Early Stages of Crystallization of Calcium Carbonate Revealed in Picoliter Droplets

In this work, we studied the heterogeneous nucleation and growth of CaCO3 within regular arrays of picoliter droplets created on patterned self-assembled monolayers (SAMs). The SAMs provide well-defined substrates that offer control over CaCO3 nucleation, and we used these impurity-free droplet arra...

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Published inJournal of the American Chemical Society Vol. 133; no. 14; pp. 5210 - 5213
Main Authors Stephens, Christopher J, Kim, Yi-Yeoun, Evans, Stephen D, Meldrum, Fiona C, Christenson, Hugo K
Format Journal Article
LanguageEnglish
Published United States American Chemical Society 13.04.2011
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Abstract In this work, we studied the heterogeneous nucleation and growth of CaCO3 within regular arrays of picoliter droplets created on patterned self-assembled monolayers (SAMs). The SAMs provide well-defined substrates that offer control over CaCO3 nucleation, and we used these impurity-free droplet arrays to study crystal growth in spatially and chemically controlled, finite-reservoir environments. The results demonstrate a number of remarkable features of precipitation within these confined volumes. CaCO3 crystallization proceeds significantly more slowly in the droplets than in the bulk, allowing the mechanism of crystallization, which progresses via amorphous calcium carbonate, to be easily observed. In addition, the precipitation reaction terminates at an earlier stage than in the bulk solution, revealing intermediate growth forms. Confinement can therefore be used as a straightforward method for studying the mechanisms of crystallization on a substrate without the requirement for specialized analytical techniques. The results are also of significance to biomineralization processes, where crystallization typically occurs in confinement and in association with organic matrices, and it is envisaged that the method is applicable to many crystallizing systems.
AbstractList In this work, we studied the heterogeneous nucleation and growth of CaCO(3) within regular arrays of picoliter droplets created on patterned self-assembled monolayers (SAMs). The SAMs provide well-defined substrates that offer control over CaCO(3) nucleation, and we used these impurity-free droplet arrays to study crystal growth in spatially and chemically controlled, finite-reservoir environments. The results demonstrate a number of remarkable features of precipitation within these confined volumes. CaCO(3) crystallization proceeds significantly more slowly in the droplets than in the bulk, allowing the mechanism of crystallization, which progresses via amorphous calcium carbonate, to be easily observed. In addition, the precipitation reaction terminates at an earlier stage than in the bulk solution, revealing intermediate growth forms. Confinement can therefore be used as a straightforward method for studying the mechanisms of crystallization on a substrate without the requirement for specialized analytical techniques. The results are also of significance to biomineralization processes, where crystallization typically occurs in confinement and in association with organic matrices, and it is envisaged that the method is applicable to many crystallizing systems.
In this work, we studied the heterogeneous nucleation and growth of CaCO3 within regular arrays of picoliter droplets created on patterned self-assembled monolayers (SAMs). The SAMs provide well-defined substrates that offer control over CaCO3 nucleation, and we used these impurity-free droplet arrays to study crystal growth in spatially and chemically controlled, finite-reservoir environments. The results demonstrate a number of remarkable features of precipitation within these confined volumes. CaCO3 crystallization proceeds significantly more slowly in the droplets than in the bulk, allowing the mechanism of crystallization, which progresses via amorphous calcium carbonate, to be easily observed. In addition, the precipitation reaction terminates at an earlier stage than in the bulk solution, revealing intermediate growth forms. Confinement can therefore be used as a straightforward method for studying the mechanisms of crystallization on a substrate without the requirement for specialized analytical techniques. The results are also of significance to biomineralization processes, where crystallization typically occurs in confinement and in association with organic matrices, and it is envisaged that the method is applicable to many crystallizing systems.
Author Christenson, Hugo K
Kim, Yi-Yeoun
Evans, Stephen D
Stephens, Christopher J
Meldrum, Fiona C
AuthorAffiliation University of Leeds
School of Physics and Astronomy
School of Chemistry
AuthorAffiliation_xml – name:
– name: School of Physics and Astronomy
– name: University of Leeds
– name: School of Chemistry
Author_xml – sequence: 1
  givenname: Christopher J
  surname: Stephens
  fullname: Stephens, Christopher J
– sequence: 2
  givenname: Yi-Yeoun
  surname: Kim
  fullname: Kim, Yi-Yeoun
– sequence: 3
  givenname: Stephen D
  surname: Evans
  fullname: Evans, Stephen D
– sequence: 4
  givenname: Fiona C
  surname: Meldrum
  fullname: Meldrum, Fiona C
  email: f.meldrum@leeds.ac.uk, h.k.christenson@leeds.ac.uk
– sequence: 5
  givenname: Hugo K
  surname: Christenson
  fullname: Christenson, Hugo K
  email: f.meldrum@leeds.ac.uk, h.k.christenson@leeds.ac.uk
BackLink https://www.ncbi.nlm.nih.gov/pubmed/21425847$$D View this record in MEDLINE/PubMed
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– volume: 12
  start-page: 538
  year: 1996
  ident: ref24/cit24
  publication-title: Langmuir
  doi: 10.1021/la950330a
  contributor:
    fullname: Archibald D. D.
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Snippet In this work, we studied the heterogeneous nucleation and growth of CaCO3 within regular arrays of picoliter droplets created on patterned self-assembled...
In this work, we studied the heterogeneous nucleation and growth of CaCO(3) within regular arrays of picoliter droplets created on patterned self-assembled...
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SubjectTerms Calcium Carbonate - chemistry
Chemical Precipitation
Crystallization - instrumentation
Crystallization - methods
Title Early Stages of Crystallization of Calcium Carbonate Revealed in Picoliter Droplets
URI http://dx.doi.org/10.1021/ja200309m
https://www.ncbi.nlm.nih.gov/pubmed/21425847
https://search.proquest.com/docview/860877959
Volume 133
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