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Title: Time Dependent Structural Evolution of Porous Organic Cage CC3

Abstract

Porous organic cage compounds are emerged with remarkable structural diversity and functionality that have applications in gas separation, catalysis and energy storage. Fundamental understanding of nucleation and growth of such materials have significant implications for understanding molecularly directed self-assembly phenomena. Herein we followed the structural evolution of a prototypical type of porous organic cage, CC3 as a function of synthesis time. Three distinctive crystal formation stages were identified: at short synthesis times, a rapid crystal growth stage in which amorphous agglomerates transformed into larger irregular particles was observed. At intermediate synthesis times, a decrease in crystal size over time was observed presumably due to crystal fragmentation, redissolution and/or homogeneous nucleation led. Finally, at longer synthesis times, a regrowth process was observed in which particles coalesced through Ostwald ripening leading to a continuous increase in crystal size. Molecular simulation studies, based on the construction of in silico CC3 models and simulation of XRD patterns and nitrogen isotherms, confirm the samples at different synthesis times to be a mixture of CC3α and CC3 amorphous phases. The CC3α phase is found to contract at different synthesis times, and the amorphous phase is found to essentially disappear at the longest synthesis time. Nitrogen andmore » carbon dioxide adsorption properties of these CC3 phases were evaluated, and were highly dependent on synthesis time.« less

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1439002
Report Number(s):
PNNL-SA-131927
Journal ID: ISSN 1528-7483; KC0203020
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Crystal Growth and Design; Journal Volume: 18; Journal Issue: 2
Country of Publication:
United States
Language:
English
Subject:
Nucleation; Growth

Citation Formats

Lucero, Jolie, Elsaidi, Sameh, Anderson, Ryther, Wu, Ting, Gómez-Gualdrón, Diego A., Thallapally, Praveen K., and Carreon, Moises A.. Time Dependent Structural Evolution of Porous Organic Cage CC3. United States: N. p., 2018. Web. doi:10.1021/acs.cgd.7b01405.
Lucero, Jolie, Elsaidi, Sameh, Anderson, Ryther, Wu, Ting, Gómez-Gualdrón, Diego A., Thallapally, Praveen K., & Carreon, Moises A.. Time Dependent Structural Evolution of Porous Organic Cage CC3. United States. doi:10.1021/acs.cgd.7b01405.
Lucero, Jolie, Elsaidi, Sameh, Anderson, Ryther, Wu, Ting, Gómez-Gualdrón, Diego A., Thallapally, Praveen K., and Carreon, Moises A.. Tue . "Time Dependent Structural Evolution of Porous Organic Cage CC3". United States. doi:10.1021/acs.cgd.7b01405.
@article{osti_1439002,
title = {Time Dependent Structural Evolution of Porous Organic Cage CC3},
author = {Lucero, Jolie and Elsaidi, Sameh and Anderson, Ryther and Wu, Ting and Gómez-Gualdrón, Diego A. and Thallapally, Praveen K. and Carreon, Moises A.},
abstractNote = {Porous organic cage compounds are emerged with remarkable structural diversity and functionality that have applications in gas separation, catalysis and energy storage. Fundamental understanding of nucleation and growth of such materials have significant implications for understanding molecularly directed self-assembly phenomena. Herein we followed the structural evolution of a prototypical type of porous organic cage, CC3 as a function of synthesis time. Three distinctive crystal formation stages were identified: at short synthesis times, a rapid crystal growth stage in which amorphous agglomerates transformed into larger irregular particles was observed. At intermediate synthesis times, a decrease in crystal size over time was observed presumably due to crystal fragmentation, redissolution and/or homogeneous nucleation led. Finally, at longer synthesis times, a regrowth process was observed in which particles coalesced through Ostwald ripening leading to a continuous increase in crystal size. Molecular simulation studies, based on the construction of in silico CC3 models and simulation of XRD patterns and nitrogen isotherms, confirm the samples at different synthesis times to be a mixture of CC3α and CC3 amorphous phases. The CC3α phase is found to contract at different synthesis times, and the amorphous phase is found to essentially disappear at the longest synthesis time. Nitrogen and carbon dioxide adsorption properties of these CC3 phases were evaluated, and were highly dependent on synthesis time.},
doi = {10.1021/acs.cgd.7b01405},
journal = {Crystal Growth and Design},
number = 2,
volume = 18,
place = {United States},
year = {Tue Jan 23 00:00:00 EST 2018},
month = {Tue Jan 23 00:00:00 EST 2018}
}