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Adsorption equilibria of CO 2 , CH 4 , and their mixtures were measured on binderless pellets of NIST reference zeolite NaY (RM 8850) using a static gravimetric setup. The unary adsorption isotherms are reported at temperatures from 298 to 393 K up to a pressure of 3 MPa and compare favorably with independent results on RM 8850 powder. The competitive adsorption measurements were performed at temperatures from 298 to 353 K and up to 3 MPa for three premixed gas mixtures with CO 2 molar feed compositions of 0.25, 0.50, and 0.75. The results constitute the first competitive adsorption dataset reported for any of the NIST reference materials. RM 8850 shows a strong selectivity for CO 2 adsorption toward CH 4 . The experimental unary and binary adsorption isotherms are accurately modeled using the simplified statistical isotherm model (SSI). Notably, the agreement with the model improves only slightly (and within experimental uncertainties) when the whole dataset is used for parameter fitting as opposed to only using the unary data., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

The use of adsorbents for direct air capture (DAC) of CO 2 is regarded as a promising and essential carbon dioxide removal technology to help meet the goals outlined by the 2015 Paris Agreement. A class of adsorbents that has gained significant attention for this application is ultramicroporous metal organic frameworks (MOFs). However, the necessary data needed to facilitate process scale evaluation of these materials is not currently available. Here, we investigate TIFSIX-3-Ni, a previously reported ultramicroporous MOF for DAC, and measure several physicochemical and equilibrium adsorption properties. We report its crystal structure, textural properties, thermal stability, specific heat capacity, CO 2 , N 2 , and H 2 O equilibrium adsorption isotherms at multiple temperatures, and Ar and O 2 isotherms at a single temperature. For CO 2 , N 2 , and H 2 O, we also report isotherm model fitting parameters and calculate heats of adsorption. We assess the manufacturability and process stability of TIFSIX-3-Ni by investigating the impact of batch reproducibility, binderless pelletization, humidity, and adsorption-desorption cycling (50 cycles) on its crystal structure, textural properties, and CO 2 adsorption. For pelletized TIFSIX-3-Ni, we also report its skeletal, pellet, and bed density, total pore volume, and pellet porosity. Overall, our data enable initial process modeling and optimization studies to evaluate TIFSIX-3-Ni for DAC at the process scale. They also highlight the possibility to pelletize TIFSIX-3-Ni and the limited stability of the MOF under humid and oxidative conditions as well as upon multiple adsorption-desorption cycles., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

The equilibrium adsorption of CO 2 , N 2 , and H 2 on commercially available Zeolite H-Y, Na-Y, and cation-exchanged NaTMA-Y was measured up to 3 MPa at 298.15, 313.15, 333.15, 353.15, and 393.15 K gravimetrically using a magnetic suspension balance. The chemical and textural characterization of the materials was carried out by thermogravimetric analysis, helium gravimetry, and N 2 (77 K) physisorption. We report the excess and net isotherms as measured and estimates of the absolute adsorption isotherms. The latter are modeled using the simplified statistical isotherm (SSI) model to evaluate adsorbate-adsorbent interactions and parametrize the data for process modeling. When reported per unit volume of zeolite supercage, the SSI model indicates that the saturation capacity for a given gas takes the same value for the three adsorbents. The Henry's constants predicted by the model show a strong effect of the cation on the affinity of each adsorbate., Competing Interests: The authors declare no competing financial interest., (© 2023 The Authors. Published by American Chemical Society.)

