Understanding Correlation Between CO2 Insertion Mechanism and Chain Length of Diamine in Metal-Organic Framework Adsorbents
DC Field | Value | Language |
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dc.contributor.author | Ju, Susan E. | - |
dc.contributor.author | Choe, Jong Hyeak | - |
dc.contributor.author | Kang, Minjung | - |
dc.contributor.author | Kang, Dong Won | - |
dc.contributor.author | Kim, Hyojin | - |
dc.contributor.author | Lee, Jung-Hoon | - |
dc.contributor.author | Hong, Chang Seop | - |
dc.date.accessioned | 2021-11-18T09:40:31Z | - |
dc.date.available | 2021-11-18T09:40:31Z | - |
dc.date.created | 2021-08-30 | - |
dc.date.issued | 2021-06-08 | - |
dc.identifier.issn | 1864-5631 | - |
dc.identifier.uri | https://scholar.korea.ac.kr/handle/2021.sw.korea/127858 | - |
dc.description.abstract | Although CO2 insertion is a predominant phenomenon in diamine-functionalized Mg-2(dobpdc) (dobpdc(4-)=4,4-dioxidobiphenyl-3,3 '-dicarboxylate) adsorbents, a high-performance metal-organic framework for capturing CO2, the fundamental function of the diamine carbon chain length in the mechanism remains unclear. Here, Mg-2(dobpdc) systems with open metal sites grafted by primary diamines NH2-(CH2)(n)-NH2 were developed, with en (n=2), pn (n=3), bn (n=4), pen (n=5), hn (n=6), and on (n=8). Based on CO2 adsorption and IR results, CO2 insertion is involved in frameworks with n=2 and 3 but not in systems with n >= 5. According to NMR data, bn-appended Mg-2(dobpdc) exhibited three different chemical environments of carbamate units, attributed to different relative conformations of carbon chains upon CO2 insertion, as validated by first-principles density functional theory (DFT) calculations. For 1-hn and 1-on, DFT calculations indicated that diamine inter-coordinated open metal sites in adjacent chains bridged by carboxylates and phenoxides of dobpdc(4-). Computed CO2 binding enthalpies for CO2 insertion (-27.8 kJ mol(-1) for 1-hn and -20.2 kJ mol(-1) for 1-on) were comparable to those for CO2 physisorption (-19.3 kJ mol(-1) for 1-hn and -20.8 kJ mol(-1) for 1-on). This suggests that CO2 insertion is likely to compete with CO2 physisorption on diamines of the framework when n >= 5. | - |
dc.language | English | - |
dc.language.iso | en | - |
dc.publisher | WILEY-V C H VERLAG GMBH | - |
dc.subject | SOLVENTS | - |
dc.title | Understanding Correlation Between CO2 Insertion Mechanism and Chain Length of Diamine in Metal-Organic Framework Adsorbents | - |
dc.type | Article | - |
dc.contributor.affiliatedAuthor | Hong, Chang Seop | - |
dc.identifier.doi | 10.1002/cssc.202100582 | - |
dc.identifier.scopusid | 2-s2.0-85105205064 | - |
dc.identifier.wosid | 000646105300001 | - |
dc.identifier.bibliographicCitation | CHEMSUSCHEM, v.14, no.11, pp.2426 - 2433 | - |
dc.relation.isPartOf | CHEMSUSCHEM | - |
dc.citation.title | CHEMSUSCHEM | - |
dc.citation.volume | 14 | - |
dc.citation.number | 11 | - |
dc.citation.startPage | 2426 | - |
dc.citation.endPage | 2433 | - |
dc.type.rims | ART | - |
dc.type.docType | Article | - |
dc.description.journalClass | 1 | - |
dc.description.journalRegisteredClass | scie | - |
dc.description.journalRegisteredClass | scopus | - |
dc.relation.journalResearchArea | Chemistry | - |
dc.relation.journalResearchArea | Science & Technology - Other Topics | - |
dc.relation.journalWebOfScienceCategory | Chemistry, Multidisciplinary | - |
dc.relation.journalWebOfScienceCategory | Green & Sustainable Science & Technology | - |
dc.subject.keywordPlus | SOLVENTS | - |
dc.subject.keywordAuthor | amine functionalization | - |
dc.subject.keywordAuthor | carbon dioxide | - |
dc.subject.keywordAuthor | CO2 capture and storage | - |
dc.subject.keywordAuthor | mechanism | - |
dc.subject.keywordAuthor | metal-organic frameworks | - |
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