Clathrate–hydrate ultrafast nucleation and crystallization from supercooled aqueous nanodroplets

Devlin, J. Paul; Monreal, I. Abrrey

doi:10.1016/j.cplett.2010.03.072

Cited by 28 publications

(35 citation statements)

References 40 publications

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“…As originally, 19 that method consists of premixing both the potential host and guest component vapors within a carrier gas at appropriate partial pressures. Upon pulsing into a cold chamber the vapors convert to solution nanodroplets which transition to ~100% CHs, all on a subsecond timescale.…”

Section: Hcl/dcl Ch Spectra From All-vapor Premixturesmentioning

confidence: 99%

Molecular Modes and Dynamics of HCl and DCl Guests of Gas Clathrate Hydrates

et al. 2015

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Recent years have yielded advances in the placement of unusual molecules as guests within clathrate hydrates (CHs) without severe distortion of the classic lattice structures. Reports describing systems for which observable but limited distortion does occur are available for methanol, ammonia, acetone, and small ether molecules. In these particular examples, the large-cage molecules often participate as non-classical guests H-bonded to the cage walls. Here, we expand the list of such components to include HCl/DCl and HBr as small-cage guests. Based on FTIR spectra of nanocrystalline CHs from two distinct preparative methods combined with critical insights derived from on-the-fly molecular dynamics and ab initio computational data, a coherent argument emerges that these strong acids serve as a source of molecular small-cage guests, ions, and orientational defects. Depending on the HCl/DCl content the ions, defects and molecular guests determine the CH structures, some of which form in sub-seconds via an all-vapor preparative method.

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Section: Hcl/dcl Ch Spectra From All-vapor Premixturesmentioning

confidence: 99%

Molecular Modes and Dynamics of HCl and DCl Guests of Gas Clathrate Hydrates

et al. 2015

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“…13,14 (This is not the case for the all-vapor method, since all of the CH components within the liquid droplets are naturally mixed at the molecular level. 21 Nevertheless, a catalyst is required for mobility; presumably to erase structural defects that arise during the subsecond crystallization. 10 ) Though others prefer to label molecules associated with such action as "promoters," a basic correctness of the term "catalyst" will be argued below from low-temperature kinetic data 14 and modern computational insights.…”

Section: Introductionmentioning

confidence: 99%

“…This conclusion is based on new data obtained using the all-vapor method of clathrate-hydrate formation. [19][20][21][22] The all-vapor aerosol approach to the sub-second formation of CHs, including formation of CHs with gas molecules populating the small cages, was first described in 2010. 21 The subsequent use of the all-vapor methodology, as a tool in the study of the properties of gas CHs and of the conditions under which the sub-second formation of numerous mixed CHs are optimized, has resulted in more recent reports.…”

Section: Introductionmentioning

confidence: 99%

Catalytic activity of methanol in all-vapor subsecond clathrate-hydrate formation

Devlin

2014

The Journal of Chemical Physics

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Methanol's property as a catalyst in the formation of gas clathrate hydrates has been recognized for several years and was recently employed in a broad ranging study [K. Shin, K. A. Udachin, I. L. Moudrakovski, D. M. Leek, S. Alavi, C. I. Ratcliffe, and J. A. Ripmeester, Proc. Natl. Acad. Sci. U.S.A. 110, 8437 (2013)]. A new measure of that activity is offered here from comparative rates of formation of methanol (MeOH) clathrate hydrates within our all-vapor aerosol methodology for which tetrahydrofuran (THF) and other small ethers have set a standard for catalytic action. We have previously described numerous examples of the complete conversion of warm all-vapor mixtures to aerosols of gas clathrate hydrates on a sub-second time scale, generally with the catalyst confined primarily to the large cage of either structure-I (s-I) or structure-II (s-II) hydrates. THF has proven to be the most versatile catalyst for the complete subsecond conversion of water to s-II hydrate nanocrystals that follows pulsing of appropriate warm vapor mixtures into a cold chamber held in the 140-220 K range. Here, the comparative ability of MeOH to catalyze the formation of s-I hydrates in the presence of a small-cage help-gas, CO2 or acetylene, is examined. The surprising result is that, in the presence of either help gas, CH-formation rates appear largely unchanged by a complete replacement of THF by MeOH in the vapor mixtures for a chamber temperature of 170 K. However, as that temperature is increased, the dependence of effective catalysis by MeOH on the partial pressure of help gases also increases. Nevertheless, added MeOH is shown to markedly accelerate the s-II THF-CO2 CH formation rate at 220 K.

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“…For this reason, a variety of studies on hydrate promoters has been performed to reduce the equilibrium pressure. In addition, CO2 hydrate formation using supercooled aqueous nanodroplets [13] and using others such as ice at temperatures just below 273 K [14] or ice melting water [15] may also be a potential candidate for rapid CO2 hydrate growth. Either way, it will be possible to reduce the energy consumed in the hydrate method.…”

Section: Boosting Energy and Cost Of The Collected Co2mentioning

confidence: 99%

A Feasibility Study on Hydrate-Based Technology for Transporting CO2 from Industrial to Agricultural Areas

et al. 2017

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Climate change caused by global warming has become a serious issue in recent years. The main purpose of this study was to evaluate the effectiveness of the above system to quantitatively supply CO2 or CO2 hydrate from industrial to agricultural areas. In this analysis, several transportation methods, namely, truck, hydrate tank lorry, and pipeline, were considered. According to this analysis, the total CO2 supply costs including transportation ranged from 15 to 25 yen/kg-CO2 when the transportation distance was 50 km or less. The cost of the hydrate-based method increased with the transport distance in contrast to the liquefied CO2 approach. However, the technology of supplying CO2 hydrate had merit by using a local cooling technique for cooling specific parts of agricultural products.

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Clathrate–hydrate ultrafast nucleation and crystallization from supercooled aqueous nanodroplets

Cited by 28 publications

References 40 publications

Molecular Modes and Dynamics of HCl and DCl Guests of Gas Clathrate Hydrates

Molecular Modes and Dynamics of HCl and DCl Guests of Gas Clathrate Hydrates

Catalytic activity of methanol in all-vapor subsecond clathrate-hydrate formation

A Feasibility Study on Hydrate-Based Technology for Transporting CO2 from Industrial to Agricultural Areas

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