Molecular insight into the micro-behaviors of CH4 and CO2 in montmorillonite slit-nanopores

Abstract

The Grand Canonical Monte Carlo (GCMC) and molecular dynamics (MD) simulation methods were used to investigate the adsorption and diffusion properties of CH₄ and CO₂ in montmorillonite slit-nanopores. It is found that, both CH₄ and CO₂ could adsorb closely onto the pore surface, while different adsorption states occur for CH₄ and CO₂, respectively, in montmorillonite slit-nanopores. Competitive adsorption of CO₂ over CH₄ exists in montmorillonite slit-nanopores, especially at the lower pressures, which is attributed to the different interaction intensity between the CH₄–CO₂ molecules and the pore surface. The diffusion coefficients of CH₄ and CO₂ both decrease with the enhanced pressures, while the CO₂ has a relative weak diffusion coefficient comparing with CH₄. A well displacement of the residual CH₄ by CO₂ in montmorillonite slit-nanopores was investigated, which is found that the displacement efficiency increases with the enhanced bulk pressures. It was determined that, the CO₂ can be captured and reserved in the montmorillonite slit-nanopores during the displacement, and the sequestration amount of CO₂ gets enhanced with the bulk pressure increasing. This study provides micro-behaviours of CH₄ and CO₂ in montmorillonite slit-nanopores, for the purpose to give out useful guidance for enhancing shale gas extraction by injecting CO₂.     

Adsorption and diffusion of CO2 and CH4 in covalent organic frameworks: an MC/MD simulation study

Covalent organic frameworks (COFs) are a promising gas separation material which have been developed recently. In this work, we have used grand canonical Monte Carlo (GCMC) and molecular dynamics (MD) simulations to investigate the adsorption and diffusion properties of CO₂ and CH₄ in five recent synthesised COF materials. We have also considered the properties of amino-modified COFs by adding –NH₂ group to the five COFs. The adsorption isotherm, adsorption/diffusion selectivity, self/transport diffusion coefficients have been examined and discussed. All of the five COFs exhibit promising adsorption selectivity which is higher than common nanoporous materials. An S-shaped adsorption isotherm can be found for CO₂ instead of CH₄ adsorption. The introduction of –NH₂ group is effective at low pressure region (<200?kPa). The diffusion coefficients are similar for TS-COFs but increase with the pore size for PI-COFs, and the diffusion coefficients seem less dependent on the –NH₂ groups.     

Molecular simulation of CO2, N2 and CH4 adsorption and separation in ZIF-78 and ZIF-79

In this study, we investigated the adsorption and separation behaviours of CO₂, N₂ and CH₄ in ZIF-78 and ZIF-79 by means of grand canonical Monte Carlo methods. Our simulations indicate that preferential adsorption sites are mainly located at the regions where guest molecules can maximise interactions with the imidazolate (IM) linkers. The –NO₂ and –CH₃ functional groups are not the major binding sites that directly bind the guest molecules. Instead, they alter the electronic structure and polarity of the adjacent IM linkers to affect the adsorption behaviours. In addition, we found that the selectivity of CO₂ over N₂ or CH₄ is found to be dependent on the component fractions of CO₂/N₂ and CO₂/CH₄ mixtures. Specifically, the selectivity of CO₂ over N₂ increases with CO₂ composition fraction, while the trend for the selectivity of CO₂/CH₄ was opposite.     

Modeling the adsorptive selectivity of carbon nanotubes for effective separation of CO2/N2 mixtures

