Engineering Porous Organic Cage Crystals with Increased Acid Gas Resistance

Guanghui Zhu; Christopher D. Hoffman; Yang Liu; Souryadeep Bhattacharyya; Uma Tumuluri; Melinda L. Jue; Zili Wu; David S. Sholl; Sankar Nair; Christopher W. Jones; Ryan P. Lively

doi:10.1002/chem.201601659

Engineering Porous Organic Cage Crystals with Increased Acid Gas Resistance

Guanghui Zhu, Christopher D. Hoffman, Yang Liu, Souryadeep Bhattacharyya, Uma Tumuluri, Melinda L. Jue, Zili Wu, David S. Sholl, Sankar Nair, Christopher W. Jones, Ryan P. Lively

Surface Chemistry & Catalysis Group

Research output: Contribution to journal › Article › peer-review

32 Scopus citations

Abstract

Both known and new CC3-based porous organic cages are prepared and exposed to acidic SO₂in vapor and liquid conditions. Distinct differences in the stability of the CC3 cages exist depending on the chirality of the diamine linkers used. The acid catalyzed CC3 degradation mechanism is probed via in situ IR and a degradation pathway is proposed and supported with computational results. CC3 crystals synthesized with racemic mixtures of diaminocyclohexane exhibited enhanced stability compared to CC3-R and CC3-S. Confocal fluorescent microscope images reveal that the stability difference in CC3 species originates from an abundance of mesoporous grain boundaries in CC3-R and CC3-S, allowing facile access of aqueous SO₂throughout the crystal, promoting decomposition. These grain boundaries are absent from CC3 crystals made with racemic linkers.

Original language	English
Pages (from-to)	10743-10747
Number of pages	5
Journal	Chemistry - A European Journal
Volume	22
Issue number	31
DOIs	https://doi.org/10.1002/chem.201601659
State	Published - Jul 25 2016

Keywords

acid gas interactions
cage compounds
grain boundaries
microporous materials
sulfur dioxide

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10.1002/chem.201601659

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title = "Engineering Porous Organic Cage Crystals with Increased Acid Gas Resistance",

abstract = "Both known and new CC3-based porous organic cages are prepared and exposed to acidic SO2in vapor and liquid conditions. Distinct differences in the stability of the CC3 cages exist depending on the chirality of the diamine linkers used. The acid catalyzed CC3 degradation mechanism is probed via in situ IR and a degradation pathway is proposed and supported with computational results. CC3 crystals synthesized with racemic mixtures of diaminocyclohexane exhibited enhanced stability compared to CC3-R and CC3-S. Confocal fluorescent microscope images reveal that the stability difference in CC3 species originates from an abundance of mesoporous grain boundaries in CC3-R and CC3-S, allowing facile access of aqueous SO2throughout the crystal, promoting decomposition. These grain boundaries are absent from CC3 crystals made with racemic linkers.",

keywords = "acid gas interactions, cage compounds, grain boundaries, microporous materials, sulfur dioxide",

author = "Guanghui Zhu and Hoffman, {Christopher D.} and Yang Liu and Souryadeep Bhattacharyya and Uma Tumuluri and Jue, {Melinda L.} and Zili Wu and Sholl, {David S.} and Sankar Nair and Jones, {Christopher W.} and Lively, {Ryan P.}",

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month = jul,

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doi = "10.1002/chem.201601659",

language = "English",

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T1 - Engineering Porous Organic Cage Crystals with Increased Acid Gas Resistance

AU - Zhu, Guanghui

AU - Hoffman, Christopher D.

AU - Liu, Yang

AU - Bhattacharyya, Souryadeep

AU - Tumuluri, Uma

AU - Jue, Melinda L.

AU - Wu, Zili

AU - Sholl, David S.

AU - Nair, Sankar

AU - Jones, Christopher W.

AU - Lively, Ryan P.

PY - 2016/7/25

Y1 - 2016/7/25

N2 - Both known and new CC3-based porous organic cages are prepared and exposed to acidic SO2in vapor and liquid conditions. Distinct differences in the stability of the CC3 cages exist depending on the chirality of the diamine linkers used. The acid catalyzed CC3 degradation mechanism is probed via in situ IR and a degradation pathway is proposed and supported with computational results. CC3 crystals synthesized with racemic mixtures of diaminocyclohexane exhibited enhanced stability compared to CC3-R and CC3-S. Confocal fluorescent microscope images reveal that the stability difference in CC3 species originates from an abundance of mesoporous grain boundaries in CC3-R and CC3-S, allowing facile access of aqueous SO2throughout the crystal, promoting decomposition. These grain boundaries are absent from CC3 crystals made with racemic linkers.

AB - Both known and new CC3-based porous organic cages are prepared and exposed to acidic SO2in vapor and liquid conditions. Distinct differences in the stability of the CC3 cages exist depending on the chirality of the diamine linkers used. The acid catalyzed CC3 degradation mechanism is probed via in situ IR and a degradation pathway is proposed and supported with computational results. CC3 crystals synthesized with racemic mixtures of diaminocyclohexane exhibited enhanced stability compared to CC3-R and CC3-S. Confocal fluorescent microscope images reveal that the stability difference in CC3 species originates from an abundance of mesoporous grain boundaries in CC3-R and CC3-S, allowing facile access of aqueous SO2throughout the crystal, promoting decomposition. These grain boundaries are absent from CC3 crystals made with racemic linkers.

KW - acid gas interactions

KW - cage compounds

KW - grain boundaries

KW - microporous materials

KW - sulfur dioxide

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DO - 10.1002/chem.201601659

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AN - SCOPUS:84978906369

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SP - 10743

EP - 10747

JO - Chemistry - A European Journal

JF - Chemistry - A European Journal

IS - 31

ER -

Engineering Porous Organic Cage Crystals with Increased Acid Gas Resistance

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Keywords

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