4.7 Article

Carbon dioxide capture with aqueous amino acids: Mechanistic study of amino acid regeneration by guanidine crystallization and process intensification

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ELSEVIER
DOI: 10.1016/j.seppur.2021.118839

关键词

CO2 capture; Amino acids; Guanidine crystallization; Process intensification

资金

  1. Seed Money Fund of the Laboratory Directed Research and Development program of the Oak Ridge National Laboratory (ORNL)
  2. US Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division

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This paper investigates CO2 capture from powerplant-generated flue gas via a phase-changing process involving absorption with aqueous amino acids and bicarbonate crystallization with bis-iminoguanidines. The results show that the thermodynamic driving force for glycine regeneration mainly comes from the GBIGH(2)(2+) bicarbonate crystallization step, while the rate-limiting step is the protonation of GBIG. This research provides a fundamental basis for developing an effective carbon capture technology with phase-changing amino acid/guanidine absorbents.
CO2 capture from powerplant-generated flue gas via a phase-changing process involving absorption with aqueous amino acids (e.g., glycine or sarcosine) and bicarbonate crystallization with bis-iminoguanidines (e.g., glyoxal-bis-iminoguanidine or GBIG) is investigated in this paper. This process is of high interest due to its potential to decrease the energy penalty for CO2 capture by significantly reducing the solvent regeneration energy typically associated with aqueous amine solvents. A critical step in the proposed CO2 capture mechanism is the regeneration of the amino acid by removal of protons and bicarbonate ions from solution through crystallization of GBIGH(2)(2+) bicarbonate salt. Here, we investigated the thermodynamics and kinetics of glycine regeneration by crystallization of GBIGH(2)(2+)(HCCO3-) (H2O)(2). A theoretical model was developed and compared to experimental data to simulate and predict the glycine regeneration and determine its reaction mechanism. This combined experimental and theoretical study led to the conclusion that, while the GBIGH(2)(2+ )bicarbonate crystallization step provides most of the thermodynamic driving force for the glycine regeneration, the rate-limiting step is the pmtonation of GBIG prior to crystallization. The CO2 loading and amino acid regeneration steps were combined into a single, intensified process using a bubble column reactor. The CO2 loading capacity of GBIG was experimentally determined to be roughly 1.36 mol CO2 per mol GBIG. These results provide the fundamental basis for developing an effective carbon capture technology with phase-changing amino acid/guanidine absorbents.

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