NH3 as unique non-classical content-former within clathrate hydrates
Küçük Resim Yok
Tarih
2017
Dergi Başlığı
Dergi ISSN
Cilt Başlığı
Yayıncı
Aip Publishing
Erişim Hakkı
info:eu-repo/semantics/openAccess
Özet
High quality FTIR spectra of aerosols of NH3-THF and NH3-TMO binary clathrate hydrates (CHs) have been measured. Our recently developed all-vapor sub-second approach to clathrate-hydrate formation combined with computational studies has been used to identify vibrational spectroscopic signatures of NH3 within the gas hydrates. The present study shows that there are three distinct NH3 types, namely, classical small-cage NH3, nonclassical small-cage NH3, and NH3 within the hydrate network. The network ammonia does not directly trigger the non-classical CH structure. Rather, the ammonia within the network structure perturbs the water bonding, introducing orientational defects that are stabilized by small and/or large cage guest molecules through H-bonding. This unusual behavior of NH3 within CHs opens a possibility for catalytic action of NH3 during CH-formation. Furthermore, impacts over time of the small-cage NH3-replacement molecules CO2 and CH4 on the structure and composition of the ternary CHs have been noted. Published by AIP Publishing.
Açıklama
Anahtar Kelimeler
Infrared-Spectra, Ice, Ammonia, Conversion, Dynamics, Hcl
Kaynak
Journal of Chemical Physics
WoS Q Değeri
Q2
Scopus Q Değeri
Q1
Cilt
146
Sayı
23
