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<p>Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols. Herein, we report efficient electrocatalytic oxidations of saturated alcohols (C<sub>1</sub>-C<sub>6</sub>) to selectively form formate using NiCo hydroxide (NiCo–OH) derived NiCo<sub>2</sub>O<sub>4</sub> solid-acid electrocatalysts with balanced Lewis acid (LASs) and Brønsted acid sites (BASs). Thermal treatment transforms BASs-rich (89.6%) NiCo–OH into NiCo<sub>2</sub>O<sub>4</sub> with nearly equal distribution of LASs (53.1%) and BASs (46.9%) which synergistically promote adsorption and activation of OH<sup>−</sup> and alcohol molecules for enhanced oxidation activity. In contrast, BASs-enriched NiCo–OH facilitates formation of higher valence metal sites, beneficial for water oxidation. The combined experimental studies and theoretical calculation imply the oxidation ability of C<sub>1</sub>-C<sub>6</sub> alcohols increases as increased number of hydroxyl groups and decreased HOMO–LUMO gaps: methanol (C<sub>1</sub>) &lt; ethylene glycol (C<sub>2</sub>) &lt; glycerol (C<sub>3</sub>) &lt; meso-erythritol (C<sub>4</sub>) &lt; xylitol (C<sub>5</sub>) &lt; sorbitol (C<sub>6</sub>), while the formate selectivity shows the opposite trend from 100 to 80%. This study unveils synergistic roles of LASs and BASs, as well as hydroxyl group effect in electro-upgrading of alcohols using solid-acid electrocatalysts.</p>

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Saturated Alcohols Electrocatalytic Oxidations on Ni-Co Bimetal Oxide Featuring Balanced B- and L-Acidic Active Sites

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月25日

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  • Junqing Ma,
  • Wenshu Luo,
  • Xunlu Wang,
  • Xu Yu,
  • Jiacheng Jayden Wang,
  • Huashuai Hu,
  • Hanxiao Du,
  • Jianrong Zeng,
  • Wei Chen,
  • Minghui Yang,
  • Jiacheng Wang,
  • Xiangzhi Cui

摘要

Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols. Herein, we report efficient electrocatalytic oxidations of saturated alcohols (C1-C6) to selectively form formate using NiCo hydroxide (NiCo–OH) derived NiCo2O4 solid-acid electrocatalysts with balanced Lewis acid (LASs) and Brønsted acid sites (BASs). Thermal treatment transforms BASs-rich (89.6%) NiCo–OH into NiCo2O4 with nearly equal distribution of LASs (53.1%) and BASs (46.9%) which synergistically promote adsorption and activation of OH− and alcohol molecules for enhanced oxidation activity. In contrast, BASs-enriched NiCo–OH facilitates formation of higher valence metal sites, beneficial for water oxidation. The combined experimental studies and theoretical calculation imply the oxidation ability of C1-C6 alcohols increases as increased number of hydroxyl groups and decreased HOMO–LUMO gaps: methanol (C1) < ethylene glycol (C2) < glycerol (C3) < meso-erythritol (C4) < xylitol (C5) < sorbitol (C6), while the formate selectivity shows the opposite trend from 100 to 80%. This study unveils synergistic roles of LASs and BASs, as well as hydroxyl group effect in electro-upgrading of alcohols using solid-acid electrocatalysts.