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<p>There is growing interest in the conversion of CO<sub>2</sub> and CO into energy-dense multi-carbon products to help mitigate climate change, but guiding selectivity remains challenging due to competing pathways. Here we show that tuning the structure of interfacial water using highly concentrated NaClO<sub>4</sub> electrolytes enhances CO electroreduction to C<sub>2</sub>H<sub>4</sub>. Increasing the NaClO<sub>4</sub> concentration from 0.01 to 10 molal increased the CO reduction rate 18-fold, achieving a Faradaic efficiency of 91% for multi-carbon products at −1.43 V versus the normal hydrogen electrode. Temperature-dependent CO reduction, combined with surface-enhanced Raman spectroscopy, revealed that changes in the interfacial H<sub>2</sub>O structure correspond to variations in the apparent activation enthalpy and entropy for the reduction of CO to C<sub>2</sub>H<sub>4</sub>. At higher ionic strength, increases in activation entropy were linked to disrupted hydrogen bonding and the emergence of non-hydrogen-bonded water modes, suggesting that disordered interfacial H<sub>2</sub>O layers facilitate CO reduction to C<sub>2</sub>H<sub>4</sub>. These findings offer valuable insights into how manipulating the structure of interfacial water can enhance the reduction of CO to multi-carbon products.</p><p></p>

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Disordered interfacial H2O promotes electrochemical C–C coupling

  • 期刊论文

  • 发表日期：

    2025年7月23日

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  • Hao Zhang,
  • David Raciti,
  • Anthony Shoji Hall

摘要

There is growing interest in the conversion of CO2 and CO into energy-dense multi-carbon products to help mitigate climate change, but guiding selectivity remains challenging due to competing pathways. Here we show that tuning the structure of interfacial water using highly concentrated NaClO4 electrolytes enhances CO electroreduction to C2H4. Increasing the NaClO4 concentration from 0.01 to 10 molal increased the CO reduction rate 18-fold, achieving a Faradaic efficiency of 91% for multi-carbon products at −1.43 V versus the normal hydrogen electrode. Temperature-dependent CO reduction, combined with surface-enhanced Raman spectroscopy, revealed that changes in the interfacial H2O structure correspond to variations in the apparent activation enthalpy and entropy for the reduction of CO to C2H4. At higher ionic strength, increases in activation entropy were linked to disrupted hydrogen bonding and the emergence of non-hydrogen-bonded water modes, suggesting that disordered interfacial H2O layers facilitate CO reduction to C2H4. These findings offer valuable insights into how manipulating the structure of interfacial water can enhance the reduction of CO to multi-carbon products.