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Spraying Water Microdroplets Containing 1,2,3-Triazole Converts Carbon Dioxide into Formic Acid.

Xiaowei SongYifan MengRichard N Zare
Published in: Journal of the American Chemical Society (2022)
We report the use of 1,2,3-triazole (Tz)-containing water microdroplets for gas-phase carbon dioxide (CO 2 ) reduction at room temperature. Using a coaxial sonic spraying setup, the CO 2 can be efficiently captured by Tz and converted to formic acid (HCOOH; FA) at the gas-liquid interface (GLI). A mass spectrometer operated in negative ion mode monitors the capture of CO 2 to form the bicarbonate anion (HCO 3 - ) and conversion to form the formate anion (HCOO - ). Varied FA species were successfully identified by MS/MS experiments including the formate monomer ([FA - H] - , m / z 45), the dimer ([2FA - H] - , m / z 91; [2FA + Na - 2H] - , m / z 113), the trimer ([3FA - H] - , m / z 137), and some other adducts (such as [FA - H + H 2 CO 3 ] - , m / z 107; [2FA + Na - 2H + Tz] - , m / z 182). The reaction conditions were systematically optimized to make the maximum conversion yield reach over 80% with an FA concentration of approximately 71 ± 3.1 μM. The mechanism for the reaction is speculated to be that Tz donates the proton and the hydroxide (OH - ) at the GLI, resulting in a stepwise yield of electrons to reduce gas-phase CO 2 to FA.
Keyphrases
  • carbon dioxide
  • room temperature
  • ionic liquid
  • ms ms
  • mass spectrometry
  • liquid chromatography tandem mass spectrometry