Abstract:International audienceOriginal calorimetric and phase equilibrium properties for hydrogen + tetrabutylammonium bromide (TBAB), tetrabutylammonium chloride (TBACl), or tetrabutylphosphonium bromide (TBPB) semiclathrate hydrates were measured using differential scanning calorimetry under pressure. The dissociation temperatures of H2 + TBACl and H2 + TBPB semiclathrate hydrates are very close to the ambient temperature at low pressures around 15.0 MPa. H2 + TBACl and H2 + TBPB systems therefore exhibit better and… Show more
“…11,[16][17][18][19][20][21][22] TBAB has also been examined for its potential to separate methane from coal methane gas. 23,24 However, the methane concentrations in these studies were relatively high, over 25 vol%.…”
This paper reports the experimentally measured phase equilibrium conditions for the clathrate hydrates formed from simulated mine ventilation air (0.50 vol% CH 4 + 99.50 vol% air) in the presence of 0, 5, 20, 37.1 and 50 wt% of Tetrabutylphosphonium Bromide (TBPB).These equilibrium conditions were measured at the temperature range of (281.62 to 292.49) K and pressure range of (1.92 to 18.55) MPa by using an isochoric equilibrium step-heating pressure search method. The results showed that addition of TBPB allowed the hydrate dissociation condition for mine ventilation air to become milder and at a given temperature, the lowest hydrate dissociation pressure was achieved at 37.1 wt% TBPB, corresponding to the stoichiometric composition for TBPB·32H 2 O. For each TBPB concentration tested, the semilogarithmic plots of hydrate dissociation pressure versus reciprocal absolute temperature can be satisfactorily fitted to two straight lines intersecting at 6.5 MPa. The slopes of these fitted straight lines are indifferent to changes in TBPB concentration. Gas composition analysis by gas chromatography also found that in the presence of 37.1 wt% TBPB, CH 4 could be enriched approximately 3.5-fold in the hydrate phase.
“…11,[16][17][18][19][20][21][22] TBAB has also been examined for its potential to separate methane from coal methane gas. 23,24 However, the methane concentrations in these studies were relatively high, over 25 vol%.…”
This paper reports the experimentally measured phase equilibrium conditions for the clathrate hydrates formed from simulated mine ventilation air (0.50 vol% CH 4 + 99.50 vol% air) in the presence of 0, 5, 20, 37.1 and 50 wt% of Tetrabutylphosphonium Bromide (TBPB).These equilibrium conditions were measured at the temperature range of (281.62 to 292.49) K and pressure range of (1.92 to 18.55) MPa by using an isochoric equilibrium step-heating pressure search method. The results showed that addition of TBPB allowed the hydrate dissociation condition for mine ventilation air to become milder and at a given temperature, the lowest hydrate dissociation pressure was achieved at 37.1 wt% TBPB, corresponding to the stoichiometric composition for TBPB·32H 2 O. For each TBPB concentration tested, the semilogarithmic plots of hydrate dissociation pressure versus reciprocal absolute temperature can be satisfactorily fitted to two straight lines intersecting at 6.5 MPa. The slopes of these fitted straight lines are indifferent to changes in TBPB concentration. Gas composition analysis by gas chromatography also found that in the presence of 37.1 wt% TBPB, CH 4 could be enriched approximately 3.5-fold in the hydrate phase.
“…In addition, the QAS semiclathrates have small 5 12 cages which are left vacant and thus, can be used for capturing small-sized gas molecules [19,22,23,[25][26][27][28][31][32][33][34][35][36][37][38][39][40][41]. Due to their significant thermodynamic stability and guest gas enclathrating ability, QAS semiclathrates have been investigated as an alternative to gas hydrates for gas storage and separation [23,27,31,[42][43][44][45][46][47][48].…”
“…SCHs have drawn increasing interest for their potential applications in gas storage [18][19] and gas separation [20,21]. Several studies of this kind have addressed coal methane gas with relatively high original methane concentrations (e.g., close to or over 30 mol%) [22][23][24].…”
Abatement of methane from mine ventilation air (MVA) is a significant challenge faced by coal mining industry. A promising method for methane capture from gas mixture is clathrate hydrate formation. In search of suitable and costeffective low-dosage promoters for hydrate-based methane capture processes, this paper reports the pressure requirement for the hydrate formation of simulated MVA (0.5 vol% CH 4 + 99.5 vol% air) and its potential for methane extraction, in the presence of tri-n-butyl phosphine oxide (TBPO) or tetra-n-butyl ammonium bromide (TBAB) at three different initial loadings (5 wt%, 15 wt%, and 26 wt%). An isochoric equilibrium step-heating pressure search method was used to measure the hydrate phase equilibrium conditions at the temperature range of (277.61 to 295.54) K and pressure range of (0.23 to 19.11) MPa. It was found that at a given initial loading, TBPO was largely more effective than TBAB in reducing the pressure requirement for hydrate formation of MVA. At a given temperature, the equilibrium pressures of the clathrate hydrates were indifferent to the change in the initial loading of TBPO from 5 wt% to 26 wt%, in contrast to those of TBAB. Gas composition analysis by gas chromatography confirmed that CH 4 could be significantly enriched in the ionic clathrate hydrates, and the highest methane enrichment ratio obtained in the present work was 300%, with TBPO at initial loading of 5 wt%. At this relatively low loading, within a given period of 5 hours, TBPO also led to higher gas uptake compared with TBAB. The advantages of TBPO as a promoter of MVA hydrate were discussed.
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