558-20-3Relevant articles and documents
Effects of rhodium dispersion on catalytic behavior of Rh/active-carbon catalysts for H/D exchange reaction between and CH4 and D2
Sakagami,Ogata,Takahashi,Matsuda
, p. 1930 - 1934 (2001)
The H/D exchange reaction between CH4 and D2 was carried out over Rh/active-carbon catalysts, which were prepared from RhCl3 and Rh(NO3)3. In the case of the catalysts prepared from RhCl3, Rh species were homogeneously dispersed on the support from external surface to the inside of pores. Metallic particles of Rh were found to be the predominant species on the catalysts prepared from Rh(NO3)3 in the low Rh-loading region of 2 wt.%. The reaction rate per unit gram of catalyst and the product distribution in methane reflected well the Rh-dispersion on the catalysts. The catalysts which contained the highly dispersed Rh species as predominant species were found to be more active for the H/D exchange reaction than the catalysts with relatively large metal particles of Rh. On the former, the ratio of CH3D/CD4 was observed to be much higher than that on the latter.
Harris,Steacie
, p. 554 (1945)
Quantitative mechanochemical methanation of CO2 with H2O in a stainless steel ball mill
Sawama, Yoshinari,Niikawa, Miki,Ban, Kazuho,Park, Kwihwan,Aibara, Shin-Yo,Itoh, Miki,Sajiki, Hironao
, p. 1074 - 1078 (2020)
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Coillet,Harris
, p. 1486 (1953)
Urey,Price
, p. 300 (1934)
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Majury,Steacie
, (1953)
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Isotopic Excange in the Sonolysis of Aqueous Solutions Containing D2 and CH4
Hart, Edwin J.,Fischer, Ch.-Herbert,Henglein, Arnim
, p. 4166 - 4169 (1987)
Water was insonated under an argon atmosphere which contained various amounts of a D2-CH4 (2:1 vol percent) mixture.Maximum yield for the formation of CH3D, CH2D2, CHD3 and CD4 was observed at 40 vol percent argon.Ethane, ethylene, acetylene, and many higher hydrocarbons were also produced with about one third of the deuterated methane yield.In addition, some H/D exchange took place between D2 and H2O, and H2 was formed from water.Carbon monoxide and carbon were produced, too.A mechanism involving free radicals and atoms is discussed to explain these observations.
Catalytic activity of systems based on supported potassium salts of transition metal carbonyl hydrides in hydrogen-deuterium exchange of hydrocarbons
Yunusov,Rummel,Herrmann,Kalyuzhnaya,Shur
, p. 1191 - 1194 (2013)
The deposition of K2[Ru4(CO)13], K 2[Os3(CO)11], K2[Fe 2(CO)8], and K[Re(CO)5] onto graphite-like carbon Sibunit followed by the thermal decomposition of the supported carbonylmetallate in a flow of dihydrogen or argon affords systems capable of activating C-H bonds of methane, ethylene, and acetylene and of introducing them into hydrogen-deuterium exchange reactions. In the case of ethylene and acetylene, the isotope exchange proceeds at room temperature, while in the case of methane reaction temperatures not lower than 150 C are needed.
Dynamics of the formation of CD4 from the direct reaction of incident D atoms with CD3/Cu(111)
Rettner,Auerbach,Lee
, p. 10115 - 10122 (1996)
Using molecular beam techniques we find that incident D atoms can abstract CD3 from a Cu(111) surface to yield CD4 in a direct (Eley-Rideal) gas-surface reaction with a cross section of ～10-16 cm2/D atom. Dynamical evidence for a direct reaction includes the observation of an extremely sharp angular distribution that is clearly displaced from the surface normal, and the determination of a very high translational energy of the product, Ef, which is ～2 eV. For a 0.25 eV D-atom beam incident at 45° on a 95 K surface, this energy varies with the detection angle, θf, as Ef(θf) = (1.8+θf/45) eV, where θf0° in the "backscattering'' direction. For these conditions, the angular distribution approximately follows the function cos70(θf-5.5), being peaked 5.5° from the normal with a full width at half maximum of 60(θf-1.5). The reaction with 0.25 eV H incident at 45° gives a similar distribution peaked at ～3.5° from the normal. The shifts in the angular distributions are approximately consistent with parallel momentum conservation. The CD3/Cu(111) surface was prepared by thermal dissociation of CD3I on the surface or by adsorbing CD3 directly from a CD3 beam produced by the pyrolvsis of azomethane.
Hydrogenation of CO2 to Methanol by Pt Nanoparticles Encapsulated in UiO-67: Deciphering the Role of the Metal-Organic Framework
Gutter?d, Emil S.,Lazzarini, Andrea,Fjermestad, Torstein,Kaur, Gurpreet,Manzoli, Maela,Bordiga, Silvia,Svelle, Stian,Lillerud, Karl P.,Skúlason, Egill,?ien-?Degaard, Sigurd,Nova, Ainara,Olsbye, Unni
supporting information, p. 999 - 1009 (2020/02/20)
Metal-organic frameworks (MOFs) show great prospect as catalysts and catalyst support materials. Yet, studies that address their dynamic, kinetic, and mechanistic role in target reactions are scarce. In this study, an exceptionally stable MOF catalyst consisting of Pt nanoparticles (NPs) embedded in a Zr-based UiO-67 MOF was subject to steady-state and transient kinetic studies involving H/D and 13C/12C exchange, coupled with operando infrared spectroscopy and density functional theory (DFT) modeling, targeting methanol formation from CO2/H2 feeds at 170 °C and 1-8 bar pressure. The study revealed that methanol is formed at the interface between the Pt NPs and defect Zr nodes via formate species attached to the Zr nodes. Methanol formation is mechanistically separated from the formation of coproducts CO and methane, except for hydrogen activation on the Pt NPs. Careful analysis of transient data revealed that the number of intermediates was higher than the number of open Zr sites in the MOF lattice around each Pt NP. Hence, additional Zr sites must be available for formate formation. DFT modeling revealed that Pt NP growth is sufficiently energetically favored to enable displacement of linkers and creation of open Zr sites during pretreatment. However, linker displacement during formate formation is energetically disfavored, in line with the excellent catalyst stability observed experimentally. Overall, the study provides firm evidence that methanol is formed at the interface of Pt NPs and linker-deficient Zr6O8 nodes resting on the Pt NP surface.
