Dataset Information

Enhancement of CO2 Adsorption/Desorption Properties of Solid Sorbents Using Tetraethylenepentamine/Diethanolamine Blends.

ABSTRACT: Mesocellular silica foam was impregnated with tetraethylenepentamine (TEPA), diethanolamine (DEA), and their mixtures and examined as sorbents for CO2 capture. The sorbents were characterized by N2 physisorption, elemental analysis, and Fourier transform infrared spectroscopy. The effects of amine blending on the CO2 uptake, working capacity, and heat of adsorption were investigated and discussed. The experimental results showed that the heat of adsorption decreased with increasing DEA-to-TEPA ratios, but the CO2 uptake improved by the blending of TEPA and DEA. Furthermore, the DEA/TEPA blend considerably improved the regeneration properties of the sorbents. Mesocellular silica foam loaded with a mixture of 40 wt % TEPA and 30 wt % DEA exhibited a CO2 adsorption uptake of 5.91 mmol/g at 50 °C and 100 kPa with a heat of adsorption of 80 kJ/mol. Additionally, these sorbents demonstrated high cyclic stability and high selectivity toward CO2/N2 separation. In situ infrared spectroscopy investigations revealed that CO2 adsorption occurred predominantly through the formation of carbamate species for both TEPA and DEA.

SUBMITTER: Dao DS

PROVIDER: S-EPMC7512444 | biostudies-literature | 2020 Sep

REPOSITORIES: biostudies-literature

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Enhancement of CO2 Adsorption/Desorption Properties of Solid Sorbents Using Tetraethylenepentamine/Diethanolamine Blends.

Dao Duc Sy DS Yamada Hidetaka H Yogo Katsunori K

ACS omega 20200904 37

Mesocellular silica foam was impregnated with tetraethylenepentamine (TEPA), diethanolamine (DEA), and their mixtures and examined as sorbents for CO2 capture. The sorbents were characterized by N2 physisorption, elemental analysis, and Fourier transform infrared spectroscopy. The effects of amine blending on the CO2 uptake, working capacity, and heat of adsorption were investigated and discussed. The experimental results showed that the heat of adsorption decrea ...[more]

PMID: 32984672

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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

Enhancement of CO2 Adsorption/Desorption Properties of Solid Sorbents Using Tetraethylenepentamine/Diethanolamine Blends.

Publications

Enhancement of CO<sub>2</sub> Adsorption/Desorption Properties of Solid Sorbents Using Tetraethylenepentamine/Diethanolamine Blends.

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