4.7 Article

CO2 capture from ambient air via crystallization with tetraalkylammonium hydroxides

期刊

DALTON TRANSACTIONS
卷 51, 期 46, 页码 17724-17732

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d2dt02262a

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资金

  1. Royal Swedish Academy of Science
  2. Swedish Research Council (Vetenskapsradet, VR) [2020-05405]
  3. Tage Erlander Guest Professorship [2018-00233]
  4. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Heavy Elements program [DE-SC0019220]
  5. U.S. NSF MRI [1828078]
  6. Division Of Chemistry
  7. Direct For Mathematical & Physical Scien [1828078] Funding Source: National Science Foundation

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This study serendipitously found that aqueous solutions of short carbon chain tetra(n-alkyl)ammonium hydroxides can be potential candidates for direct air carbon capture when used as reagents. The presence of certain compounds can enhance the sorption efficiency of carbon dioxide.
Aqueous solutions of a series of short carbon chain tetra(n-alkyl)ammonium hydroxides, [N-nnnn][OH] with n = 2: n-ethyl, 3: n-propyl, 4: n-butyl, have been serendipitously found to be potential candidates for direct air carbon capture (DAC) when being used as reagents in more complicated reactions. Aqueous solutions of [N-3333][OH], [N-2222][OH], or [N-3333][OH] with UO2SO4.3H(2)O and 1,4-diamidoximylbenzene, and [N-4444][OH] with cytosine (HCyt) directly absorb CO2 from the atmosphere upon mild heating in the open atmosphere crystallizing in complexes reaching up to 2 : 1 CO2/[N-nnnn]OH ratio. [N-2222][HCO3].3H(2)O (1), [N-2222](2)[H(HCO3)(3)].5H(2)O (2), [N-3333][HCO3].0.5H(2)O (3), [N-3333][H(HCO3)(2)] (4), [N-3333](2)[(tpa)(H2CO3)(2)] (5; tpa = terephthalate), [N-4444][H(Cyt)(HCO3)].H2O (6) and [N-4444][H-2(Cyt)(2)(HCO3)].H2O (7) have been isolated in crystalline form and structurally characterized by single crystal X-ray diffraction. The compounds are characterized by complex polyanionic formations from bicarbonate dimers ([(HCO3)(2).(H2O)](2)(4-)) or chains ([H(HCO3)(2)](n)(n-) or [H-2(tpa)(HCO3)(2)](n)(2n-)) to water-bicarbonate associates ([(HCO3)(2).6H(2)O](2-) and [(H2CO3.(HCO3)(2))(2).6H(2)O.2H(2)O](2-)) and three-component anionic layers ([H(Cyt)(HCO3).H2O](n)(n-) and [H-2(Cyt)(2)(HCO3).H2O](n)(n-)) frequently showing proton sharing. While some hydroxides themselves can maintain a high CO2/[N-nnnn][OH] ratio, particularly 2 and 4, the presence of secondary hydrogen bond donors/acceptors may increase the sorption efficiency through decreased solubility and enhanced crystallization.

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