Singlet oxygen (¹O₂) is a reactive species with oxidation selectivity that is preferred in advanced oxidation processes. However, the underlying mechanism of ¹O₂ selective production remain ambiguous. In this study, we demonstrated that electron localization and high spin state of metal active sites favored peroxymonosulfate (PMS) co-adsorption and dissociation, which promoted selective production of ¹O₂. Under theoretical guidance, single Co atoms anchored on uneven graphite carbon nitride nanosheet (Co-SA/CMN) was fabricated and exhibited the highest ¹O₂ production selectivity so far with 87.8% of the PMS consumed was converted to ¹O₂. The Co-SA/CMN/PMS system exhibited remarkable degradation efficiency to multiple organic pollutants, show strong resistance to environmental interference and robust stability at the device level. Co-SA/CMN/PMS oxidation was assessed as a safe and detoxifying technology, the estrogenic activity and toxicity originating from 17β-estradiol (E2) or its degradation by-products were sufficiently removed. These findings deepen the mechanistic understanding of the origins of high ¹O₂ production selectivity and provide a rational strategy for precisely controlling ¹O₂ generation in PMS activation.

单线态氧 ( ¹ O ₂ ) 是一种具有氧化选择性的活性物质，在高级氧化过程中是首选。然而，¹ O ₂选择性生产的潜在机制仍然不明确。在这项研究中，我们证明了金属活性位点的电子局域化和高自旋态有利于过一硫酸盐 (PMS) 的共吸附和解离，从而促进了¹ O ₂的选择性生产。在理论指导下，制备了锚定在不均匀石墨氮化碳纳米片 (Co-SA/CMN) 上的单个 Co 原子，并表现出最高的¹ O ₂到目前为止，87.8% 消耗的 PMS 的生产选择性转化为¹ O ₂。Co-SA/CMN/PMS系统对多种有机污染物表现出显着的降解效率，在器件层面表现出很强的抗环境干扰能力和稳健稳定性。Co-SA/CMN/PMS 氧化被评估为一种安全的解毒技术，源自 17β-雌二醇 (E2) 或其降解副产物的雌激素活性和毒性已被充分去除。^{这些发现加深了对高1} O ₂生产选择性起源的机理理解，并为精确控制PMS 激活中¹ O ₂的生成提供了合理的策略。