Uncovering the Role of Bicarbonate in Calcium Carbonate Formation at Near-Neutral pH

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2021
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Huang, Shing-Jong
Chang, Chun-Yu
Drechsler, Markus
Chan, Jerry Chun Chung
Raiteri, Paolo
Gale, Julian D
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Angewandte Chemie International Edition. Wiley. 2021, 60(30), pp. 16707-16713. ISSN 1433-7851. eISSN 1521-3773. Available under: doi: 10.1002/anie.202104002
Zusammenfassung

Mechanistic pathways relevant to mineralization are not well-understood fundamentally, let alone in the context of their biological and geological environments. Through quantitative analysis of ion association at near-neutral pH, we identify the involvement of HCO3 - ions in CaCO3 nucleation. Incorporation of HCO3 - ions into the structure of amorphous intermediates is corroborated by solid-state nuclear magnetic resonance spectroscopy, complemented by quantum mechanical calculations and molecular dynamics simulations. We identify the roles of HCO3 - ions as being through (i) competition for ion association during the formation of ion pairs and ion clusters prior to nucleation and (ii) incorporation as a significant structural component of amorphous mineral particles. The roles of HCO3 - ions as active soluble species and structural constituents in CaCO3 formation are of fundamental importance and provide a basis for a better understanding of physiological and geological mineralization.

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ISO 690HUANG, Yu-Chieh, Ashit RAO, Shing-Jong HUANG, Chun-Yu CHANG, Markus DRECHSLER, Jennifer KNAUS, Jerry Chun Chung CHAN, Paolo RAITERI, Julian D GALE, Denis GEBAUER, 2021. Uncovering the Role of Bicarbonate in Calcium Carbonate Formation at Near-Neutral pH. In: Angewandte Chemie International Edition. Wiley. 2021, 60(30), pp. 16707-16713. ISSN 1433-7851. eISSN 1521-3773. Available under: doi: 10.1002/anie.202104002
BibTex
@article{Huang2021-07-19Uncov-54194,
  year={2021},
  doi={10.1002/anie.202104002},
  title={Uncovering the Role of Bicarbonate in Calcium Carbonate Formation at Near-Neutral pH},
  number={30},
  volume={60},
  issn={1433-7851},
  journal={Angewandte Chemie International Edition},
  pages={16707--16713},
  author={Huang, Yu-Chieh and Rao, Ashit and Huang, Shing-Jong and Chang, Chun-Yu and Drechsler, Markus and Knaus, Jennifer and Chan, Jerry Chun Chung and Raiteri, Paolo and Gale, Julian D and Gebauer, Denis}
}
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    <dcterms:abstract xml:lang="eng">Mechanistic pathways relevant to mineralization are not well-understood fundamentally, let alone in the context of their biological and geological environments. Through quantitative analysis of ion association at near-neutral pH, we identify the involvement of HCO&lt;sub&gt;3&lt;/sub&gt; &lt;sup&gt;-&lt;/sup&gt; ions in CaCO&lt;sub&gt;3&lt;/sub&gt; nucleation. Incorporation of HCO&lt;sub&gt;3&lt;/sub&gt;&lt;sup&gt; -&lt;/sup&gt; ions into the structure of amorphous intermediates is corroborated by solid-state nuclear magnetic resonance spectroscopy, complemented by quantum mechanical calculations and molecular dynamics simulations. We identify the roles of HCO&lt;sub&gt;3&lt;/sub&gt; &lt;sup&gt;-&lt;/sup&gt; ions as being through (i) competition for ion association during the formation of ion pairs and ion clusters prior to nucleation and (ii) incorporation as a significant structural component of amorphous mineral particles. The roles of HCO&lt;sub&gt;3 &lt;/sub&gt;&lt;sup&gt;-&lt;/sup&gt; ions as active soluble species and structural constituents in CaCO&lt;sub&gt;3&lt;/sub&gt; formation are of fundamental importance and provide a basis for a better understanding of physiological and geological mineralization.</dcterms:abstract>
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