The application of the classical Fenton reaction has long been limited by several problems, such as metallic sludge and narrow pH range, which derived from the metal components in the catalyst. Developing a metal-free Fenton catalyst may efficiently address these problems. Here, we firstly perform a density functional theory (DFT) study to explore the possibility of developing the 4-phenoxyphenol molecule-doped reduced graphene oxide nanocomposite (rGO-4-PP Nc) as a metal-free Fenton-like catalyst by tuning the electron distribution. The theoretical calculation results reveal that rGO-4-PP Nc can act as an efficient Fenton-like catalyst for H₂O₂ activation and pollutant degradation through formation of electron-rich O and electron-deficient C centers on the C–O–C bridge. The actual rGO-4-PP Nc is also prepared via a surface complexation and copolymerization process. The experimental evidence, such as that gained from XRD, FIIR and EPR analysis, confirm the theoretical models and the dual-reaction-center Fenton-like mechanism. This work provides a basis for theoretical calculation to guide the actual synthesis and prediction of catalytic activity of the Fenton-like catalysts, and also offers a creative perspective to develop new generation metal-free Fenton catalysts by tuning the electron distribution using organic polymers.

中文翻译：

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rGO-4-PP Nc 通过调节电子分布作为无金属类芬顿催化剂的理论和实验证据

经典 Fenton 反应的应用长期以来一直受到一些问题的限制，例如金属污泥和窄 pH 范围，这些问题源于催化剂中的金属成分。开发无金属芬顿催化剂可以有效解决这些问题。在这里，我们首先进行了密度泛函理论 (DFT) 研究，以探索开发 4-苯氧基苯酚分子掺杂的还原氧化石墨烯纳米复合材料 (rGO-4-PP Nc) 作为无金属类芬顿催化剂的可能性电子分布。理论计算结果表明rGO-4-PP Nc可以作为H ₂ O _{2的高效类Fenton催化剂。}通过在 C-O-C 桥上形成富电子 O 和缺电子 C 中心来活化和降解污染物。实际的 rGO-4-PP Nc 也是通过表面络合和共聚过程制备的。XRD、FIIR和EPR分析等实验证据证实了理论模型和双反应中心类Fenton机理。该工作为指导实际合成和预测类芬顿催化剂的催化活性提供了理论计算基础，也为利用有机聚合物调节电子分布开发新一代无金属芬顿催化剂提供了创造性的视角。