Particle breakage kinetics and mechanisms in attrition-enhanced deracemization

Christos Xiouras, Antonios A. Fytopoulos, Joop H. Ter Horst, Andreas G. Boudouvis, Tom Van Gerven, Georgios D. Stefanidis

Research output: Contribution to journalArticle

Abstract

In this study, we report on experiments designed to deconvolute the particle breakage kinetics and mechanism from the parallel phenomena (growth-dissolution, agglomeration) in attrition-enhanced deracemization processes. Through such experiments, we derived the specific breakage rates and cumulative breakage distribution functions for three grinding methods typically used in deracemization experiments: (a) bead grinding, (b) ultrasound grinding, and (c) the combination of bead and ultrasound grinding. Subsequently, we tested these methods on their ability to induce deracemization. We show that in the conventional bead grinding process, breakage occurs mostly by fracture. This results in slow deracemization rates due to the delayed formation of submicron particles that are essential to the process. Conversely, ultrasound grinding very efficiently breaks particles by abrasion. This leads to fast generation of an abundance of submicron fragments resulting in fast deracemization. However, using ultrasound, large crystals fracture rates are an order of magnitude lower than those using bead grinding, which results in an insufficient size decrease of the large counter enantiomer crystals and eventually to incomplete deracemization. Remarkably, the simultaneous application of bead and ultrasound grinding leads, due to synergistic effects of both fracture and abrasion, to 2-fold higher total deracemization rates compared to bead grinding alone. The present work offers new insights into the key role of particle breakage in attrition-enhanced deracemization, together with a basis for decoupling the individual phenomena involved in the process.

LanguageEnglish
Pages3051-3061
Number of pages11
JournalCrystal Growth and Design
Volume18
Issue number5
Early online date28 Mar 2018
DOIs
StatePublished - 2 May 2018

Fingerprint

comminution
grinding
Ultrasonics
beads
Kinetics
kinetics
Abrasion
abrasion
Crystals
Enantiomers
Experiments
Distribution functions
Dissolution
Agglomeration
enantiomers
agglomeration
decoupling
crystals
dissolving
counters

Keywords

  • deracemization
  • Viedma ripening
  • particle breakage
  • bead grinding
  • ultrasound grinding
  • abrasion
  • fracture
  • sodium chlorate

Cite this

Xiouras, C., Fytopoulos, A. A., Ter Horst, J. H., Boudouvis, A. G., Van Gerven, T., & Stefanidis, G. D. (2018). Particle breakage kinetics and mechanisms in attrition-enhanced deracemization. Crystal Growth and Design, 18(5), 3051-3061. DOI: 10.1021/acs.cgd.8b00201
Xiouras, Christos ; Fytopoulos, Antonios A. ; Ter Horst, Joop H. ; Boudouvis, Andreas G. ; Van Gerven, Tom ; Stefanidis, Georgios D./ Particle breakage kinetics and mechanisms in attrition-enhanced deracemization. In: Crystal Growth and Design. 2018 ; Vol. 18, No. 5. pp. 3051-3061
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Xiouras, C, Fytopoulos, AA, Ter Horst, JH, Boudouvis, AG, Van Gerven, T & Stefanidis, GD 2018, 'Particle breakage kinetics and mechanisms in attrition-enhanced deracemization' Crystal Growth and Design, vol. 18, no. 5, pp. 3051-3061. DOI: 10.1021/acs.cgd.8b00201

Particle breakage kinetics and mechanisms in attrition-enhanced deracemization. / Xiouras, Christos; Fytopoulos, Antonios A.; Ter Horst, Joop H.; Boudouvis, Andreas G.; Van Gerven, Tom; Stefanidis, Georgios D.

In: Crystal Growth and Design, Vol. 18, No. 5, 02.05.2018, p. 3051-3061.

Research output: Contribution to journalArticle

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T1 - Particle breakage kinetics and mechanisms in attrition-enhanced deracemization

AU - Xiouras,Christos

AU - Fytopoulos,Antonios A.

AU - Ter Horst,Joop H.

AU - Boudouvis,Andreas G.

AU - Van Gerven,Tom

AU - Stefanidis,Georgios D.

N1 - This document is the Accepted Manuscript version of a Published Work that appeared in final form in Crustal Growth and Design, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see hrrps://doi.org/10.1021/acs.cgd.8b00201.

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Y1 - 2018/5/2

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AB - In this study, we report on experiments designed to deconvolute the particle breakage kinetics and mechanism from the parallel phenomena (growth-dissolution, agglomeration) in attrition-enhanced deracemization processes. Through such experiments, we derived the specific breakage rates and cumulative breakage distribution functions for three grinding methods typically used in deracemization experiments: (a) bead grinding, (b) ultrasound grinding, and (c) the combination of bead and ultrasound grinding. Subsequently, we tested these methods on their ability to induce deracemization. We show that in the conventional bead grinding process, breakage occurs mostly by fracture. This results in slow deracemization rates due to the delayed formation of submicron particles that are essential to the process. Conversely, ultrasound grinding very efficiently breaks particles by abrasion. This leads to fast generation of an abundance of submicron fragments resulting in fast deracemization. However, using ultrasound, large crystals fracture rates are an order of magnitude lower than those using bead grinding, which results in an insufficient size decrease of the large counter enantiomer crystals and eventually to incomplete deracemization. Remarkably, the simultaneous application of bead and ultrasound grinding leads, due to synergistic effects of both fracture and abrasion, to 2-fold higher total deracemization rates compared to bead grinding alone. The present work offers new insights into the key role of particle breakage in attrition-enhanced deracemization, together with a basis for decoupling the individual phenomena involved in the process.

KW - deracemization

KW - Viedma ripening

KW - particle breakage

KW - bead grinding

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KW - abrasion

KW - fracture

KW - sodium chlorate

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Xiouras C, Fytopoulos AA, Ter Horst JH, Boudouvis AG, Van Gerven T, Stefanidis GD. Particle breakage kinetics and mechanisms in attrition-enhanced deracemization. Crystal Growth and Design. 2018 May 2;18(5):3051-3061. Available from, DOI: 10.1021/acs.cgd.8b00201