Thermodynamic Properties of Crystalline Cellulose Allomorphs Studied with Dispersion-Corrected Density Functional Methods

Thumbnail Image

Access rights

openAccess

URL

Journal Title

Journal ISSN

Volume Title

A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä

Date

2022-10

Major/Subject

Mcode

Degree programme

Language

en

Pages

11

Series

Molecules, Volume 27, issue 19

Abstract

The phonon properties and thermodynamics of four crystalline cellulose allomorphs, I (Formula presented.), I (Formula presented.), II, and III (Formula presented.), have been investigated using dispersion-corrected density functional theory (DFT). In line with experimental findings, the free energy differences between the studied cellulose allomorphs are small, less than 1 kJ/mol per atom. The calculated specific heat at constant volume ((Formula presented.)) has been compared with the available experimental data in the temperature range 10–300 K. Quasiharmonic approximation has been employed to study thermodynamics and specific heat at constant pressure ((Formula presented.)). For the studied temperature range of 10–400 K, the specific heat of all cellulose allomorphs shows very similar behavior. The calculated and experimental specific heat agree well at low temperatures below 100 K, but the deviation between theory and experiment increases with temperature. This may be due to increasing phonon anharmonicity as the temperature increases.

Description

Publisher Copyright: © 2022 by the authors.

Keywords

cellulose, density functional theory, phonon properties, quantum chemical calculations, quasiharmonic approximation, thermodynamics

Other note

Citation

Srivastava , D , Ahopelto , J & Karttunen , A J 2022 , ' Thermodynamic Properties of Crystalline Cellulose Allomorphs Studied with Dispersion-Corrected Density Functional Methods ' , Molecules , vol. 27 , no. 19 , 6240 . https://doi.org/10.3390/molecules27196240