Dataset Information

Quaternary functionalized mesoporous adsorbents for ultra-high kinetics of CO₂ capture from air.

ABSTRACT: Obstacles to widespread deployments of direct air capture of CO₂ (DAC) lie in high material and energy costs. By grafting quaternary ammonium (QA) functional group to mesoporous polymers with high surface area, a unique DAC adsorbent with moisture swing adsorption (MSA) ability and ultra-high kinetics was developed in this work. Functionalization is designed for efficient delivery of QA group through mesopores to active substitution sites. This achieved ultra-high kinetics adsorbent with half time of 2.9 min under atmospheric environment, is the highest kinetics value reported among DAC adsorbents. A cyclic adsorption capacity of 0.26 mmol g^-1 is obtained during MSA process. Through adsorption thermodynamics, it is revealed that adsorbent with uniform cylindrical pore structure has higher functional group efficiency and CO₂ capacity. Pore structure can also tune the MSA ability of adsorbent through capillary condensation of water inside its mesopores. The successful functionalization of mesoporous polymers with superb CO₂ adsorption kinetics opens the door to facilitate DAC adsorbents for large-scale carbon capture deployments.

SUBMITTER: Wang T

PROVIDER: S-EPMC7722900 | biostudies-literature | 2020 Dec

REPOSITORIES: biostudies-literature

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Quaternary functionalized mesoporous adsorbents for ultra-high kinetics of CO<sub>2</sub> capture from air.

Wang Tao T Wang Xinru X Hou Chenglong C Liu Jun J

Scientific reports 20201208 1

Obstacles to widespread deployments of direct air capture of CO<sub>2</sub> (DAC) lie in high material and energy costs. By grafting quaternary ammonium (QA) functional group to mesoporous polymers with high surface area, a unique DAC adsorbent with moisture swing adsorption (MSA) ability and ultra-high kinetics was developed in this work. Functionalization is designed for efficient delivery of QA group through mesopores to active substitution sites. This achieved ultra-high kinetics adsorbent w ...[more]

PMID: 33293560

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Project description:An excessive amount of CO2 is the leading cause of climate change, and hence, its reduction in the Earth's atmosphere is critical to stop further degradation of the environment. Although a large body of work has been carried out for post-combustion low-temperature CO2 capture, there are very few high temperature pre-combustion CO2 capture processes. Lithium silicate (Li4SiO4), one of the best known high-temperature CO2 capture sorbents, has two main challenges, moderate capture kinetics and poor sorbent stability. In this work, we have designed and synthesized lithium silicate nanosheets (LSNs), which showed high CO2 capture capacity (35.3 wt% CO2 capture using 60% CO2 feed gas, close to the theoretical value) with ultra-fast kinetics and enhanced stability at 650 °C. Due to the nanosheet morphology of the LSNs, they provided a good external surface for CO2 adsorption at every Li-site, yielding excellent CO2 capture capacity. The nanosheet morphology of the LSNs allowed efficient CO2 diffusion to ensure reaction with the entire sheet as well as providing extremely fast CO2 capture kinetics (0.22 g g-1 min-1). Conventional lithium silicates are known to rapidly lose their capture capacity and kinetics within the first few cycles due to thick carbonate shell formation and also due to the sintering of sorbent particles; however, the LSNs were stable for at least 200 cycles without any loss in their capture capacity or kinetics. The LSNs neither formed a carbonate shell nor underwent sintering, allowing efficient adsorption-desorption cycling. We also proposed a new mechanism, a mixed-phase model, to explain the unique CO2 capture behavior of the LSNs, using detailed (i) kinetics experiments for both adsorption and desorption steps, (ii) in situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy measurements, (iii) depth-profiling X-ray photoelectron spectroscopy (XPS) of the sorbent after CO2 capture and (iv) theoretical investigation through systematic electronic structure calculations within the framework of density functional theory (DFT) formalism.

Dataset Information

Quaternary functionalized mesoporous adsorbents for ultra-high kinetics of CO2 capture from air.

Publications

Quaternary functionalized mesoporous adsorbents for ultra-high kinetics of CO<sub>2</sub> capture from air.

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Quaternary functionalized mesoporous adsorbents for ultra-high kinetics of CO₂ capture from air.