Studying the impact of the pre-exponential factor on templated nucleation
OA Location
Author(s)
Verma, Vivek
Mitchell, Hamish
Guo, Mingxia
Hodnett, Benjamin K
Heng, Jerry YY
Type
Journal Article
Abstract
Traditionally, the enhancement of nucleation rates in the presence of heterogeneous surfaces in crystallisation processes has been attributed to the modification of the interfacial energy of the system according to the classical nucleation theory. However, recent developments have shown that heterogeneous surfaces instead alter the pre-exponential factor of nucleation. In this work, the nucleation kinetics of glycine and diglycine in aqueous solutions have been explored in the presence and absence of a heterogeneous surface. Results from induction time experiments show that the presence of a heterogeneous surface increases the pre-exponential factor by 2-fold or more for both glycine and diglycine, while the interfacial energy remains unchanged for both species. This study suggests that the heterogeneous surface enhances the nucleation rate via hydrogen bond formation with both glycine and diglycine. This is verified by hydrogen bond propensity calculations, molecular functionality analysis, and calculation of the time taken for a solute molecule to attach to the growing nucleus, which is an order of magnitude shorter than the estimated lifetime of the hydrogen bond. The effect of the heterosurface is of greater magnitude for diglycine than for glycine, which may be due to the heightened molecular complementarity between the hydrogen bond donor and acceptor sites on diglycine and the heterosurface.
Date Issued
2022-07-01
Date Acceptance
2021-12-13
Citation
Faraday Discussions, 2022, 235, pp.199-218
ISSN
1359-6640
Publisher
Royal Society of Chemistry
Start Page
199
End Page
218
Journal / Book Title
Faraday Discussions
Volume
235
Copyright Statement
This journal is © The Royal Society of Chemistry 2022. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
License URL
Sponsor
Engineering & Physical Science Research Council (EPSRC)
Engineering & Physical Science Research Council (EPSRC)
Identifier
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000779730600001&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=a2bf6146997ec60c407a63945d4e92bb
Grant Number
EP/N015916/1
EP/T005556/1
Subjects
ALPHA-GLYCYLGLYCINE
Chemistry
Chemistry, Physical
CRYSTAL NUCLEATION
DESIGN
GAMMA-GLYCINE
GLYCINE NUCLEATION
GROWTH
HETEROGENEOUS NUCLEATION
PHASE
Physical Sciences
Science & Technology
SELECTIVE CRYSTALLIZATION
SURFACE-CHEMISTRY
Publication Status
Published
Date Publish Online
2021-12-13