Canonical Monte Carlo (CMC) simulations were carried out to investigate the behavior of CO₂ and N₂ mixtures upon adsorption on single walled carbon nanotubes (CNTs). In the simulation, all the particle–particle interactions between CO₂, N and C were modeled using Lennard-Jones (LJ) potential. To provide deep insight into the effect of pore width, temperature, pressure and bulk composition on the adsorption behavior of CO₂ /N₂ mixtures, five different CNTs [(6,6), (7,7), (8,8) (9,9) and (10,10) CNT] with diameters ranging from 0.807 to 1.35 nm, three temperatures (300 323 and 343 K), six pressures (0.15, 2, 4, 6, 8 and 10 MPa), and three bulk mole compositions of carbon dioxide (0.3 0.5 and 0.7) were tested. The results from all the simulation conditions investigated in this work show that CNTs preferentially adsorb carbon dioxide relative to nitrogen in a binary mixture. The results are consistent with the hypothesis that stronger interaction of one component with the nanotube surface results in a higher adsorption capacity compared to the other component. An optimized pore size of D = 8.07 nm corresponding to (6, 6) CNT, at T = 300 K and P = 0.15 MPa at a bulk mole composition of y_CO2 =0.3 was identified in which carbon nanotubes demonstrate the greatest selectivity for separation of carbon dioxide relative to nitrogen. In addition, it is worth pointing out that, under similar simulation conditions, CNTs exhibit higher selectivity compared to other carbon-based materials [carbon membrane polyimide (PI) and PI/multi-wall carbon nanotubes (MWCNTs)] for CO₂ adsorption. As a prototype, the selectivity of an equimolar mixture of CO₂ /N₂ for adsorption on (6, 6) CNTs at 300 K and 0.15 MPa reaches 9.68, which is considerably larger than that reported in carbon membrane. Therefore, it can be concluded that carbon nanotubes can act as a capable adsorbent for adsorption/desorption of CO₂ in comparison with other carbon-based materials in the literature.     

Gas adsorption and diffusion in a highly CO2 selective metal–organic framework: molecular simulations

Grand canonical Monte Carlo and equilibrium molecular dynamics simulations were used to assess the performance of an rht-type metal–organic framework (MOF), Cu-TDPAT, in adsorption-based and membrane-based separation of CH₄/H₂, CO₂/CH₄ and CO₂/H₂ mixtures. Adsorption isotherms and self-diffusivities of pure gases and binary gas mixtures in Cu-TDPAT were computed using detailed molecular simulations. Several properties of Cu-TDPAT such as adsorption selectivity, working capacity, diffusion selectivity, gas permeability and permeation selectivity were computed and compared with well-known zeolites and MOFs. Results showed that Cu-TDPAT is a very promising adsorbent and membrane material especially for separation of CO₂ and it can outperform traditional zeolites and MOFs such as DDR, MFI, CuBTC, IRMOF-1 in adsorption-based CO₂/CH₄ and CO₂/H₂ separations.     

Biogas upgrading using single-walled carbon nanotubes by molecular simulation

Abstract

Biogas from anaerobic digestion of biological wastes is a renewable energy resource that mainly contains CH₄, CO₂, trace amounts of H₂S and a fraction of H₂O vapour. In order to transfer biogas into biomethane to meet the standards for use as vehicle fuel or for injection in the natural gas grid, removing H₂S from biogas in advance is necessary. In addition, biogas is usually saturated with water vapour. It is significant to study the effect of the presence of H₂O on the biogas separation performance. Adsorption of H₂S/CO₂/CH₄ and H₂O/CO₂/CH₄ ternary mixtures using single-walled carbon nanotubes (SWCNT) were investigated via the Grand Canonical Monte Carlo (GCMC) method. We studied the effects of carbon nanotube diameter, –COOH modification, temperature and pressure on H₂S adsorption. The results indicate that the presence of hydrophilic –COOH groups does affect the separation of H₂S/CO₂/CH₄ mixtures. Temperature swing adsorption is more suitable than pressure swing adsorption for the separation of H₂S/CO₂/CH₄ mixtures. The effect of water vapour on the separation of CO₂/CH₄ was also investigated. The result shows that the presence of H₂O has little effect on the selectivity of CO₂/CH₄ in pristine CNT, but the selectivity of CO₂/CH₄ with the presence of H₂O is markedly enhanced after modification in –COOH modified SWCNT with specific modification degree. It is expected that this work could provide some useful information for biogas upgrading.     

Computer simulation of gas adsorption in modified COF-108: the impregnation of C60 into COF-108

Gas adsorption and separation performance of COF-108 framework impregnated by C₆₀ clusters were simulated. The adsorption properties of pure CO₂, the mixtures of CO₂/CH₄, CO₂/N₂ and N₂/O₂ were investigated. The simulated results of the adsorption isotherms, the adsorption quantity, the density fields, the isosteric heats and the selectivity in COF-108s were obtained. It is shown that the impregnation of C₆₀ can enhance the adsorption capacity of CO₂, N₂ and O₂, and the selectivity of CO₂/CH₄, CO₂/N₂ and N₂/O₂ in COF-108. The impregnation of C₆₀ can increase the surface area COF-108 but decrease its free volume and the pore diameter. At low adsorption pressures, the monolayer surface adsorption is dominant. With the increase in adsorption pressure, the dominant factor is changed into the free volume of COF-108 by the multilayer adsorption. The impregnation of C₆₀ plays different roles for the polar or non-polar gases at different pressures.     

