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Hybrid porous solids, with their tunable structures, their multifunctional properties and their numerous applications, are currently topical, particularly in the domain of adsorption and storage of greenhouse gases. Most of the data reported so far concern the performances of these solids in this domain, particularly in terms of adsorbed amounts of gas but do not explain at the atomic level why and how adsorption and storage occur. From a combination of structural, spectroscopic, thermodynamic experiments and of molecular simulations, this tutorial review proposes answers to these open questions with a special emphasis on CO2 and CH4storage by some rigid and flexible hybrid porous materials. [ABSTRACT FROM AUTHOR]

• Study of hybrid CO 2 capture system combining VPSA and CPU technologies. • Optimization of integrated capture CO 2 process and purification unit. • High CO 2 recovery (90–99 %) and high CO 2 purity (>99.99 %) • Complete analyses considering recovery, energy consumption, and capture cost. • Impact of the electricity source on the total CO 2 recovery. The imperative challenge posed by climate change requires urgent actions to counteract the harmful effects of greenhouse gas emissions, particularly CO 2 , which contributes to approximately 80 % of emissions responsible for global warming. A hybrid system combining Vacuum Pressure Swing Adsorption (VPSA) unit with a Cryogenic Carbon Purification Unit (CPU) is evaluated to enhance recovery and purity of CO 2 captured from flue gas containing CO 2 concentration ranging from 5 % to 20 %. VPSA preconcentrates the CO 2 and CPU completes the separation and purifies the CO 2. The study uses surrogate models for multi-objective optimization, considering energy consumption, cost, and CO 2 recovery, providing a time-efficient approach for investigating computationally demanding processes. Results from the study indicate that the hybrid system achieves over 90 % recovery for flue gas concentration range considered, while ensuring the production of high-purity CO 2 (>99.99 %) suitable for transportation. A trade-off analysis reveals the balance between recovery, electricity consumption, and economic viability. A sensitivity analysis identifies parameters influencing recovery and energy consumption, providing guidance for future optimization efforts. The techno-economic analysis highlights the impact of electricity prices and carbon taxes on total costs, identifying an optimum towards higher recovery values under rising carbon taxes. Furthermore, the research underscores concentration-dependent economic feasibility, emphasizing the attractiveness of concentrations above 10 % compared with other technologies, which require higher concentrations. For an electricity price of 75 €.MWh−1, the total cost of the CO 2 capture hydride system considering CO 2 emissions with carbon tax of 100 €.t CO2 −1 for concentrations ranging from 10 % to 20 % is from 123 to 80 €.t CO2 −1, respectively. The analysis of the electricity source shows the importance of a low-carbon emission energy mix for optimal carbon emission reduction. [ABSTRACT FROM AUTHOR]