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Technoeconomic Investigation of Amine-Grafted Zeolites and Their Kinetics for CO₂ Capture.

ABSTRACT: Solid adsorbents with precise surface structural chemistry and porosity are of immense interest to decode the structure-property relationships and maintain an energy-intensive path while achieving high activity and durability. In this work, we reported a series of amine-modified zeolites and their CO₂ capture efficiencies. The amine impregnated molecular zeolite compounds were characterized and systematically investigated for CO₂ adsorption capacity through thermogravimetric analysis for the occurrence of atmospheric pure CO₂ gas at 75 °C with diethylenetriamine (DETA), ethylenediamine (EDA), monoethanolamine (MEA), and triethanolamine (TEA)-loaded zeolite 13X, 4A, and 5A adsorbents. The kinetics of the adsorption study indicated that the adsorption capacity for CO₂ adsorption was improved with amine loading up to a certain concentration over 13X-DETA-40, showing an adsorption capacity of 1.054 mmol of CO₂ per gram of zeolite in a very short amount of time. The result was especially promising in terms of the initial adsorption capacity of zeolite, which adsorbed approximately 0.8 mmol/g zeolite within the first two minutes of experimentation. A detailed flow chart that includes a brief look into the process adopted for adsorption was included. Lagergren pseudo-first- and pseudo-second-order models of 40 wt % DETA zeolite 13X gave CO₂ adsorption capacities of 1.055 and 1.058 mmol/g and also activation energies of 86 and 76 kJ/mol, respectively. The CO₂ adsorption capacity of 13X-DETA-40 in a lab-scale reactor was found to be 1.69 mmol/g. A technoeconomic study was conducted for the solid amine zeolites to understand the investment per ton of CO₂ adsorbed. This study was used as a basis to improve cost estimates from a microscale to a lab-scale reactor. The cost of investment for 13X-DETA-40 was reduced by 84% from $49,830/ton CO₂ adsorbed in a microscale reactor to $7,690/ton of CO₂ adsorbed in a lab-scale reactor.

SUBMITTER: Tejavath V

PROVIDER: S-EPMC7948227 | biostudies-literature | 2021 Mar

REPOSITORIES: biostudies-literature

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Technoeconomic Investigation of Amine-Grafted Zeolites and Their Kinetics for CO2 Capture.

Tejavath Vijaya V Kasarabada Viswateja V Gonuguntla Spandana S Perupoga Vijayanand V Nandury Satyanarayana V SV Bojja Sreedhar S Pal Ujjwal U

ACS omega 20210219 9

Solid adsorbents with precise surface structural chemistry and porosity are of immense interest to decode the structure-property relationships and maintain an energy-intensive path while achieving high activity and durability. In this work, we reported a series of amine-modified zeolites and their CO2 capture efficiencies. The amine impregnated molecular zeolite compounds were characterized and systematically investigated for CO2 adsorption capacity through thermogravimetri ...[more]

PMID: 33718706

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Project description:Rising CO2 emissions are responsible for increasing global temperatures causing climate change. Significant efforts are underway to develop amine-based sorbents to directly capture CO2 from air (called direct air capture (DAC)) to combat the effects of climate change. However, the sorbents' performances have usually been evaluated at ambient temperatures (25 °C) or higher, most often under dry conditions. A significant portion of the natural environment where DAC plants can be deployed experiences temperatures below 25 °C, and ambient air always contains some humidity. In this study, we assess the CO2 adsorption behavior of amine (poly(ethyleneimine) (PEI) and tetraethylenepentamine (TEPA)) impregnated into porous alumina at ambient (25 °C) and cold temperatures (-20 °C) under dry and humid conditions. CO2 adsorption capacities at 25 °C and 400 ppm CO2 are highest for 40 wt% TEPA-incorporated γ-Al2O3 samples (1.8 mmol CO2/g sorbent), while 40 wt % PEI-impregnated γ-Al2O3 samples exhibit moderate uptakes (0.9 mmol g-1). CO2 capacities for both PEI- and TEPA-incorporated γ-Al2O3 samples decrease with decreasing amine content and temperatures. The 40 and 20 wt % TEPA sorbents show the best performance at -20 °C under dry conditions (1.6 and 1.1 mmol g-1, respectively). Both the TEPA samples also exhibit stable and high working capacities (0.9 and 1.2 mmol g-1) across 10 cycles of adsorption-desorption (adsorption at -20 °C and desorption conducted at 60 °C). Introducing moisture (70% RH at -20 and 25 °C) improves the CO2 capacity of the amine-impregnated sorbents at both temperatures. The 40 wt% PEI, 40 wt % TEPA, and 20 wt% TEPA samples show good CO2 uptakes at both temperatures. The results presented here indicate that γ-Al2O3 impregnated with PEI and TEPA are potential materials for DAC at ambient and cold conditions, with further opportunities to optimize these materials for the scalable deployment of DAC plants at different environmental conditions.

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

Technoeconomic Investigation of Amine-Grafted Zeolites and Their Kinetics for CO₂ Capture.

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Technoeconomic Investigation of Amine-Grafted Zeolites and Their Kinetics for CO<sub>2</sub> Capture.

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