Dataset Information

Direct CO2 Capture from Air via Crystallization with a Trichelating Iminoguanidine Ligand.

ABSTRACT: Effectively reducing the concentration of CO2 in ambient air is essential to mitigate global warming. Existing carbon capture and storage technology can only slow down the carbon emissions of large point sources but cannot treat the already accumulated CO2 in the environment. Herein, we demonstrated a simple direct CO2 capture method from air via reactive crystallization with a new trichelating iminoguanidine ligand (BTIG). It could strongly bind CO2 to form insoluble carbonate crystals that could be easily isolated. In the crystal, CO2 was transformed to CO3 2- and trapped in a dense hydrogen bonding network in terms of carbonate-water clusters. This capture process was reversible, and the BTIG ligand could be regenerated by heating the BTIG-CO2 crystal at a mild temperature, which was much lower than the decomposition temperature of CaCO3 (?900 °C). Thermodynamic and kinetics analyses indicate that the crystallization process was exothermic with an enthalpy of -292 kJ/mol, and the decomposition energy consumption was 169 kJ per mol CO2. In addition, BTIG could also be employed for CO2 capture from flue gas with a capacity of 1.46 mol/mol, which was superior to that of most of the reported sorbents.

SUBMITTER: Cai H

PROVIDER: S-EPMC7439369 | biostudies-literature | 2020 Aug

REPOSITORIES: biostudies-literature

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Direct CO2 Capture from Air via Crystallization with a Trichelating Iminoguanidine Ligand.

Cai He H Zhang Xingwang X Lei Lecheng L Xiao Chengliang C

ACS omega 20200806 32

Effectively reducing the concentration of CO2 in ambient air is essential to mitigate global warming. Existing carbon capture and storage technology can only slow down the carbon emissions of large point sources but cannot treat the already accumulated CO2 in the environment. Herein, we demonstrated a simple direct CO2 capture method from air via reactive crystallization with a new trichelating iminoguanidine ligand (BTIG). It could strongly bind CO2 t ...[more]

PMID: 32832796

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Project description:Aminopolymer-based sorbents are preferred materials for extraction of CO2 from ambient air [direct air capture (DAC) of CO2] owing to their high CO2 adsorption capacity and selectivity at ultra-dilute conditions. While those adsorptive properties are important, the stability of a sorbent is a key element in developing high-performing, cost-effective, and long-lasting sorbents that can be deployed at scale. Along with process upsets, environmental components such as CO2, O2, and H2O may contribute to long-term sorbent instability. As such, unraveling the complex effects of such atmospheric components on the sorbent lifetime as they appear in the environment is a critical step to understanding sorbent deactivation mechanisms and designing more effective sorbents and processes. Here, a poly(ethylenimine) (PEI)/Al2O3 sorbent is assessed over continuous and cyclic dry and humid conditions to determine the effect of the copresence of CO2 and O2 on stability at an intermediate temperature of 70 °C. Thermogravimetric and elemental analyses in combination with in situ horizontal attenuated total reflection infrared (HATR-IR) spectroscopy are performed to measure the extent of deactivation, elemental content, and molecular level changes in the sorbent due to deactivation. The thermal/thermogravimetric analysis results reveal that incorporating CO2 with O2 accelerates sorbent deactivation using these sorbents in dry and humid conditions compared to that using CO2-free air in similar conditions. The in situ HATR-IR spectroscopy results of PEI/Al2O3 sorbent deactivation under a CO2-air environment show the formation of primary amine species in higher quantity (compared to that in conditions without O2 or CO2), which arises due to the C-N bond cleavage at secondary amines due to oxidative degradation. We hypothesize that the formation of bound CO2 species such as carbamic acids catalyzes C-N cleavage reactions in the oxidative degradation pathway by shuttling protons, resulting in a low activation energy barrier for degradation, as probed by metadynamics simulations. In the cyclic experiment after 30 cycles, results show a gradual loss in stability (dry: 29%, humid: 52%) under CO2-containing air (0.04% CO2/21% O2 balance N2). However, the loss in capacity during cyclic studies is significantly less than that during continuous deactivation, as expected.

Dataset Information

Direct CO2 Capture from Air via Crystallization with a Trichelating Iminoguanidine Ligand.

Publications

Direct CO<sub>2</sub> Capture from Air via Crystallization with a Trichelating Iminoguanidine Ligand.

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