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Pregled bibliografske jedinice broj: 870726

Reversible Gas−Solid Ammonia N−H Bond Activation Mediated by an Organopalladium Complex


Juribašić Kulcsar, Marina; Halasz, Ivan; Budimir, Ana; Užarević, Krunoslav; Lukin, Stipe; Monas, Andrea; Emmerling, Franziska; Plavec, Janez; Ćurić, Manda
Reversible Gas−Solid Ammonia N−H Bond Activation Mediated by an Organopalladium Complex // Inorganic chemistry, 56 (2017), 9; 5342-5351 doi:10.1021/acs.inorgchem.7b00422 (međunarodna recenzija, članak, znanstveni)


Naslov
Reversible Gas−Solid Ammonia N−H Bond Activation Mediated by an Organopalladium Complex

Autori
Juribašić Kulcsar, Marina ; Halasz, Ivan ; Budimir, Ana ; Užarević, Krunoslav ; Lukin, Stipe ; Monas, Andrea ; Emmerling, Franziska ; Plavec, Janez ; Ćurić, Manda

Izvornik
Inorganic chemistry (0020-1669) 56 (2017), 9; 5342-5351

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

Ključne riječi
N-H activation ; gas-solid reaction ; dipalladated complex ; spectroscopy ; DFT calculations

Sažetak
N−H bond activation of gaseous ammonia is achieved at room temperature in a reversible solvent-free reaction using a solid dicyclopalladated azobenzene complex. Monitoring of the gas−solid reaction in real-time by in situ solid-state Raman spectroscopy enabled a detailed insight into the stepwise activation pathway proceeding to the final amido complex via a stable diammine intermediate. Gas−solid synthesis allowed for isolation and subsequent structural characterization of the intermediate and the final amido product, which presents the first dipalladated complex with the PdII−(μ-NH2)−PdII bridge. Gas−solid reaction is readily followed via color changes associated with conformational switching of the palladated azobenzene backbone. The reaction proceeds analogously in solution and was characterized by UV−vis and NMR spectroscopies showing the same stepwise route to the amido complex. Combining the experimental data with density functional theory calculations we propose a stepwise mechanism of this heterolytic N−H bond activation assisted by exogenous ammonia.

Izvorni jezik
Engleski

Znanstvena područja
Kemija



POVEZANOST RADA


Projekt / tema
HRZZ-IP-2014-09-7984 - Zelena sinteza organopaladijevih foto-osjetljivih spojeva
HRZZ-UIP-2014-09-4744 - Mehaniokemijska reaktivnost pod kontroliranim uvjetima temperature i atmosfere za čišću sintezu funkcionalnih materijala (Krunoslav Užarević, )

Ustanove
Farmaceutsko-biokemijski fakultet, Zagreb,
Institut "Ruđer Bošković", Zagreb

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


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