Unary Adsorption Equilibria of Hydrogen, Nitrogen, and Carbon Dioxide on Y-Type Zeolites at Temperatures from 298 to 393 K and at Pressures up to 3 MPa.

The equilibrium adsorption of CO2, N2, and H2 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 N2 (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.

Measurement of Physicochemical Properties and CO2, N2, Ar, O2, and H2O Unary Adsorption Isotherms of Purolite A110 and Lewatit VP OC 1065 for Application in Direct Air Capture.

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 CO2 isotherms at 288, 298, 308, 333, 343, 353, and 393 K, N2 and H2O isotherms at 288, 298, and 308 K, and Ar and O2 isotherms at 298 K. For CO2, N2, and H2O, 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.

En Route to Zero Emissions for Power and Industry with Amine-Based Post-combustion Capture.

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 CO2 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 CO2. In most cases, increasing the capture rate from 90 to 95% has a negligible impact on capture cost, thereby reducing CO2 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, CO2 composition, capture rate, interest rate, steam cost, and electricity cost.

Adsorption of CO2, N2, and CH4 in Cs-exchanged chabazite: a combination of van der Waals density functional theory calculations and experiment study.

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_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.

Physicochemical Properties, Equilibrium Adsorption Performance, Manufacturability, and Stability of TIFSIX-3-Ni for Direct Air Capture of CO2.

The use of adsorbents for direct air capture (DAC) of CO2 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, CO2, N2, and H2O equilibrium adsorption isotherms at multiple temperatures, and Ar and O2 isotherms at a single temperature. For CO2, N2, and H2O, 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 CO2 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.