Coke oven gases processing by vacuum swing adsorption: Carbon capture and methane recovery

Coke oven gas (COG), a by-product gas from the steel industry with great potential for chemical utilization, contains multiple high-value gases including H₂, CO₂, and CH₄. Our previous work has successfully achieved hydrogen production from COG with a purity greater than 99.99 %. For further separation of COG-to-hydrogen tail gas, a two-phase vacuum swing adsorption (VSA) strategy for CO₂ capture and CH₄ upgrading was carried out in this study. The accuracy of the 4-bed 8-step and 4-bed 7-step cycles established in the in-house mathematical model was verified through a series of multi-component breakthrough and VSA experiments for the two-stage CO₂ capture and CH₄ upgrading processes employing zeolite NaY and activated carbon RB3, respectively. To achieve more excellent separation performance, several novel VSA cycles were designed and developed in terms of each stage, and the Pareto fronts of purity and recovery of CO₂ or CH₄ for each cycle were obtained through a multi-objective optimization framework. Based on this, the separation performance and energy consumption of the optimal cycle for each stage were parametrically analyzed under various feed gas concentrations, vacuum pressures, and feed velocities. Moreover, the CO₂ product with a purity of 95.58 % and a recovery of 90.11 % can be obtained ultimately by using a 4-bed 8-step cycle for the first stage and a 4-bed 7-step cycle for the second stage of the CO₂ capture process under 0.1 bar vacuum pressure. The CH₄ upgrading process using a 4-bed 7-step cycle at 0.1 bar vacuum pressure produced a product with 92.07 % purity and 98.81 % recovery. The specific energy consumption was 32.17 kJ/mol and 1.80 kJ/mol for CO₂ capture and CH₄ upgrading, respectively. Recovery of high-purity CO₂ and CH₄ at such medium vacuum pressure and low energy consumption through a two-phase VSA strategy from COG has great application potential.