Hydrophilicity effect on CO2/CH4 separation using carbon nanotube membranes: insights from molecular simulation

Abstract

Molecular simulation methods were applied to study the effect of hydrophilicity on CO₂/CH₄ separation using carbon nanotube (CNT) membranes. CNTs with a diameter of ~1 nm were functionalised by varying amounts of carbonyl groups, in order to achieve various hydrophilicity. The presence of –CO groups inside the CNT allow a significant gain in the diffusion selectivity of CO₂, while in contrast the adsorption selectivity is hardly changed. The corresponding permeation selectivity increases as the hydrophilicity of the CNT-based membrane increases. However, the permeability of CO₂ decreases due to a combination of the intermolecular interactions between the gas and functional groups and the steric effects of the added functional groups. Considering both the permeation selectivity and permeability, it was found that the maximum separation performance is achieved in a certain hydrophilic CNT membrane. Moreover, the separation performance of hydrophilic CNTs for CO₂/CH₄ mixtures breaks the Robeson upper bound.     

Monte Carlo Simulation Study of Adsorption Characteristics in Slit-Like Micropores Under Supercritical Conditions

Abstract

Adsorption characteristics of a solute diluted in supercritical fluids has been investigated by using the Monte Carlo simulation techniques. The Lennard-Jones potential function is used for describing interactions for a model system of CO₂ + benzene in slit-like micropores with infinite graphitic carbon walls. A modified μVT ensemble method with particle exchange proposed by Cracknell, Nicholson and Quirke (1993) is found to be much superior to the conventional μVT ensemble method especially for dense mixtures in a pore. Adsorption isotherms of CO₂ and benzene, in equilibrium with a dilute benzene mixture in CO₂ (mole fraction of benzene = 0.001), are computed by varying pressure, temperature, the benzene–surface interaction potential, and the slitwidth. Adsorption isotherm curve of CO₂ increases with an increase in pressure while that of benzene shows a maximum at a pressure far below the critical pressure of CO₂ and then it decreases with increasing pressure. The decrease in benzene adsorption with increasing pressure is attributable to both the enhanced solubility in supercritical CO₂ and the competitive adsorption of CO₂. The isotherm curves of each component at two temperatures, 313.2 K and 323.2 K, show to cross at a pressure near the critical pressure due to the “density effect” on the chemical potentials of a solute at supercritical fluid conditions. When the interaction between a solute and a surface increases, the adsorption isotherm increases. Narrowing the slitwidth results in the increase in the adsorption of solute since the external potential from two walls becomes deeper.     

Transitional slopes act as hotspots of both soil CO<Subscript>2</Subscript> emission and CH<Subscript>4</Subscript> uptake in a temperate forest landscape

Forest soils are an important component of CO₂ and CH₄ fluxes at the global scale, but the magnitude of these fluxes varies greatly in space and time within a landscape. Understanding the spatial and temporal distributions of these fluxes across complex landscapes remains a major challenge for researchers and land managers alike. We investigated the spatiotemporal variability of soil-atmosphere CO₂ and CH₄ fluxes and the relationships of these fluxes to chemical and physical soil properties distributed across a topographically-heterogeneous landscape. Soil CO₂ and CH₄ fluxes were measured along with soil temperature, moisture, bulk density, texture, carbon, sorption capacity, and dissolved organic matter quality over 2 years along hillslope transects spanning valley bottom, transition zone, and upland landscape positions in a temperate forest watershed. Transition zone soil CO₂ efflux was 54–160% higher than low-lying valley bottoms, and 15–54% higher than uplands. Net seasonal CH₄ uptake was 58–150% higher in transition zone soils than in uplands, while valley bottoms were occasionally large net sources (up to 19 nmol CH₄ m^?2 s^?1). Soil CO₂ efflux and net CH₄ uptake were both positively associated with seasonal temperature, and were highest in soils with relatively high carbon and clay content, and relatively low bulk density, moisture, and sorption capacity. We concluded that: (1) transition zone soils act as landscape hotspots for net CH₄ uptake in addition to CO₂ efflux, and (2) that this spatial distribution is more consistent across seasons for net CH₄ uptake than for CO₂ efflux.     

