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Quantitative plane-resolved crystal growth and dissolution kinetics by coupling in situ optical microscopy and diffusion models : the case of salicylic acid in aqueous solution
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Perry, Amelia R., Peruffo, Massimo and Unwin, Patrick R. (2013) Quantitative plane-resolved crystal growth and dissolution kinetics by coupling in situ optical microscopy and diffusion models : the case of salicylic acid in aqueous solution. Crystal Growth & Design, Volume 13 (Number 2). pp. 614-622. doi:10.1021/cg301282q
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WRAP_Perry, Crystal Growth and Design, 2013.pdf - Accepted Version Download (5Mb) | Preview |
Official URL: http://dx.doi.org/10.1021/cg301282q
Abstract
The growth and dissolution kinetics of salicylic acid crystals are investigated in situ by focusing on individual microscale crystals. From a combination of optical microscopy and finite element method (FEM) modeling, it was possible to obtain a detailed quantitative picture of dissolution and growth dynamics for individual crystal faces. The approach uses real-time in situ growth and dissolution data (crystal size and shape as a function of time) to parametrize a FEM model incorporating surface kinetics and bulk to surface diffusion, from which concentration distributions and fluxes are obtained directly. It was found that the (001) face showed strong mass transport (diffusion) controlled behavior with an average surface concentration close to the solubility value during growth and dissolution over a wide range of bulk saturation levels. The (1̅10) and (110) faces exhibited mixed mass transport/surface controlled behavior, but with a strong diffusive component. As crystals became relatively large, they tended to exhibit peculiar hollow structures in the end (001) face, observed by interferometry and optical microscopy. Such features have been reported in a number of crystals, but there has not been a satisfactory explanation for their origin. The mass transport simulations indicate that there is a large difference in flux across the crystal surface, with high values at the edge of the (001) face compared to the center, and this flux has to be redistributed across the (001) surface. As the crystal grows, the redistribution process evidently can not be maintained so that the edges grow at the expense of the center, ultimately creating high index internal structures. At later times, we postulate that these high energy faces, starved of material from solution, dissolve and the extra flux of salicylic acid causes the voids to close.
| Item Type: | Journal Article | ||||
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| Subjects: | Q Science > QD Chemistry | ||||
| Divisions: | Faculty of Science > Chemistry | ||||
| Library of Congress Subject Headings (LCSH): | Salicylic acid, Crystals, Crystal growth, Chemical kinetics, Chemical microscopy | ||||
| Journal or Publication Title: | Crystal Growth & Design | ||||
| Publisher: | American Chemical Society | ||||
| ISSN: | 1528-7483 | ||||
| Official Date: | 6 February 2013 | ||||
| Dates: |
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| Date of first compliant deposit: | 24 December 2015 | ||||
| Volume: | Volume 13 | ||||
| Number: | Number 2 | ||||
| Page Range: | pp. 614-622 | ||||
| DOI: | 10.1021/cg301282q | ||||
| Status: | Peer Reviewed | ||||
| Publication Status: | Published | ||||
| Access rights to Published version: | Restricted or Subscription Access | ||||
| Funder: | European Research Council (ERC), Engineering and Physical Sciences Research Council (EPSRC) | ||||
| Grant number: | ERC-2009-AdG 247143-QUANTIF |
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