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<p>Electrolysis of CO<sub>2</sub> in molten salts promises efficient carbon capture, but the underlying reaction mechanisms remain incompletely understood, as research thus far has been limited by a lack of tools for <i>operando</i> investigations. Here, we use a high-temperature <i>operando</i> Raman spectroelectrochemical system to look for signatures of reaction intermediates and study the evolution of carbon structures over electrolysis time. The analysis reveals the existence of O<sub>2</sub><sup>2−</sup> concurrently with the deposition of carbon on Au, W, Inconel, and Ni electrode materials, pointing to a common reaction mechanism with O<sub>2</sub><sup>2−</sup> as an intermediate. Secondly, the G peak of the as-deposited carbon experiences a noticeable blue-shift as the material is cooled down and purified, suggesting either a growth in crystallite size even after the electrolysis is stopped or lithium deintercalation. Elucidating the cathodic carbon deposition mechanism could help create greater value-added products and increase the economic viability of carbon capture.</p>

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Operando spectroelectrochemical identification of peroxide intermediate in molten carbonate CO2-to-carbon electroreduction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月21日

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  • Sander Ratso,
  • Michael L. Whittaker,
  • Kätlin Kaare,
  • Raluca O. Scarlat

摘要

Electrolysis of CO2 in molten salts promises efficient carbon capture, but the underlying reaction mechanisms remain incompletely understood, as research thus far has been limited by a lack of tools for operando investigations. Here, we use a high-temperature operando Raman spectroelectrochemical system to look for signatures of reaction intermediates and study the evolution of carbon structures over electrolysis time. The analysis reveals the existence of O22− concurrently with the deposition of carbon on Au, W, Inconel, and Ni electrode materials, pointing to a common reaction mechanism with O22− as an intermediate. Secondly, the G peak of the as-deposited carbon experiences a noticeable blue-shift as the material is cooled down and purified, suggesting either a growth in crystallite size even after the electrolysis is stopped or lithium deintercalation. Elucidating the cathodic carbon deposition mechanism could help create greater value-added products and increase the economic viability of carbon capture.