Patterns in CH4 and CO2 concentrations across boreal rivers: Major drivers and implications for fluvial greenhouse emissions under climate change scenarios

It is now widely accepted that boreal rivers and streams are regionally significant sources of carbon dioxide (CO₂), yet their role as methane (CH₄) emitters, as well as the sensitivity of these greenhouse gas (GHG) emissions to climate change, are still largely undefined. In this study, we explore the large‐scale patterns of fluvial CO₂ and CH₄ partial pressure (pCO₂, pCH₄) and gas exchange (k) relative to a set of key, climate‐sensitive river variables across 46 streams and rivers in two distinct boreal landscapes of Northern Québec. We use the resulting models to determine the direction and magnitude of C‐gas emissions from these boreal fluvial networks under scenarios of climate change. River pCO₂ and pCH₄ were positively correlated, although the latter was two orders of magnitude more variable. We provide evidence that in‐stream metabolism strongly influences the dynamics of surface water pCO₂ and pCH₄, but whereas pCO₂ is not influenced by temperature in the surveyed streams and rivers, pCH₄ appears to be strongly temperature‐dependent. The major predictors of ambient gas concentrations and exchange were water temperature, velocity, and DOC, and the resulting models indicate that total GHG emissions (C‐CO₂ equivalent) from the entire network may increase between by 13 to 68% under plausible scenarios of climate change over the next 50 years. These predicted increases in fluvial GHG emissions are mostly driven by a steep increase in the contribution of CH₄ (from 36 to over 50% of total CO₂‐equivalents). The current role of boreal fluvial networks as major landscape sources of C is thus likely to expand, mainly driven by large increases in fluvial CH₄ emissions.     

Simulation of separation of C2H6 from CH4 using zeolitic imidazolate frameworks

Separation of important chemical feedstocks, such as C₂H₆ from natural gas, can greatly benefit the petrochemical industry. In this paper, the grand canonical Monte Carlo method has been used to study the adsorption and separation of CH₄ and C₂H₆ in zeolites, isoreticular metal-organic framework-1 (IRMOF-1) and zeolitic imidazolate frameworks (ZIFs) with different topology, including soadlite, gmelinite and RHO topologies. Compared with mordenite zeolite and IRMOF-1, ZIFs and mordenite framework inverted (MFI) zeolite have better separation performance for C₂H₆/CH₄ mixtures at different mole fractions of C₂H₆. From the study of equilibrium snapshots and density distribution profiles, adsorption sites could be grouped as (1) sites with strong interactions with adsorbent and (2) sites with strong interactions with surrounding adsorbates. The gas molecules occupied the first site and then went on to occupy the second site. In CH₄/C₂H₆ mixture adsorption/separation, the adsorption of CH₄ was confined by the existence of C₂H₆. Due to energetic effect, C₂H₆ selectivity was affected by temperature at a low-pressure range, but did not change as much in a high-pressure range because of packing effect in micropore. In binary adsorption, large C₂H₆ molecules favour sites with strong adsorbent interactions. At high pressures, packing effects played an important role and it became easy for small CH₄ molecules to access the sites with strong adsorbate interactions.     

Function and limits of biofilters for the removal of methane in exhaust gases from the pig industry

The agricultural sector is responsible for an important part of Canadian greenhouse gas (GHG) emissions, 8 % of the 747 Mt eq. CO₂ emitted each year. The pork industry, a key sector of the agrifood industry, has had a rapid growth in Canada since the middle 1980s. For this industry, slurry storage accounts for the major part of methane (CH₄) emissions, a GHG 25 times higher than carbon dioxide (CO₂) on a 100-year time horizon. Intending to reduce these emissions, biofiltration, a process effective to treat CH₄ from landfills and coal mines, could be effective to treat CH₄ from the pig industry. Biofiltration is a complex process that requires the understanding of the biological process of CH₄ oxidation and a control of the engineering parameters (filter bed, temperature, etc.). Some biofiltration studies show that this technology could be used to treat CH₄ at a relatively low cost and with a relatively high purification performance.     

