Quantifying the Effect of Guest Binding on Host Environment Article Swipe
Hugh P. Ryan
,
Zachary S. Fishman
,
Jacob T. Pawlik
,
Angela B. Grommet
,
Małgorzata Musiał
,
Felix J. Rizzuto
,
James C. Booth
,
Christian J. Long
,
Kathleen Schwarz
,
Nathan D. Orloff
,
Jonathan R. Nitschke
,
Angela C. Stelson
·
YOU?
·
· 2023
· Open Access
·
· DOI: https://doi.org/10.1021/jacs.3c01409
YOU?
·
· 2023
· Open Access
·
· DOI: https://doi.org/10.1021/jacs.3c01409
The environment around a host-guest complex is defined by intermolecular interactions between the complex, solvent molecules, and counterions. These interactions govern both the solubility of these complexes and the rates of reactions occurring within the host molecules and can be critical to catalytic and separation applications of host-guest systems. However, these interactions are challenging to detect using standard analytical chemistry techniques. Here, we quantify the hydration and ion pairing of a FeII4L4 coordination cage with a set of guest molecules having widely varying physicochemical properties. The impact of guest properties on host ion pairing and hydration was determined through microwave microfluidic measurements paired with principal component analysis (PCA). This analysis showed that introducing guest molecules into solution displaced counterions that were bound to the cage, and that the solvent solubility of the guest has the greatest impact on the solvent and ion-pairing dynamics surrounding the host. Specifically, we found that when we performed PCA of the measured equivalent circuit parameters and the solubility and dipole moment, we observed a high (>90%) explained variance for the first two principal components for each circuit parameter. We also observed that cage-counterion pairing is well-described by a single ion-pairing type, with a one-step reaction model independent of the type of cargo, and that the ion-pairing association constant is reduced for cargo with higher water solubility. Quantifying hydration and cage-counterion interactions is a critical step to building the next generation of design criteria for host-guest chemistries.
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Metadata
- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1021/jacs.3c01409
- OA Status
- green
- Cited By
- 8
- References
- 38
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W4386263167
All OpenAlex metadata
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https://openalex.org/W4386263167Canonical identifier for this work in OpenAlex
- DOI
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https://doi.org/10.1021/jacs.3c01409Digital Object Identifier
- Title
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Quantifying the Effect of Guest Binding on Host EnvironmentWork title
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articleOpenAlex work type
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enPrimary language
- Publication year
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2023Year of publication
- Publication date
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2023-08-29Full publication date if available
- Authors
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Hugh P. Ryan, Zachary S. Fishman, Jacob T. Pawlik, Angela B. Grommet, Małgorzata Musiał, Felix J. Rizzuto, James C. Booth, Christian J. Long, Kathleen Schwarz, Nathan D. Orloff, Jonathan R. Nitschke, Angela C. StelsonList of authors in order
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https://doi.org/10.1021/jacs.3c01409Publisher landing page
- Open access
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YesWhether a free full text is available
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greenOpen access status per OpenAlex
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https://pmc.ncbi.nlm.nih.gov/articles/PMC10510717/pdf/ja3c01409.pdfDirect OA link when available
- Concepts
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Counterion, Chemistry, Pairing, Chemical physics, Intermolecular force, Solubility, Molecule, Solvent, Ion, Dipole, Computational chemistry, Physical chemistry, Organic chemistry, Quantum mechanics, Superconductivity, PhysicsTop concepts (fields/topics) attached by OpenAlex
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8Total citation count in OpenAlex
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2025: 2, 2024: 5, 2023: 1Per-year citation counts (last 5 years)
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10Other works algorithmically related by OpenAlex
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| abstract_inverted_index.systems. | 48 |
| abstract_inverted_index.variance | 172 |
| abstract_inverted_index.catalytic | 42 |
| abstract_inverted_index.chemistry | 59 |
| abstract_inverted_index.complexes | 26 |
| abstract_inverted_index.component | 105 |
| abstract_inverted_index.displaced | 117 |
| abstract_inverted_index.explained | 171 |
| abstract_inverted_index.hydration | 65, 95, 222 |
| abstract_inverted_index.microwave | 99 |
| abstract_inverted_index.molecules | 36, 79, 114 |
| abstract_inverted_index.occurring | 32 |
| abstract_inverted_index.performed | 152 |
| abstract_inverted_index.principal | 104, 177 |
| abstract_inverted_index.reactions | 31 |
| abstract_inverted_index.analytical | 58 |
| abstract_inverted_index.components | 178 |
| abstract_inverted_index.determined | 97 |
| abstract_inverted_index.equivalent | 157 |
| abstract_inverted_index.generation | 234 |
| abstract_inverted_index.host-guest | 4, 47, 239 |
| abstract_inverted_index.molecules, | 15 |
| abstract_inverted_index.parameter. | 182 |
| abstract_inverted_index.parameters | 159 |
| abstract_inverted_index.properties | 89 |
| abstract_inverted_index.separation | 44 |
| abstract_inverted_index.solubility | 23, 129, 162 |
| abstract_inverted_index.Quantifying | 221 |
| abstract_inverted_index.association | 211 |
| abstract_inverted_index.challenging | 53 |
| abstract_inverted_index.counterions | 118 |
| abstract_inverted_index.environment | 1 |
| abstract_inverted_index.independent | 201 |
| abstract_inverted_index.introducing | 112 |
| abstract_inverted_index.ion-pairing | 141, 194, 210 |
| abstract_inverted_index.properties. | 84 |
| abstract_inverted_index.solubility. | 220 |
| abstract_inverted_index.surrounding | 143 |
| abstract_inverted_index.techniques. | 60 |
| abstract_inverted_index.applications | 45 |
| abstract_inverted_index.chemistries. | 240 |
| abstract_inverted_index.coordination | 72 |
| abstract_inverted_index.counterions. | 17 |
| abstract_inverted_index.interactions | 10, 19, 51, 225 |
| abstract_inverted_index.measurements | 101 |
| abstract_inverted_index.microfluidic | 100 |
| abstract_inverted_index.Specifically, | 146 |
| abstract_inverted_index.intermolecular | 9 |
| abstract_inverted_index.well-described | 190 |
| abstract_inverted_index.cage-counterion | 187, 224 |
| abstract_inverted_index.physicochemical | 83 |
| abstract_inverted_index.Fe<sup>II</sup><sub>4</sub>L<sub>4</sub> | 71 |
| cited_by_percentile_year.max | 98 |
| cited_by_percentile_year.min | 89 |
| corresponding_author_ids | https://openalex.org/A5085365122 |
| countries_distinct_count | 2 |
| institutions_distinct_count | 12 |
| corresponding_institution_ids | https://openalex.org/I1321296531, https://openalex.org/I4210101396 |
| sustainable_development_goals[0].id | https://metadata.un.org/sdg/6 |
| sustainable_development_goals[0].score | 0.7099999785423279 |
| sustainable_development_goals[0].display_name | Clean water and sanitation |
| citation_normalized_percentile.value | 0.66369212 |
| citation_normalized_percentile.is_in_top_1_percent | False |
| citation_normalized_percentile.is_in_top_10_percent | False |