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<p>The existence of polymeric carbonic acid (H<sub>2</sub>CO<sub>3</sub>) at elevated pressures has been predicted, but has not been investigated experimentally. Here, polymeric carbonic acid containing <i>s</i><i>p</i><sup>3</sup>-hybridized carbon was synthesized and characterized at &#xa0;≈40 GPa. H<sub>2</sub>CO<sub>3</sub> single crystals were obtained by laser-heating a H<sub>2</sub>O + CO<sub>2</sub> mixture in a diamond anvil cell. The orthorhombic crystal structure (<i>C</i><i>m</i><i>c</i>2<sub>1</sub> with <i>Z</i>&#xa0;=&#xa0;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<sub>2</sub>CO<sub>3</sub>-<i>C</i><i>m</i><i>c</i>2<sub>1</sub> is characterized by <InlineEquation ID="IEq1"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="42004_2025_1614_Article_IEq1.gif" Format="GIF" Height="22" Rendition="HTML" Resolution="72" Type="Linedraw" Width="57" /> </InlineMediaObject> <EquationSource Format="TEX">\({[{{\rm{CO}}}_{4}]}^{4-}\)</EquationSource> <EquationSource Format="MATHML"><math> <msup> <mrow> <mrow> <mo>[</mo> <mrow> <msub> <mrow> <mi mathvariant="normal">CO</mi> </mrow> <mrow> <mn>4</mn> </mrow> </msub> </mrow> <mo>]</mo> </mrow> </mrow> <mrow> <mn>4</mn> <mo>−</mo> </mrow> </msup> </math></EquationSource> </InlineEquation> building blocks which are connected via corner sharing, forming chains along the <i>c</i>-axis. The combination of single crystal X-ray data with experimental Raman spectroscopy and DFT-calculations confirms that the structural model of H<sub>2</sub>CO<sub>3</sub>-<i>C</i><i>m</i><i>c</i>2<sub>1</sub> 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.</p>

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Synthesis and characterization of crystalline polymeric carbonic acid (H2CO3) with sp3-hybridized carbon at elevated pressures

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月8日

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  • Dominik Spahr,
  • Lkhamsuren Bayarjargal,
  • Lukas Brüning,
  • Valentin Kovalev,
  • Lena M. Wedek,
  • Maxim Bykov,
  • Victor Milman,
  • Nico Giordano,
  • Björn Winkler,
  • Elena Bykova

摘要

The existence of polymeric carbonic acid (H2CO3) 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. H2CO3 single crystals were obtained by laser-heating a H2O + CO2 mixture in a diamond anvil cell. The orthorhombic crystal structure (Cmc21 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 H2CO3-Cmc21 is characterized by \({[{{\rm{CO}}}_{4}]}^{4-}\) [ 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 H2CO3-Cmc21 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.