Molecular dynamics investigation of clustering in aqueous glycine solutions

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Sweatman, Martin B. and Afify, Nasser D. and Ferreiro-Rangel, Carlos A. and Jorge, Miguel and Sefcik, Jan (2022) Molecular dynamics investigation of clustering in aqueous glycine solutions. Journal of Physical Chemistry B, 126 (25). pp. 4711-4722. ISSN 1520-6106 (https://doi.org/10.1021/acs.jpcb.2c01975)

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Abstract

Recent experiments with undersaturated aqueous glycine solutions have repeatedly exhibited the presence of giant liquid-like clusters or nanodroplets around 100 nm in diameter. These nanodroplets re-appear even after careful efforts for their removal and purification of the glycine solution. The composition of these clusters is not clear, although it has been suggested that they are mainly composed of glycine, a small and very soluble amino acid. To gain insights into this phenomenon, we study the aggregation of glycine in aqueous solutions at concentrations below the experimental solubility limit using large-scale molecular dynamics simulations under ambient conditions. Three protonation states of glycine (zwitterion = GLZ, anion = GLA, and cation = GLC) are simulated using molecular force fields based on the 1.14*CM1A partial charge scheme, which incorporates the OPLS all-atom force field and TIP3P water. When initiated from dispersed states, we find that giant clusters do not form in our simulations unless salt impurities are present. Moreover, if simulations are initiated from giant cluster states, we find that they tend to dissolve in the absence of salt impurities. Therefore, the simulation results provide little support for the possibility that the giant clusters seen in experiments are composed purely of glycine (and water). Considering that strenuous efforts are made in experiments to remove impurities such as salt, we propose that the giant clusters observed might instead result from the aggregation of reaction products of aqueous glycine, such as diketopiperazine or other oligoglycines which may be difficult to separate from glycine using conventional methods, or their co-aggregation with glycine.

ORCID iDs

Sweatman, Martin B., Afify, Nasser D., Ferreiro-Rangel, Carlos A., Jorge, Miguel ORCID logoORCID: https://orcid.org/0000-0003-3009-4725 and Sefcik, Jan ORCID logoORCID: https://orcid.org/0000-0002-7181-5122;
CORE (COnnecting REpositories)