Dataset Information

Integration of thermochemical water splitting with CO₂ direct air capture.

ABSTRACT: Renewable production of fuels and chemicals from direct air capture (DAC) of CO₂ is a highly desired goal. Here, we report the integration of the DAC of CO₂ with the thermochemical splitting of water to produce CO₂, H₂, O₂, and electricity. The produced CO₂ and H₂ can be converted to value-added chemicals via existing technologies. The integrated process uses thermal solar energy as the only energy input and has the potential to provide the dual benefits of combating anthropogenic climate change while creating renewable chemicals. A sodium-manganese-carbonate (Mn-Na-CO₂) thermochemical water-splitting cycle that simultaneously drives renewable H₂ production and DAC of CO₂ is demonstrated. An integrated reactor is designed and fabricated to conduct all steps of the thermochemical water-splitting cycle that produces close to stoichiometric amounts (∼90%) of H₂ and O₂ (illustrated with 6 consecutive cycles). The ability of the cycle to capture 75% of the ∼400 ppm CO₂ from air is demonstrated also. A technoeconomic analysis of the integrated process for the renewable production of H₂, O₂, and electricity, as well as DAC of CO₂ shows that the proposed scheme of solar-driven H₂ production from thermochemical water splitting coupled with CO₂ DAC may be economically viable under certain circumstances.

SUBMITTER: Brady C

PROVIDER: S-EPMC6911180 | biostudies-literature | 2019 Dec

REPOSITORIES: biostudies-literature

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Integration of thermochemical water splitting with CO2 direct air capture.

Brady Casper C Davis Mark E ME Xu Bingjun B

Proceedings of the National Academy of Sciences of the United States of America 20191121 50

Renewable production of fuels and chemicals from direct air capture (DAC) of CO2 is a highly desired goal. Here, we report the integration of the DAC of CO2 with the thermochemical splitting of water to produce CO2, H2, O2, and electricity. The produced CO2 and H2 can be converted to value-added chemicals via existing technologies. The integrated process uses thermal solar energy as the only energy input and has the pot ...[more]

PMID: 31754029

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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:Zeolites, silica-supported amines, and metal-organic frameworks (MOFs) have been demonstrated as promising adsorbents for direct air CO2 capture (DAC), but the shaping and structuring of these materials into sorbent modules for practical processes have been inadequately investigated compared to the extensive research on powder materials. Furthermore, there have been relatively few studies reporting the DAC performance of sorbent contactors under cold, subambient conditions (temperatures below 20 °C). In this work, we demonstrate the successful fabrication of adsorbent monoliths composed of cellulose acetate (CA) and adsorbent particles such as zeolite 13X and MOF MIL-101(Cr) by a 3D printing technique: solution-based additive manufacturing (SBAM). These monoliths feature interpenetrated macroporous polymeric frameworks in which microcrystals of zeolite 13X or MIL-101(Cr) are evenly distributed, highlighting the versatility of SBAM in fabricating monoliths containing sorbents with different particle sizes and density. Branched poly(ethylenimine) (PEI) is successfully loaded into the CA/MIL-101(Cr) monoliths to impart CO2 uptakes of 1.05 mmol gmonolith-1 at -20 °C and 400 ppm of CO2. Kinetic analysis shows that the CO2 sorption kinetics of PEI-loaded MIL-101(Cr) sorbents are not compromised in the monoliths compared to the powder sorbents. Importantly, these monoliths exhibit promising working capacities (0.95 mmol gmonolith-1) over 14 temperature swing cycles with a moderate regeneration temperature of 60 °C. Dynamic breakthrough experiments at 25 °C under dry conditions reveal a CO2 uptake capacity of 0.60 mmol gmonolith-1, which further increases to 1.05 and 1.43 mmol gmonolith-1 at -20 °C under dry and humid (70% relative humidity) conditions, respectively. Our work showcases the successful implementation of SBAM in making DAC sorbent monoliths with notable CO2 capture performance over a wide range of sorption temperatures, suggesting that SBAM can enable the preparation of efficient sorbent contactors in various form factors for other important chemical separations.

Project description:Addressing climate change constitutes one of the major scientific challenges of this century, and it is widely acknowledged that anthropogenic CO2 emissions largely contribute to this issue. To achieve the "net-zero" target and keep the rise in global average temperature below 1.5 °C, negative emission technologies must be developed and deployed at a large scale. This study investigates the feasibility of using membranes as direct air capture (DAC) technology to extract CO2 from atmospheric air to produce low-purity CO2. In this work, a two-stage hollow fiber membrane module process is designed and modeled using the AVEVA Process Simulation platform to produce a low-purity (≈5%) CO2 permeate stream. Such low-purity CO2 streams could have several possible applications such as algae growth, catalytic oxidation, and enhanced oil recovery. An operability analysis is performed by mapping a feasible range of input parameters, which include membrane surface area and membrane performance metrics, to an output set, which consists of CO2 purity, recovery, and net energy consumption. The base case for this simulation study is generated considering a facilitated transport membrane with high CO2/N2 separation performance (CO2 permeance = 2100 GPU and CO2/N2 selectivity = 1100), when tested under DAC conditions. With a constant membrane area, both membranes' intrinsic performances are found to have a considerable impact on the purity, recovery, and energy consumption. The area of the first module plays a dominant role in determining the recovery, purity, and energy demands, and in fact, increasing the area of the second membrane has a negative impact on the overall energy consumption, without improving the overall purities. The CO2 capture capacity of DAC units is important for implementation and scale-up. In this context, the performed analysis showed that the m-DAC process could be appropriate as a small-capacity system (0.1-1 Mt/year of air), with reasonable recoveries and overall purity. Finally, a preliminary CO2 emissions analysis is carried out for the membrane-based DAC process, which leads to the conclusion that the overall energy grid must be powered by renewable sources for the technology to qualify within the negative emissions category.

Dataset Information

Integration of thermochemical water splitting with CO₂ direct air capture.

Publications

Integration of thermochemical water splitting with CO<sub>2</sub> direct air capture.

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