Heterogeneous Nucleation of an n-Alkane on Tetrahedrally Coordinated Crystals.
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| Title: | Heterogeneous Nucleation of an n-Alkane on Tetrahedrally Coordinated Crystals. |
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| Authors: | Bourque, Alexander J.1, Locker, C. Rebecca2, Rutledge, Gregory C.1 rutledge@mit.edu |
| Source: | Journal of Physical Chemistry B. Feb2017, Vol. 121 Issue 4, p904-911. 8p. |
| Subjects: | Heterogenous nucleation, Alkanes, Chemical reactions, Aliphatic compounds, Hexane |
| Abstract: | Heterogeneous nucleation refers to the propensity for phase transformations to initiate preferentially on foreign surfaces, such as vessel walls, dust particles, or formulation additives. In crystallization, the form of the initial nucleus has ramifications for the crystallographic form, morphology, and properties of the resulting solid. Nevertheless, the discovery and design of nucleating agents remains a matter of trial and error because of the very small spatiotemporal scales over which the critical nucleus is formed and the extreme difficulty of examining such events empirically. Using molecular dynamics simulations, we demonstrate a method for the rapid screening of entire families of materials for activity as nucleating agents and for characterizing their mechanism of action. The method is applied to the crystallization of n-pentacontane, a model surrogate for polyethylene, on the family of tetrahedrally coordinated crystals, including diamond and silicon. A systematic variation of parameters in the interaction potential permits a comprehensive, physically based screening of nucleating agents in this class of materials, including both real and hypothetical candidates. The induction time for heterogeneous nucleation is shown to depend strongly on crystallographic registry between the nucleating agent and the critical nucleus, indicative of an epitaxial mechanism in this class of materials. Importantly, the severity of this registry requirement weakens with decreasing rigidity of the substrate and increasing strength of attraction to the surface of the nucleating agent. Employing this method, a high-throughput computational screening of nucleating agents becomes possible, facilitating the discovery of novel nucleating agents within a broad "materials genome" of possible additives. [ABSTRACT FROM AUTHOR] |
| Copyright of Journal of Physical Chemistry B is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.) | |
| Database: | Engineering Source |
| FullText | Text: Availability: 0 |
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| Header | DbId: egs DbLabel: Engineering Source An: 121102238 AccessLevel: 6 PubType: Academic Journal PubTypeId: academicJournal PreciseRelevancyScore: 0 |
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| Items | – Name: Title Label: Title Group: Ti Data: Heterogeneous Nucleation of an n-Alkane on Tetrahedrally Coordinated Crystals. – Name: Author Label: Authors Group: Au Data: <searchLink fieldCode="AR" term="%22Bourque%2C+Alexander+J%2E%22">Bourque, Alexander J.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Locker%2C+C%2E+Rebecca%22">Locker, C. Rebecca</searchLink><relatesTo>2</relatesTo><br /><searchLink fieldCode="AR" term="%22Rutledge%2C+Gregory+C%2E%22">Rutledge, Gregory C.</searchLink><relatesTo>1</relatesTo><i> rutledge@mit.edu</i> – Name: TitleSource Label: Source Group: Src Data: <searchLink fieldCode="JN" term="%22Journal+of+Physical+Chemistry+B%22">Journal of Physical Chemistry B</searchLink>. Feb2017, Vol. 121 Issue 4, p904-911. 8p. – Name: Subject Label: Subjects Group: Su Data: <searchLink fieldCode="DE" term="%22Heterogenous+nucleation%22">Heterogenous nucleation</searchLink><br /><searchLink fieldCode="DE" term="%22Alkanes%22">Alkanes</searchLink><br /><searchLink fieldCode="DE" term="%22Chemical+reactions%22">Chemical reactions</searchLink><br /><searchLink fieldCode="DE" term="%22Aliphatic+compounds%22">Aliphatic compounds</searchLink><br /><searchLink fieldCode="DE" term="%22Hexane%22">Hexane</searchLink> – Name: Abstract Label: Abstract Group: Ab Data: Heterogeneous nucleation refers to the propensity for phase transformations to initiate preferentially on foreign surfaces, such as vessel walls, dust particles, or formulation additives. In crystallization, the form of the initial nucleus has ramifications for the crystallographic form, morphology, and properties of the resulting solid. Nevertheless, the discovery and design of nucleating agents remains a matter of trial and error because of the very small spatiotemporal scales over which the critical nucleus is formed and the extreme difficulty of examining such events empirically. Using molecular dynamics simulations, we demonstrate a method for the rapid screening of entire families of materials for activity as nucleating agents and for characterizing their mechanism of action. The method is applied to the crystallization of n-pentacontane, a model surrogate for polyethylene, on the family of tetrahedrally coordinated crystals, including diamond and silicon. A systematic variation of parameters in the interaction potential permits a comprehensive, physically based screening of nucleating agents in this class of materials, including both real and hypothetical candidates. The induction time for heterogeneous nucleation is shown to depend strongly on crystallographic registry between the nucleating agent and the critical nucleus, indicative of an epitaxial mechanism in this class of materials. Importantly, the severity of this registry requirement weakens with decreasing rigidity of the substrate and increasing strength of attraction to the surface of the nucleating agent. Employing this method, a high-throughput computational screening of nucleating agents becomes possible, facilitating the discovery of novel nucleating agents within a broad "materials genome" of possible additives. [ABSTRACT FROM AUTHOR] – Name: AbstractSuppliedCopyright Label: Group: Ab Data: <i>Copyright of Journal of Physical Chemistry B is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.) |
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| RecordInfo | BibRecord: BibEntity: Identifiers: – Type: doi Value: 10.1021/acs.jpcb.6b12590 Languages: – Code: eng Text: English PhysicalDescription: Pagination: PageCount: 8 StartPage: 904 Subjects: – SubjectFull: Heterogenous nucleation Type: general – SubjectFull: Alkanes Type: general – SubjectFull: Chemical reactions Type: general – SubjectFull: Aliphatic compounds Type: general – SubjectFull: Hexane Type: general Titles: – TitleFull: Heterogeneous Nucleation of an n-Alkane on Tetrahedrally Coordinated Crystals. Type: main BibRelationships: HasContributorRelationships: – PersonEntity: Name: NameFull: Bourque, Alexander J. – PersonEntity: Name: NameFull: Locker, C. Rebecca – PersonEntity: Name: NameFull: Rutledge, Gregory C. IsPartOfRelationships: – BibEntity: Dates: – D: 02 M: 02 Text: Feb2017 Type: published Y: 2017 Identifiers: – Type: issn-print Value: 15206106 Numbering: – Type: volume Value: 121 – Type: issue Value: 4 Titles: – TitleFull: Journal of Physical Chemistry B Type: main |
| ResultId | 1 |
