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Pregled bibliografske jedinice broj: 865670

Ligand-induced substrate steering and reshaping of [Ag2(H)]+ scaffold for selective CO2 extrusion from formic acid

Zavras, Athanasios; Khairallah, George N.; Krstić, Marjan; Girod, Marion; Daly, Steven; Antoine, Rodolphe; Maitre, Philippe; Mulder, Roger J.; Alexander, Stefanie-Ann; Bonačić-Koutecký, Vlasta et al.
Ligand-induced substrate steering and reshaping of [Ag2(H)]+ scaffold for selective CO2 extrusion from formic acid // Nature Communications, 7 (2016), 11746-1 doi:10.1038/ncomms11746 (međunarodna recenzija, članak, znanstveni)

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Naslov
Ligand-induced substrate steering and reshaping of [Ag2(H)]+ scaffold for selective CO2 extrusion from formic acid

Autori
Zavras, Athanasios ; Khairallah, George N. ; Krstić, Marjan ; Girod, Marion ; Daly, Steven ; Antoine, Rodolphe ; Maitre, Philippe ; Mulder, Roger J. ; Alexander, Stefanie-Ann ; Bonačić-Koutecký, Vlasta ; Dugourd, Philippe ; O’Hair, Richard A. J.

Izvornik
Nature Communications (2041-1723) 7 (2016); 11746-1

Vrsta, podvrsta i kategorija rada
Radovi u časopisima, članak, znanstveni

Ključne riječi
ligated silver hydride, formic acid, decomposition, hydrogen release, experiments, DFT

Sažetak
Metalloenzymes preorganize the reaction environment to steer substrate(s) along the required reaction coordinate. Here, we show that phosphine ligands selectively facilitate protonation of binuclear silver hydride cations, [LAg2(H)]+ by optimizing the geometry of the active site. This is a key step in the selective, catalysed extrusion of carbon dioxide from formic acid, HO2CH, with important applications (for example, hydrogen storage). Gas- phase ion-molecule reactions, collision-induced dissociation (CID), infrared and ultraviolet action spectroscopy and computational chemistry link structure to reactivity and mechanism. [Ag2(H)]+ and [Ph3PAg2(H)]+ react with formic acid yielding Lewis adducts, while [(Ph3P)2Ag2(H)]+ is unreactive. Using bis(diphenylphosphino)methane (dppm) reshapes the geometry of the binuclear Ag2(H)+ scaffold, triggering reactivity towards formic acid, to produce [dppmAg2(O2CH)]+ and H2. Decarboxylation of [dppmAg2(O2CH)]+ via CID regenerates [dppmAg2(H)]+. These gas-phase insights inspired variable temperature NMR studies that show CO2 and H2 production at 70 °C from solutions containing dppm, AgBF4, NaO2CH and HO2CH.

Izvorni jezik
Engleski

Znanstvena područja
Fizika, Kemija



POVEZANOST RADA

Ustanove:
Sveučilište u Splitu

Profili:

Avatar Url Marjan Krstić (autor)

Poveznice na cjeloviti tekst rada:

doi www.nature.com

Citiraj ovu publikaciju:

Zavras, Athanasios; Khairallah, George N.; Krstić, Marjan; Girod, Marion; Daly, Steven; Antoine, Rodolphe; Maitre, Philippe; Mulder, Roger J.; Alexander, Stefanie-Ann; Bonačić-Koutecký, Vlasta et al.
Ligand-induced substrate steering and reshaping of [Ag2(H)]+ scaffold for selective CO2 extrusion from formic acid // Nature Communications, 7 (2016), 11746-1 doi:10.1038/ncomms11746 (međunarodna recenzija, članak, znanstveni)
Zavras, A., Khairallah, G., Krstić, M., Girod, M., Daly, S., Antoine, R., Maitre, P., Mulder, R., Alexander, S. & Bonačić-Koutecký, V. (2016) Ligand-induced substrate steering and reshaping of [Ag2(H)]+ scaffold for selective CO2 extrusion from formic acid. Nature Communications, 7, 11746-1 doi:10.1038/ncomms11746.
@article{article, author = {Zavras, Athanasios and Khairallah, George N. and Krsti\'{c}, Marjan and Girod, Marion and Daly, Steven and Antoine, Rodolphe and Maitre, Philippe and Mulder, Roger J. and Alexander, Stefanie-Ann and Bona\v{c}i\'{c}-Kouteck\'{y}, Vlasta and Dugourd, Philippe and O’Hair, Richard A. J.}, year = {2016}, pages = {11746-1-11746-8}, DOI = {10.1038/ncomms11746}, keywords = {ligated silver hydride, formic acid, decomposition, hydrogen release, experiments, DFT}, journal = {Nature Communications}, doi = {10.1038/ncomms11746}, volume = {7}, issn = {2041-1723}, title = {Ligand-induced substrate steering and reshaping of [Ag2(H)]+ scaffold for selective CO2 extrusion from formic acid}, keyword = {ligated silver hydride, formic acid, decomposition, hydrogen release, experiments, DFT} }
@article{article, author = {Zavras, Athanasios and Khairallah, George N. and Krsti\'{c}, Marjan and Girod, Marion and Daly, Steven and Antoine, Rodolphe and Maitre, Philippe and Mulder, Roger J. and Alexander, Stefanie-Ann and Bona\v{c}i\'{c}-Kouteck\'{y}, Vlasta and Dugourd, Philippe and O’Hair, Richard A. J.}, year = {2016}, pages = {11746-1-11746-8}, DOI = {10.1038/ncomms11746}, keywords = {ligated silver hydride, formic acid, decomposition, hydrogen release, experiments, DFT}, journal = {Nature Communications}, doi = {10.1038/ncomms11746}, volume = {7}, issn = {2041-1723}, title = {Ligand-induced substrate steering and reshaping of [Ag2(H)]+ scaffold for selective CO2 extrusion from formic acid}, keyword = {ligated silver hydride, formic acid, decomposition, hydrogen release, experiments, DFT} }

Časopis indeksira:


  • Current Contents Connect (CCC)
  • Web of Science Core Collection (WoSCC)
    • Science Citation Index Expanded (SCI-EXP)
    • SCI-EXP, SSCI i/ili A&HCI
  • Scopus
  • MEDLINE
  • Nature Index

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