ABSTRACT
Carbon Capture Utilization and Storage technologies are essential mitigation options to reach net-zero CO2 emissions. However, this challenge requires the development of sustainable and economic separation technologies. This work presents a novel CO2 capture technology strategy based on non-dispersive CO2 absorption and membrane vacuum regeneration (MVR) technology, and employs two imidazolium ionic liquids (ILs), [emim][Ac] and [emim][MS], with different behavior to absorb CO2. Continuous absorption-desorption experiments were carried out using polypropylene hollow fiber membrane contactors. The results show the highest desorption behavior in the case of [emim][Ac], with a MVR performance efficiency of 92% at 313 K and vacuum pressure of 0.04 bar. On the other hand, the IL [emim][MS] reached an efficiency of 83% under the same conditions. The MVR technology could increase the overall CO2 capture performance by up to 61% for [emim][Ac] and 21% for [emim][MS], which represents an increase of 26% and 9%, respectively. Moreover, adding 30%vol. demonstrates that the process was only favorable by using the physical IL. The results presented here indicate the interest in membrane vacuum regeneration technology based on chemical ILs, but further techno-economic evaluation is needed to ensure the competitiveness of this novel CO2 desorption approach for large-scale application.
ABSTRACT
In this work, the membrane vacuum regeneration (MVR) process was considered as a promising technology for solvent regeneration in post-combustion CO2 capture and utilization (CCU) since high purity CO2 is needed for a technical valorization approach. First, a desorption test by MVR using polypropylene hollow fiber membrane contactor (PP-HFMC) was carried out in order to evaluate the behavior of physical and physico-chemical absorbents in terms of CO2 solubility and regeneration efficiency. The ionic liquid 1-ethyl-3-methylimidazolium acetate, [emim][Ac], was presented as a suitable alternative to conventional amine-based absorbents. Then, a rigorous two-dimensional mathematical model of the MVR process in a HFMC was developed based on a pseudo-steady-state to understand the influence of the solvent regeneration process in the absorption-desorption process. CO2 absorption-desorption experiments in PP-HFMC at different operating conditions for desorption, varying vacuum pressure and temperature, were used for model validation. Results showed that MVR efficiency increased from 3% at room temperature and 500 mbar to 95% at 310K and 40 mbar vacuum. Moreover, model deviation studies were carried out using sensitivity analysis of Henry's constant and pre-exponential factor of chemical interaction, thus as to contribute to the knowledge in further works.
ABSTRACT
Polymeric carbon nitride materials have been used in numerous light-to-energy conversion applications ranging from photocatalysis to optoelectronics. For a new application and modelling, we first refined the crystal structure of potassium poly(heptazine imide) (K-PHI)-a benchmark carbon nitride material in photocatalysis-by means of X-ray powder diffraction and transmission electron microscopy. Using the crystal structure of K-PHI, periodic DFT calculations were performed to calculate the density-of-states (DOS) and localize intra band states (IBS). IBS were found to be responsible for the enhanced K-PHI absorption in the near IR region, to serve as electron traps, and to be useful in energy transfer reactions. Once excited with visible light, carbon nitrides, in addition to the direct recombination, can also undergo singlet-triplet intersystem crossing. We utilized the K-PHI centered triplet excited states to trigger a cascade of energy transfer reactions and, in turn, to sensitize, for example, singlet oxygen (1 O2 ) as a starting point to synthesis up to 25â different N-rich heterocycles.
