Adsorption of Formamide at the Surface of Amorphous and Crystalline Ices under Interstellar and Tropospheric Conditions. A Grand Canonical Monte Carlo Simulation Study

Kiss, Bálint; Picaud, Sylvain; Szőri, Milán; Jedlovszky, Pál

doi:10.1021/acs.jpca.9b00850

Cited by 15 publications

(17 citation statements)

References 106 publications

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“…In addition, the temperature dependence of μ 0 is shown in the inset of Figure . As is seen, similarly to other molecules, ,− the chemical potential value corresponding to the point of condensation of propylene oxide decreases linearly with increasing temperature.…”

Section: Resultssupporting

confidence: 57%

“…In other words, completion of the first layer clearly precedes the building up of the outer molecular layers at 200 K and the condensation of PO at lower temperatures. In this respect, PO behaves in a similar way as methylamine (with the only difference that methylamine exhibits multilayer adsorption even at as low temperature as 20 K) 44 and in a clearly different way than formamide 43 and cyanamide, 45 the condensation of which occurs well before the saturation of the first molecular layer.…”

Section: Properties Of the Adsorption Layermentioning

confidence: 95%

“…In particular, in a GCMC simulation, the chemical potential rather than the number of the adsorbate molecules is fixed in the system, and hence a set of GCMC simulations, in which the chemical potential of the adsorbate is systematically varied, can readily provide the adsorption isotherm. In fact, in the past two decades, the GCMC method has widely been used to study the adsorption of various molecular adsorbents at a number of different surfaces, such as carbonaceous materials, − covalent organic frameworks, , self-assembled monolayers, , zeolites, , metal oxides, − clay minerals (e.g., kaolinite), , and protein crystals, as well as inside clathrate hydrates − and at the surface of crystalline − and even of amorphous ice. − …”

Section: Introductionmentioning

confidence: 99%

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Adsorption of Propylene Oxide on Amorphous Ice under Interstellar Conditions. A Grand Canonical Monte Carlo Simulation Study

2020

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The adsorption of propylene oxide at the surface of amorphous ice at temperatures characteristic of various domains of the interstellar medium is investigated by grand canonical Monte Carlo computer simulations. It is found that the formation of a saturated monolayer, and even the occurrence of traces of a second layer, precedes the condensation of propylene oxide in the entire temperature range investigated of 35−200 K, and even multilayer adsorption occurs at 200 K. The adsorption isotherms exhibit non-Langmuir shape due to the considerable lateral interaction between the adsorbed molecules. The surface concentration of the saturated monolayer is estimated from that of the first molecular layer of condensed-phase propylene oxide as 6.75 ± 0.15 μmol/m 2 . Adsorbed propylene oxide molecules of the first molecular layer are found to preferentially align in such a way that their threemember ring lays parallel to the macroscopic plane of the ice surface, and they typically form one hydrogen bond with the surface water molecules. The adsorption energy and heat of adsorption at infinitely low surface coverage are estimated to be −51.8 ± 3.6 kJ/mol and −51.0 ± 3.7 kJ/mol, respectively. Our results indicate that considering its astrochemically relevant concentration range, adsorption of propylene oxide on amorphous ice can only be expected to occur in the lowest temperature domains of the interstellar medium and involves a highly unsaturated adsorption layer.

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Section: Resultssupporting

confidence: 57%

Section: Properties Of the Adsorption Layermentioning

confidence: 95%

Section: Introductionmentioning

confidence: 99%

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Adsorption of Propylene Oxide on Amorphous Ice under Interstellar Conditions. A Grand Canonical Monte Carlo Simulation Study

2020

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“…The LDA phase (Figure 1b) has been created as described in Refs. 37,38 , i.e., by thermalizing first the Ih phase at 300 K with 10 8 Monte Carlo (MC) steps long followed by a 2 × 10 8 MC steps at 350 K, and another 10 8 MC steps again at 300 K. Finally, the system has been quenched to 200 K, and equilibrated for another 10 8 MC steps at this temperature.…”

