Heterogeneous electro-Fenton (e-Fenton) is considered a prospective technology for persistent organic contaminants removal that relies on the strongly oxidizing •OH. However, the efficiency of e-Fenton is still low as the sluggish Fe(II) regeneration caused by the difficulty modulating the electronic structure of Fe(III) center. Herein, the Fe-doped oxidized carbon nanotube catalysts (OCNT-Fe) is prepared to accelerate Fe(II) regeneration by introducing electronegative oxygen-containing groups and inducing local charge distribution of Fe(III) center. The OCNT-1Fe exhibits an excellent e-Fenton performance for phenol degradation with a kinetic rate of 0.11 min⁻¹ at pH 6.5, which is the highest among reported state-of-the-art e-Fenton catalysts. Moreover, OCNT-1Fe catalyst is demonstrated to be more energy efficient in coking wastewater treatment with an energy consumption of 6.5 kW h kg_COD⁻¹ than other e-Fenton systems of 9.2–29.7 kW h kg_COD⁻¹. This work offers a new perspective on the high-performance e-Fenton catalysts design by rationally modulating the electronic structure for organic pollutants removal.

多相电芬顿 (e-Fenton) 被认为是一种有前途的技术，用于去除依赖于强氧化性 •OH 的持久性有机污染物。然而，e-Fenton 的效率仍然很低，因为难以调节 Fe(III) 中心的电子结构，导致 Fe(II) 再生缓慢。在此，制备了 Fe 掺杂的氧化碳纳米管催化剂 (OCNT-Fe)，通过引入电负性含氧基团和诱导 Fe(III) 中心的局部电荷分布来加速 Fe(II) 的再生。OCNT-1Fe 表现出优异的 e-Fenton 苯酚降解性能，动力学速率为 0.11 min ^-1在 pH 6.5 下，这是已报道的最先进的 e-Fenton 催化剂中最高的。_{此外，与 9.2–29.7 kW h kg COD} ^{- 1}的其他 e-Fenton 系统相比，OCNT-1Fe 催化剂在焦化废水处理中的能效更高，能耗为 6.5 kW h kg _COD ^{- 1}。这项工作通过合理调节电子结构以去除有机污染物，为高性能 e-Fenton 催化剂的设计提供了新的视角。