Opposing seasonal temperature dependencies of CO2 and CH4 emissions from wetlands

Wetlands are critically important to global climate change because of their role in modulating the release of atmospheric greenhouse gases (GHGs) carbon dioxide (CO₂) and methane (CH₄). Temperature plays a crucial role in wetland GHG emissions, while the general pattern for seasonal temperature dependencies of wetland CO₂ and CH₄ emissions is poorly understood. Here we show opposite seasonal temperature dependencies of CO₂ and CH₄ emissions by using 36,663 daily observations of simultaneous measurements of ecosystem-scale CO₂ and CH₄ emissions in 42 widely distributed wetlands from the FLUXNET-CH₄ database. Specifically, the temperature dependence of CO₂ emissions decreased with increasing monthly mean temperature, but the opposite was true for that of CH₄ emissions. Neglecting seasonal temperature dependencies may overestimate wetland CO₂ and CH₄ emissions compared to the use of a year-based static and consistent temperature dependence parameter when only considering temperature effects. Our findings highlight the importance of incorporating the remarkable seasonality in temperature dependence into process-based biogeochemical models to predict feedbacks of wetland GHG emissions to climate warming.     

Increased night temperature reduces the stimulatory effect of elevated carbon dioxide concentration on methane emission from rice paddy soil

To determine how elevated night temperature interacts with carbon dioxide concentration ([CO₂]) to affect methane (CH₄) emission from rice paddy soil, we conducted a pot experiment using four controlled‐environment chambers and imposed a combination of two [CO₂] levels (ambient: 380 ppm; elevated: 680 ppm) and two night temperatures (22 and 32 °C). The day temperature was maintained at 32 °C. Rice (cv. IR72) plants were grown outside until the early‐reproductive growth stage and then transferred to the chambers. After onset of the treatment, day and night CH₄ fluxes were measured every week. The CH₄ fluxes changed significantly with the growth stage, with the largest fluxes occurring around the heading stage in all treatments. The total CH₄ emission during the treatment period was significantly increased by both elevated [CO₂] (P=0.03) and elevated night temperature (P<0.01). Elevated [CO₂] increased CH₄ emission by 3.5% and 32.2% under high and low night temperature conditions, respectively. Elevated [CO₂] increased the net dry weight of rice plants by 12.7% and 38.4% under high and low night temperature conditions, respectively. These results imply that increasing night temperature reduces the stimulatory effect of elevated [CO₂] on both CH₄ emission and rice growth. The CH₄ emission during the day was larger than at night even under the high‐night‐temperature treatment (i.e. a constant temperature all day). This difference became larger after the heading stage. We observed significant correlations between the night respiration and daily CH₄ flux (P<0.01). These results suggest that net plant photosynthesis contributes greatly to CH₄ emission and that increasing night temperature reduces the stimulatory effect of elevated [CO₂] on CH₄ emission from rice paddy soil.     

Tunable Polyaniline‐Based Porous Carbon with Ultrahigh Surface Area for CO2 Capture at Elevated Pressure

Natural gas is the cleanest fossil fuel source. However, natural gas wells typically contain considerable amounts of CO₂, with on‐site CO₂ capture necessary. Solid sorbents are advantageous over traditional amine scrubbing due to their relatively low regeneration energies and non‐corrosive nature. However, it remains a challenge to improve the sorbent's CO₂ capacity at elevated pressures relevant to natural gas purification. Here, the synthesis of porous carbons derived from a 3D hierarchical nanostructured polymer hydrogel, with simple and effective tunability over the pore size distribution is reported. The optimized surface area reaches 4196 m² g^?1, which is among the highest of carbon‐based materials, with abundant micro‐ and narrow mesopores (2.03 cm³ g^?1 with d < 4 nm). This carbon exhibits a record‐high CO₂ capacity among reported carbons at elevated pressure (i.e., 28.3 mmol g^?1 total adsorption at 25 °C and 30 bar). This carbon also shows good CO₂/CH₄ selectivity and excellent cyclability. Molecular simulations suggest increased CO₂ density in micro‐ and narrow mesopores at high pressures. This is consistent with the observation that these pores are mainly responsible for the material's high‐pressure CO₂ capacity. This work provides insights into material design and further development for CO₂ capture from natural gas.     

