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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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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.

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Integration of thermochemical water splitting with CO₂ direct air capture.

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Dataset Information

Integration of thermochemical water splitting with CO2 direct air capture.

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OmicsDI is part of the ELIXIR infrastructure

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Integration of thermochemical water splitting with CO₂ direct air capture.