Section: Simulations Detailsmentioning

confidence: 99%

Adsorption of CO and N2 molecules at the surface of solid water. A grand canonical Monte Carlo study

Patt

Simon

Salazar

et al. 2020

The Journal of Chemical Physics

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The adsorption of carbon monoxide and nitrogen molecules at the surface of four forms of solid water is investigated by means of grand canonical Monte Carlo simulations. The trapping ability of crystalline Ih and low-density amorphous ices, along with clathrate hydrates of structures I and II, are compared at temperatures relevant for astrophysics. It is shown that, when considering a gas phase that contains mixtures of carbon monoxide and nitrogen, the trapping of carbon monoxide is favored with respect to that of nitrogen at the surface of all solids, irrespective of the temperature. The results of the calculations also indicate that some amounts of molecules can be incorporated in the bulk of the water structures and the molecular selectivity of the incorporation process is investigated. Again, it is shown that the incorporation of carbon monoxide is favored with respect to that of nitrogen in most of the situations considered here. In addition, the conclusions of the present simulations emphasize the importance of the strength of the interactions between the guest molecules and the water network. They indicate that the accuracy of the corresponding interaction potentials is a key point, especially for simulating clathrate selectivity. This highlights the necessity of having interaction potential models that are transferable to different water environments.

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“…Thus, performing a set of GCMC simulations in which the adsorbate chemical potential is systematically varied and, as its function, the number of adsorbed molecules is determined, the adsorption isotherm can readily be calculated. Indeed, the GCMC method was successfully applied to investigate the adsorption of a number of small adsorbate molecules on various adsorbents, such as self-assembled monolayers, , carbonaceous materials, − metal oxides, − clay minerals, , zeolites, , covalent organic frameworks, , protein crystals, clathrate hydrates, − and crystalline − and amorphous ice. , …”

Section: Introductionmentioning

confidence: 99%

Computer Simulation Investigation of the Adsorption of Cyanamide on Amorphous Ice at Low Temperatures

2020

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The adsorption of cyanamide at the surface of low density amorphous (LDA) ice is studied by grand canonical Monte Carlo simulations in the temperature range of 50–200 K, under conditions characteristic of the interstellar medium and prebiotic Earth. The obtained results show that the adsorption is strictly monomolecular; moreover, condensation of cyanamide even precedes the saturation of the adsorption monolayer in the entire temperature range studied. Adsorbed cyanamide molecules are found to form altogether 3–4 hydrogen bonds with each other and with the surface water molecules at every surface concentration. As a consequence, their adsorption is strongly an exothermic process and hence becomes progressively more pronounced with decreasing temperature. Lateral H-bonding between the adsorbed cyanamide molecules leads to their noticeable clustering, evidenced also by the non-Langmuir character of the adsorption isotherm, becoming more pronounced at lower temperatures. Besides adsorption, cyanamide molecules are also found to be able to dissolve in the bulk LDA phase in a noticeable extent. However, contrary to the surface adsorption, dissolution turns out to be an entropy-driven, endothermic process and hence becomes more pronounced at higher rather than at lower temperatures.

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Adsorption of Formamide at the Surface of Amorphous and Crystalline Ices under Interstellar and Tropospheric Conditions. A Grand Canonical Monte Carlo Simulation Study

Cited by 15 publications

References 106 publications

Adsorption of Propylene Oxide on Amorphous Ice under Interstellar Conditions. A Grand Canonical Monte Carlo Simulation Study

Adsorption of Propylene Oxide on Amorphous Ice under Interstellar Conditions. A Grand Canonical Monte Carlo Simulation Study

Adsorption of CO and N2 molecules at the surface of solid water. A grand canonical Monte Carlo study

Computer Simulation Investigation of the Adsorption of Cyanamide on Amorphous Ice at Low Temperatures

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