Visible-light-assisted peroxymonosulfate (PMS) activation is flourishing in wastewater decontamination, but exploiting safe and efficient activators remains challenging due to a deficient cognition of the activated mechanisms. Hereby, a metal-free g-CN isotype heterojunction (HCN) was successfully synthesized and activated PMS under visible light. The Z-scheme isotype heterojunction significantly meliorated light absorption and carrier migration, thereby enhancing PMS activation. The optimal HCN + PMS system almost completely removed ranitidine (RAN) in 30 min with 7.46–8.48 times higher activity than the monomers. Through systematic experiments and characterizations, we proposed a non-radical mechanism of PMS activation, which generated predominated surface-activated complex and singlet oxygen (O) for pollutant removal. The surface-activated complex degraded RAN by drawing its electrons. This non-radical pathway exhibited tolerance towards background substances and pH fluctuations. Additionally, the broad-spectrum decontamination and recyclability of the system further enhanced its practical applicability. Notably, intermediate analyses confirmed the RAN degradation pathways predicted by theoretical calculations, with the resulting intermediates found to be non-toxic. This study significantly contributes to our understanding of the non-radical mechanisms of PMS activation on g-CN-based activators for micropollutant degradation.

中文翻译：

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用于水净化的无金属 g-C3N4 同型异质结的可见光辅助过一硫酸盐活化：表面活化络合物和 1O2 主导的非自由基机制

可见光辅助过一硫酸盐（PMS）活化在废水净化领域蓬勃发展，但由于对活化机制的认识不足，开发安全高效的活化剂仍然具有挑战性。由此，成功合成了无金属的g-CN同型异质结（HCN）并在可见光下激活了PMS。 Z 型同种型异质结显着改善了光吸收和载流子迁移，从而增强了 PMS 激活。最佳的 HCN + PMS 系统在 30 分钟内几乎完全去除雷尼替丁 (RAN)，其活性比单体高 7.46–8.48 倍。通过系统的实验和表征，我们提出了一种 PMS 活化的非自由基机制，该机制产生主要的表面活化复合物和单线态氧 (O) 以去除污染物。表面活化复合物通过吸引电子来降解 RAN。这种非自由基途径表现出对背景物质和 pH 值波动的耐受性。此外，该系统的广谱净化和可回收性进一步增强了其实际适用性。值得注意的是，中间体分析证实了理论计算预测的 RAN 降解途径，所得中间体被发现是无毒的。这项研究极大地有助于我们理解基于 g-CN 的微污染物降解活化剂 PMS 活化的非自由基机制。