Using organic oxidation reactions to replace the oxygen evolution reaction is a promising approach for producing high-value organic products and hydrogen. Here, we report a photoelectrochemical benzyl alcohol oxidation system based on an α-Fe₂O₃ photoanode coated with a NiCo-layered double hydroxide (NiCo-LDH) cocatalyst. By adjustment of the relative content of Ni and Co in the NiCo-LDH, the optimized photoanode achieved a benzyl alcohol conversion efficiency of 99.1% and benzoic acid selectivity of 90.9%. Experimental studies revealed that the benzyl alcohol oxidation reaction proceeds via an indirect catalytic mechanism involving high-valence species of the NiCo-LDH cocatalyst. Co in NiCo-LDH reduced the formation energy barrier and oxidative capability of the high-valence species, thereby influencing the performance of the photoanode. This work provides insights into the crucial role of cocatalyst composition in organic reaction oxidation and contributes to developing various photoelectrochemical organic oxidation systems.

中文翻译：

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优化 NiCo-LDH 助催化剂的形成能垒以增强光电化学苯甲醇氧化


使用有机氧化反应代替析氧反应是生产高价值有机产物和氢气的一种很有前途的方法。在这里，我们报道了一种基于 α-Fe₂O₃ 光阳极涂覆有 NiCo 层状双氢氧化物 （NiCo-LDH） 助催化剂的光电化学苯甲醇氧化系统。通过调整 NiCo-LDH 中 Ni 和 Co 的相对含量，优化的光阳极实现了 99.1% 的苯甲醇转化率和 90.9% 的苯甲酸选择性。实验研究表明，苯甲醇氧化反应通过间接催化机制进行，涉及 NiCo-LDH 助催化剂的高价物质。NiCo-LDH 中的 Co 降低了高价物质的形成能垒和氧化能力，从而影响了光阳极的性能。这项工作为助催化剂组成在有机反应氧化中的关键作用提供了见解，并为开发各种光电化学有机氧化系统做出了贡献。