized at this interface by aggregation around the hydrophilic sulfonic acid groups attached to the backbone of the polyelectrolyte. This architecture retains water near the dehydrated sodium sulfate, preventing phase separation and, consequently, stabilizing SSD rehydration. This work provides atomistic insight into selecting and designing stable and high-performance PCMs for heating and cooling applications in building technologies.

AB - Sodium sulfate decahydrate (SSD) is a low-cost phase-change material (PCM) for thermal energy storage applications that offers substantial melting enthalpy and a suitable temperature range for near-ambient applications. However, SSD’s consistent phase separation with decreased melting enthalpy over repeated thermal cycles limits its application as a PCM. Sulfonated polyelectrolytes, such as dextran sulfate sodium (DSS), have shown great effectiveness in preventing phase separation in SSD. However, there is limited understanding of the stabilization mechanism of SSD by DSS at the atomic length and time scales. In this work, we investigate SSD stabilization via DSS using neutron scattering and molecular dynamics (MD) simulations. Neutron scattering and pair distribution function analysis revealed the structural evolution of the PCM samples below and above the phase change temperatures. MD simulations revealed that water from the hydrate structure migrates from the hydrate crystal to the SSD-DSS interfacial region upon melting. The water is stabilized at this interface by aggregation around the hydrophilic sulfonic acid groups attached to the backbone of the polyelectrolyte. This architecture retains water near the dehydrated sodium sulfate, preventing phase separation and, consequently, stabilizing SSD rehydration. This work provides atomistic insight into selecting and designing stable and high-performance PCMs for heating and cooling applications in building technologies.

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Nanoscale Stabilization Mechanism of Sodium Sulfate Decahydrate at Polyelectrolyte Interfaces

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