Direct air capture (DAC) using solid adsorbents has gained significant attention as a carbon dioxide removal (CDR) technology to help limit global temperature rise to below 2 °C. One large area of focus is the development of new adsorbent materials for DAC. However, the necessary data needed to employ these materials in process models for adsorbent screening are rarely available. Here, we showcase Purolite A110, a commercially available amine-functionalized polymeric resin, as a new candidate adsorbent for DAC and compare its properties to a current benchmark, Lewatit VP OC 1065. For both materials, we report their chemical features and composition, skeletal, particle, and bed density, total pore volume, particle porosity, BET area, thermal stability, and specific heat capacity. We determine their equilibrium sorption properties by measuring the volumetric CO 2 isotherms at 288, 298, 308, 333, 343, 353, and 393 K, N 2 and H 2 O isotherms at 288, 298, and 308 K, and Ar and O 2 isotherms at 298 K. For CO 2 , N 2 , and H 2 O, we also present the corresponding isotherm model fitting parameters and heats of adsorption. These data can help facilitate process modeling and optimization studies to properly assess these adsorbents at scale., Competing Interests: The authors declare no competing financial interest., (© 2023 The Authors. Published by American Chemical Society.)

Porosity and surface area analysis play a prominent role in modern materials science. At the heart of this sits the Brunauer-Emmett-Teller (BET) theory, which has been a remarkably successful contribution to the field of materials science. The BET method was developed in the 1930s for open surfaces but is now the most widely used metric for the estimation of surface areas of micro- and mesoporous materials. Despite its widespread use, the calculation of BET surface areas causes a spread in reported areas, resulting in reproducibility problems in both academia and industry. To prove this, for this analysis, 18 already-measured raw adsorption isotherms were provided to sixty-one labs, who were asked to calculate the corresponding BET areas. This round-robin exercise resulted in a wide range of values. Here, the reproducibility of BET area determination from identical isotherms is demonstrated to be a largely ignored issue, raising critical concerns over the reliability of reported BET areas. To solve this major issue, a new computational approach to accurately and systematically determine the BET area of nanoporous materials is developed. The software, called "BET surface identification" (BETSI), expands on the well-known Rouquerol criteria and makes an unambiguous BET area assignment possible., (© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

As more countries commit to a net-zero GHG emission target, we need a whole energy and industrial system approach to decarbonization rather than focus on individual emitters. This paper presents a techno-economic analysis of monoethanolamine-based post-combustion capture to explore opportunities over a diverse range of power and industrial applications. The following ranges were investigated: feed gas flow rate between 1-1000 kg ·s -1 , gas CO 2 concentrations of 2-42% mol , capture rates of 70-99%, and interest rates of 2-20%. The economies of scale are evident when the flue gas flow rate is <20 kg ·s -1 and gas concentration is below 20% mol CO 2 . In most cases, increasing the capture rate from 90 to 95% has a negligible impact on capture cost, thereby reducing CO 2 emissions at virtually no additional cost. The majority of the investigated space has an operating cost fraction above 50%. In these instances, reducing the cost of capital ( i.e. , interest rate) has a minor impact on the capture cost. Instead, it would be more beneficial to reduce steam requirements. We also provide a surrogate model which can evaluate capture cost from inputs of the gas flow rate, CO 2 composition, capture rate, interest rate, steam cost, and electricity cost.

The crucial role of dispersion force in correctly describing the adsorption of some typical small-size gas molecules (e.g., CO2, N2, and CH4) in ion-exchanged chabazites has been investigated at different levels of theory, including the standard density functional theory calculation using the Perdew, Burke, and Ernzerhof (PBE) exchange-correlation functional and van der Waals density functional theory (vdWDFT) calculations using different exchange-correlation models - vdW&#95;DF2, optB86b, optB88, and optPBE. Our results show that the usage of different vdWDFT functionals does not significantly change the adsorption configuration or the profile of static charge rearrangement of the gas-chabazite complexes, in comparison with the results obtained using the PBE. The calculated values of adsorption enthalpy using different functionals are compared with our experimental results. We conclude that the incorporation of dispersion interaction is imperative to correctly predict the trend of adsorption enthalpy values, in terms of different gas molecules and Cs(+) cation densities in the adsorbents, even though the absolute values of adsorption enthalpy are overestimated by approximate 10 kJ/mol compared with experiments.