(600b) Evaluation of Tetraamine Functionalized Metal-Organic Framework (MOF) for Temperature Swing Adsorption (TSA)-Based CO2 Capture

Recently E.J. Kim, et al.[1] described a new class of tetraamine-based metal-organic framework that shows a characteristic type 6 CO2 isotherm. The isotherm has two inflection points giving it a characteristic double-S shape. This material has been described to be an ideal candidate for temperature swing adsorption (TSA) process. In this study we evaluate the potential of this material using detailed process modeling and optimization for a wide range of CO2 compositions.

The experimental CO₂ isotherm data obtained from Kim et.al. were fit to an empirical form that provides an explicit relationship between the fluid phase pressure and the equilibrium loading as a function of temperature. As a first step a series of breakthrough simulations are considered to elucidate the propagation of heat and mass transfer fronts that are strikingly different compared to classical type-1 systems. These were also validated based on the breakthrough experiments provided in the original paper. Based on the understanding of these breakthrough simulations, a four-step TSA cycle consisting was designed. A series of parametric studies allowed us to identify the key operating parameters. Detailed process optimization was performed to identify the Pareto curves of purity and recovery for a wide range of CO2 feed compositions. This was followed by optimization studies to minimize energy consumption and maximize productivity. The results show that the deployment of such materials in practical systems rely not just on identification of the correct operating condition but also on effective heat management [2-4]. A detailed discussion of the case studies and results of the optimization will be discussed at the meeting.

Keywords: double S shaped isotherm, MOF, carbon capture, temperature swing adsorption, steam purge

References:

1. Kim, E.J., Siegelman, R.L., Jiang, H.Z., Forse, A.C., Lee, J.H., Martell, J.D., Milner, P.J., Falkowski, J.M., Neaton, J.B., Reimer, J.A. and Weston, S.C., 2020. Cooperative carbon capture and steam regeneration with tetraamine-appended metal–organic frameworks. Science, 369(6502), pp.392-396.
2. Hefti, M., Joss, L., Bjelobrk, Z. and Mazzotti, M., 2016. On the potential of phase-change adsorbents for CO2 capture by temperature swing adsorption. Faraday discussions, 192, pp.153-179.
3. Pai, K.N., Baboolal, J.D., Sharp, D.A. and Rajendran, A., 2019. Evaluation of diamine-appended metal-organic frameworks for post-combustion CO2 capture by vacuum swing adsorption. Separation and Purification Technology, 211, pp.540-550.
4. Hughes, R., Kotamreddy, G., Ostace, A., Bhattacharyya, D., Siegelman, R.L., Parker, S.T., Didas, S.A., Long, J.R., Omell, B. and Matuszewski, M., 2021. Isotherm, Kinetic, Process Modeling, and Techno-Economic Analysis of a Diamine-Appended Metal–Organic Framework for CO2 Capture Using Fixed Bed Contactors. Energy & Fuels.