Dehydrogenation of ammonia-borane by cationic Pd(II) and Ni(II) complexes in a nitromethane medium: hydrogen release and spent fuel characterization
DC Field | Value | Language |
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dc.contributor.author | Kim, Sung-Kwan | - |
dc.contributor.author | Hong, Sung-Ahn | - |
dc.contributor.author | Son, Ho-Jin | - |
dc.contributor.author | Han, Won-Sik | - |
dc.contributor.author | Michalak, Artur | - |
dc.contributor.author | Hwang, Son-Jong | - |
dc.contributor.author | Kang, Sang Ook | - |
dc.date.accessioned | 2021-09-05T00:47:02Z | - |
dc.date.available | 2021-09-05T00:47:02Z | - |
dc.date.created | 2021-06-15 | - |
dc.date.issued | 2015 | - |
dc.identifier.issn | 1477-9226 | - |
dc.identifier.uri | https://scholar.korea.ac.kr/handle/2021.sw.korea/96139 | - |
dc.description.abstract | A highly electrophilic cationic Pd-II complex, [Pd(MeCN)(4)][BF4](2) (1), brings about the preferential activation of the B-H bond in ammonia-borane (NH3 center dot BH3, AB). At room temperature, the reaction between 1 in CH3NO2 and AB in tetraglyme leads to Pd nanoparticles and formation of spent fuels of the general formula MeNHxBOy as reaction byproducts, while 2 equiv. of H-2 is efficiently released per AB equiv. at room temperature within 60 seconds. For a mechanistic understanding of dehydrogenation by 1, the chemical structures of spent fuels were intensely characterized by a series of analyses such as elemental analysis (EA), X-ray photoelectron spectroscopy (XPS), solid state magic-angle-spinning (MAS) NMR spectra (H-2, C-13, N-15, and B-11), and cross polarization (CP) MAS methods. During AB dehydrogenation, the involvement of MeNO2 in the spent fuels showed that the mechanism of dehydrogenation catalyzed by 1 is different from that found in the previously reported results. This AB dehydrogenation derived from MeNO2 is supported by a subsequent digestion experiment of the AB spent fuel: B(OMe)(3) and N-methyl-hydroxylamine ([Me(OH)N](2)CH2), which are formed by the methanolysis of the AB spent fuel (MeNHxBOy), were identified by means of B-11 NMR and single crystal structural analysis, respectively. A similar catalytic behavior was also observed in the AB dehydrogenation catalyzed by a nickel catalyst, [Ni(MeCN)(6)][BF4](2) (2). | - |
dc.language | English | - |
dc.language.iso | en | - |
dc.publisher | ROYAL SOC CHEMISTRY | - |
dc.subject | CATALYZED DEHYDROGENATION | - |
dc.subject | AMINE-BORANE | - |
dc.subject | THERMAL-DECOMPOSITION | - |
dc.subject | TRANSITION-METAL | - |
dc.subject | BORON-NITRIDE | - |
dc.subject | DIMETHYLAMINE BORANE | - |
dc.subject | STORAGE MATERIALS | - |
dc.subject | NMR | - |
dc.subject | ADDUCTS | - |
dc.subject | B-11 | - |
dc.title | Dehydrogenation of ammonia-borane by cationic Pd(II) and Ni(II) complexes in a nitromethane medium: hydrogen release and spent fuel characterization | - |
dc.type | Article | - |
dc.contributor.affiliatedAuthor | Son, Ho-Jin | - |
dc.contributor.affiliatedAuthor | Kang, Sang Ook | - |
dc.identifier.doi | 10.1039/c5dt00599j | - |
dc.identifier.scopusid | 2-s2.0-84927722479 | - |
dc.identifier.wosid | 000352784000036 | - |
dc.identifier.bibliographicCitation | DALTON TRANSACTIONS, v.44, no.16, pp.7373 - 7381 | - |
dc.relation.isPartOf | DALTON TRANSACTIONS | - |
dc.citation.title | DALTON TRANSACTIONS | - |
dc.citation.volume | 44 | - |
dc.citation.number | 16 | - |
dc.citation.startPage | 7373 | - |
dc.citation.endPage | 7381 | - |
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.journalWebOfScienceCategory | Chemistry, Inorganic & Nuclear | - |
dc.subject.keywordPlus | CATALYZED DEHYDROGENATION | - |
dc.subject.keywordPlus | AMINE-BORANE | - |
dc.subject.keywordPlus | THERMAL-DECOMPOSITION | - |
dc.subject.keywordPlus | TRANSITION-METAL | - |
dc.subject.keywordPlus | BORON-NITRIDE | - |
dc.subject.keywordPlus | DIMETHYLAMINE BORANE | - |
dc.subject.keywordPlus | STORAGE MATERIALS | - |
dc.subject.keywordPlus | NMR | - |
dc.subject.keywordPlus | ADDUCTS | - |
dc.subject.keywordPlus | B-11 | - |
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