The two-electron water oxidation reaction (2e⁻-WOR) provides a promising route to produce hydrogen peroxide (H₂O₂) from water; but it is currently hampered by low H₂O₂ partial current. Here, intrinsic carbon defect-rich carbon nanofibers are demonstrated to be highly effective for electrochemical 2e⁻-water oxidation. A H₂O₂ current density of 72.6 mA cm⁻² is achieved at 2.9 V vs. RHE which is among the highest values reported for the 2e⁻-WOR. XPS and NEXAFS studies indicate that pentagonal and octagonal ring defects are dominant in the optimal sample. A combination of DFT calculations and a methanol competitive oxidation experiment reveals that ring defects effectively reduce the adsorption strength of OH*, which ultimately promotes the 2e⁻-WOR for valuable H₂O₂ production. Our study makes a helpful attempt in exploring carbon-based materials for efficient 2e⁻-WOR electrocatalysts.

中文翻译：

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在富含固有碳缺陷的碳纳米纤维上高效电化学水氧化成过氧化氢

双电子水氧化反应 (2e ^- -WOR) 为从水中生产过氧化氢 (H ₂ O ₂ )提供了一条有前景的途径；但它目前受到低 H ₂ O ₂部分电流的阻碍。在这里，内在的富含碳缺陷的碳纳米纤维被证明对电化学 2e ^-水氧化非常有效。AH ₂ O ₂电流密度为 72.6 mA cm ^-2在 2.9 V vs. RHE 下实现，这是 2e ^-报告的最高值之​​一-WOR。XPS 和 NEXAFS 研究表明，五边形和八边形环缺陷在最佳样品中占主导地位。DFT 计算和甲醇竞争氧化实验的结合表明，环缺陷有效地降低了 OH* 的吸附强度，最终促进了 2e ^- -WOR 以生产有价值的 H ₂ O ₂。我们的研究在探索用于高效 2e ^- -WOR 电催化剂的碳基材料方面做出了有益的尝试。