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Experimental evidence for excess entropy discontinuities in glass-forming solutions

Lienhard, Daniel M. and Zobrist, Bernhard and Zuend, Andreas and Krieger, Ulrich K. and Peter, Thomas (2012) Experimental evidence for excess entropy discontinuities in glass-forming solutions. Journal of Chemical Physics, 136 (7). Art. No. 074515. ISSN 0021-9606. https://resolver.caltech.edu/CaltechAUTHORS:20120403-103055518

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Abstract

Glass transition temperatures T_g are investigated in aqueous binary and multi-component solutions consisting of citric acid, calcium nitrate (Ca(NO_3)_2), malonic acid, raffinose, and ammonium bisulfate (NH_4HSO_4) using a differential scanning calorimeter. Based on measured glass transition temperatures of binary aqueous mixtures and fitted binary coefficients, the T_g of multi-component systems can be predicted using mixing rules. However, the experimentally observed T_g in multi-component solutions show considerable deviations from two theoretical approaches considered. The deviations from these predictions are explained in terms of the molar excess mixing entropy difference between the supercooled liquid and glassy state at T_g. The multi-component mixtures involve contributions to these excess mixing entropies that the mixing rules do not take into account.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1063/1.3685902 DOIArticle
http://jcp.aip.org/resource/1/jcpsa6/v136/i7/p074515_s1PublisherArticle
ORCID:
AuthorORCID
Zuend, Andreas0000-0003-3101-8521
Additional Information:© 2012 American Institute of Physics. Received 20 September 2011; accepted 31 January 2012; published online 21 February 2012. This research was supported by the European Commission through the EC Integrated Projects SCOUT-O3 (505390-GOCE-CT-2004) and the ETH Research Grant ETH-0210-1.
Funders:
Funding AgencyGrant Number
European Commission EC Integrated Projects SCOUT-O3505390-GOCE-CT-2004
ETH ZurichETH-0210-1
Subject Keywords:ammonium compounds, calcium compounds, differential scanning calorimetry, entropy, glass transition, organic compounds, solutions, vitrification
Issue or Number:7
Classification Code:PACS: 65.20.Jk; 64.70.pm; 82.60.Lf
Record Number:CaltechAUTHORS:20120403-103055518
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20120403-103055518
Official Citation:Experimental evidence for excess entropy discontinuities in glass-forming solutions Daniel M. Lienhard, Bernhard Zobrist, Andreas Zuend, Ulrich K. Krieger, and Thomas Peter J. Chem. Phys. 136, 074515 (2012); http://dx.doi.org/10.1063/1.3685902 (9 pages) Online Publication Date: 21 February 2012
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:29954
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:03 Apr 2012 18:07
Last Modified:03 Oct 2019 03:46

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