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This work presents a comprehensive thermodynamic model for both pure component isotherms and mixed‐gas adsorption equilibria. A generalization of thermodynamic Langmuir isotherm, the proposed model assumes competitive adsorption of multiple adsorbates on adsorbent surface for mixed‐gas adsorption equilibria, and it applies an area‐based adsorption nonrandom two‐liquid activity coefficient model in the activity coefficient calculations for the adsorbate phase. The resulting generalized Langmuir isotherm properly captures both surface loading dependence and adsorbate phase composition dependence for mixed‐gas adsorption equilibria. The model is validated with accurate representations of gas adsorption equilibrium data for varieties of unary, binary, and ternary gas systems. The model results are further compared with those calculated from extended Langmuir isotherm and Ideal Adsorbed Solution Theory.

Ammonia (NH3) is conventionally produced using fossil natural gas (NG) for hydrogen production through steam reformation, and synthesis in Haber-Bosch (HB) process. Conventional ammonia global production contributes to more than...

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Developed for multilayer adsorption, the Brunauer-Emmett-Teller (BET) isotherm considers the adsorption of the first layer as an equilibrium chemical reaction between adsorbate molecules and adsorption sites and the adsorption of the second and subsequent layers as a condensation-evaporation process. Following the recent development of an activity-based formulation for the Langmuir isotherm for monolayer adsorption, we present an activity-based formulation for the BET isotherm in which species concentrations are replaced with species activities. Capturing the adsorbent surface heterogeneity for the adsorption of the first layer, the resulting thermodynamic BET isotherm is shown to accurately represent pure component adsorption isotherms over the relative pressure range of zero to unity or prior to the onset of capillary condensation. The thermodynamic BET isotherm should facilitate accurate estimation of monolayer adsorption capacity and the corresponding adsorbent surface area.

In 2019, U.S. petroleum refineries emitted 196 million metric tons (MT) of CO2, while the well-to-gate and the full life cycle CO2 emissions were significantly higher, reaching 419 and 2843 million MT of CO2, respectively. This analysis examines decarbonization opportunities for U.S. refineries and the cost to achieve both refinery-level and complete life-cycle CO2 emission reductions. We used 2019 life-cycle CO2 emissions from U.S. refineries as a baseline and identified three categories of decarbonization opportunity: (1) switching refinery energy inputs from fossil to renewable sources (e.g., switch hydrogen source); (2) carbon capture and storage of CO2 from various refining units; and (3) changing the feedstock from petroleum crude to biocrude using various blending levels. While all three options can reduce CO2 emissions from refineries, only the third can reduce emissions throughout the life cycle of refinery products, including the combustion of fuels (e.g., gasoline and diesel) during end use applications. A decarbonization approach that combines strategies 1, 2, and 3 can achieve negative life-cycle CO2 emissions, with an average CO2 avoidance cost of $113–$477/MT CO2, or $54–$227/bbl of processed crude; these costs are driven primarily by the high cost of biocrude feedstock.

The well-to-wheel analysis encompasses both the upstream activities of primary energy recovery and processing, and the downstream activities of packaging, delivering, and dispensing H2 into vehicles.