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Carbon dioxide fixation in prokaryotes enables the assimilation of inorganic carbon into organic molecules, supporting biosynthetic pathways, sustaining ecosystems, and contributing to the global carbon cycle. It also has industrial applications in carbon capture and bioproduct synthesis. Autotrophic organisms rely on this process to utilize CO₂ as a carbon source in diverse environments.The Calvin CycleThe Calvin cycle is the most widespread carbon fixation mechanism, primarily used by...
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Unveiling the Direct Air Capture and Transformation to Formate Under Mild Conditions.

Julián E Sánchez-Velandia1,2, Vitoria Gonçalves Pina2,3, Mónica Oliva3

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This study optimizes hydroxide-based systems for direct air capture and conversion (DACC) of CO2 to formate. Researchers enhanced CO2 capture efficiency using specific cations and solvents, achieving high formate yields under mild conditions.

Keywords:
CO2 conversionIonic liquiddirect air capturehomogenous catalysis

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Area of Science:

  • Chemical Engineering
  • Materials Science
  • Catalysis

Background:

  • Direct air capture and conversion (DACC) technologies face challenges in efficiency and scalability.
  • Previous hydroxide-based systems showed promise for CO2 capture but required optimization regarding solvent and cation effects.

Purpose of the Study:

  • To develop and optimize hydroxide-based absorbents for efficient CO2 capture and subsequent hydrogenation to formate.
  • To investigate the impact of various organic cations and solvents on CO2 capture efficiency.
  • To optimize the catalytic hydrogenation of captured CO2 to formate.

Main Methods:

  • Systematic experimental and theoretical investigation of organic cations (tetrabutyl ammonium, phosphonium) and solvents (DMSO, H2O, MeOH).
  • Molecular dynamics simulations to understand solvent effects on solvation and aggregation.
  • Optimization of hydrogenation using Ru-based catalysts (Ru3(CO)12) and DFT calculations.

Main Results:

  • Achieved CO2 capture efficiency up to 1.0 mol CO2 per mol of tetrabutylammonium (TBA+) in DMSO/water mixtures.
  • Demonstrated that water addition enhances the CO2 sorption process.
  • Obtained >99% formate yield using Ru3(CO)12 under a mild 5 bar H2 pressure, a record low for DACC.

Conclusions:

  • Solvent composition critically influences CO2 capture performance in hydroxide-based systems.
  • Efficient CO2-to-formate conversion is achievable under mild conditions with optimized Ru-based catalysts.
  • The findings advance DACC technologies by lowering H2 pressure requirements and improving conversion rates.