Journal Article PUBDB-2025-03831

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Synthesis and characterization of crystalline polymeric carbonic acid (H$_2$CO$_3$) with sp$^{3-}$hybridized carbon at elevated pressures

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2025
Macmillan Publishers Limited, part of Springer Nature [London]

Communications chemistry 8(1), 237 () [10.1038/s42004-025-01614-y]
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Abstract: The existence of polymeric carbonic acid (H$_2$CO$_3$) at elevated pressures has been predicted, but has not been investigated experimentally. Here, polymeric carbonic acid containing sp3-hybridized carbon was synthesized and characterized at ≈40 GPa. H$_2$CO$_3$ single crystals were obtained by laser-heating a H$_2$O + CO$_2$ mixture in a diamond anvil cell. The orthorhombic crystal structure (Cmc2$_1$ with Z = 4) was refined from synchrotron single crystal X-ray diffraction data and is in agreement with a structural model predicted earlier. The crystal structure of H$_2$CO$_3$-Cmc2$_1$ is characterized by $[CO_4]^{4-}$ building blocks which are connected via corner sharing, forming chains along the c-axis. The combination of single crystal X-ray data with experimental Raman spectroscopy and DFT-calculations confirms that the structural model of H$_2$CO$_3$-Cmc2$_1$ is appropriate. The synthesis condition of polymeric carbonic acid points towards its potential existence in ice giants including the ones present in our solar system.

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Note: We gratefully acknowledge funding from the DFG (WI1232, BA4020, and FOR2125/CarboPaT) and the DFG Emmy-Noether Program (projects BY101/2-1 and BY112/2-1).

Contributing Institute(s):
  1. FS DOOR-User (FS DOOR-User)
  2. Experimentebetreuung PETRA III (FS-PET-D)
Research Program(s):
  1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
  2. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
  3. DFG project G:(GEPRIS)264049573 - Carbonate und Schock-Kompression: Stabilität, Phasentransformation und chemische Reaktionen mit Silikaten (264049573) (264049573)
Experiment(s):
  1. PETRA Beamline P02.2 (PETRA III)

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 Record created 2025-08-28, last modified 2025-09-07


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