Large‐scale patterns in summer diffusive CH4 fluxes across boreal lakes,and contribution to diffusive C emissions

Lakes are a major component of boreal landscapes, and whereas lake CO₂ emissions are recognized as a major component of regional C budgets, there is still much uncertainty associated to lake CH₄ fluxes. Here, we present a large‐scale study of the magnitude and regulation of boreal lake summer diffusive CH₄ fluxes, and their contribution to total lake carbon (C) emissions, based on in situ measurements of concentration and fluxes of CH₄ and CO₂ in 224 lakes across a wide range of lake type and environmental gradients in Québec. The diffusive CH₄ flux was highly variable (mean 11.6 ± 26.4 SD mg m^?2 d^?1), and it was positively correlated with temperature and lake nutrient status, and negatively correlated with lake area and colored dissolved organic matter (CDOM). The relationship between CH₄ and CO₂ concentrations fluxes was weak, suggesting major differences in their respective sources and/or regulation. For example, increasing water temperature leads to higher CH₄ flux but does not significantly affect CO₂ flux, whereas increasing CDOM concentration leads to higher CO₂ flux but lower CH₄ flux. CH₄ contributed to 8 ± 23% to the total lake C emissions (CH₄ + CO₂), but 18 ± 25% to the total flux in terms of atmospheric warming potential, expressed as CO₂‐equivalents. The incorporation of ebullition and plant‐mediated CH₄ fluxes would further increase the importance of lake CH₄. The average Q₁₀ of CH₄ flux was 3.7, once other covarying factors were accounted for, but this apparent Q₁₀ varied with lake morphometry and was higher for shallow lakes. We conclude that global climate change and the resulting shifts in temperature will strongly influence lake CH₄ fluxes across the boreal biome, but these climate effects may be altered by regional patterns in lake morphometry, nutrient status, and browning.     

温带针阔混交林土壤碳氮气体通量的主控因子与耦合关系

中高纬度森林地区由于气候条件变化剧烈,土壤温室气体排放量的估算存在很大的不确定性,并且不同碳氮气体通量的主控因子与耦合关系尚不明确。以长白山温带针阔混交林为研究对象,采用静态箱-气相色谱法连续4a(2005—2009年)测定土壤二氧化碳(CO2)、甲烷(CH4)和氧化亚氮(N2O)净交换通量以及温度、水分等相关环境因子。研究结果表明:温带针阔混交林土壤整体上表现为CO2和N2O的排放源和CH4的吸收汇。土壤CH4、CO2和N2O通量的年均值分别为-1.3 kg CH4hm-2a-1、15102.2 kg CO2hm-2a-1和6.13 kg N2O hm-2a-1。土壤CO2通量呈现明显的季节性规律,主要受土壤温度的影响,水分次之;土壤CH4通量的季节变化不明显,与土壤水分显著正相关;土壤N2O通量季节变化与土壤CO2通量相似,与土壤水分、温度显著正相关。土壤CO2通量和CH4通量不存在任何类型的耦合关系,与N2O通量也不存在耦合关系;土壤CH4和N2O通量之间表现为消长型耦合关系。这项研究显示温带针阔混交林土壤碳氮气体通量主要受环境因子驱动,不同气体通量产生与消耗之间存在复杂的耦合关系,下一步研究需要深入探讨环境变化对其耦合关系的影响以及内在的生物驱动机制。     

Ultra‐High Surface Area Activated Porous Asphalt for CO2 Capture through Competitive Adsorption at High Pressures

This study reports an improved method for activating asphalt to produce ultra‐high surface area porous carbons. Pretreatment of asphalt (untreated Gilsonite, uGil ) at 400 °C for 3 h removes the more volatile organic compounds to form pretreated asphalt ( uGil‐P ) material with a larger fraction of higher molecular weight π‐conjugated asphaltenes. Subsequent activation of uGil‐P at 900 °C gives an ultra‐high surface area (4200 m² g^?1) porous carbon material ( uGil‐900 ) with a mixed micro and mesoporous structure. uGil‐900 shows enhanced room temperature CO₂ uptake capacity at 54 bar of 154 wt% (35 mmol g^?1). The CH₄ uptake capacity is 37.5 wt% (24 mmol g^?1) at 300 bar. These are relevant pressures in natural gas production. The room temperature working CO₂ uptake capacity for uGil‐900 is 19.1 mmol g^?1 (84 wt%) at 20 bar and 32.6 mmol g^?1 (143 wt%) at 50 bar. In order to further assess the reliability of uGil‐900 for CO₂ capture at elevated pressures, the authors study competitive sorption of CO₂ and CH₄ on uGil‐900 at pressures from 1 to 20 bar at 25 °C. CO₂/CH₄ displacement constants are measured at 2 to 40 bar, and found to increase significantly with pressure and surface area.