It remains crucial but challenging to construct single-atom photocatalysts based on covalent organic framework (COF) materials in a simple, fast, and controllable manner and to clarify their structure–efficacy relationship. Here, a single-atom photocatalyst (Ni-TpBpy) featuring atomically dispersed Ni sites with a high loading content and a specific tetra-coordinated N₂–Ni–Cl₂ environment in a bipyridine-based COF was for the first time rapidly synthesized using dielectric barrier discharge (DBD) plasma and a wet chemical method. Visible light-driven Ni-TpBpy can achieve 97.8% photodegradation efficiency of acetaminophen at 0.177 min⁻¹ in 30 min, outperforming other advanced photocatalysts. Experimental studies and density-functional theory (DFT) calculation clarified the role of well-dispersed Ni active sites in enhanced photodegradation, which not only narrowed the bandgap, facilitating carrier separation and migration, but also promoted the generation of reactive superoxide radicals. This study represents the first use of single-atom Ni-TpBpy in the efficient photocatalytic degradation of emerging pollutants with remarkable stability and universality, bringing new insights into the application of COF-based single-atom materials in environmental remediation.

中文翻译：

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锚定在基于联吡啶的共价有机框架上的镍单原子：促进对乙酰氨基酚光降解的活性位点


基于共价有机框架 （COF） 材料以简单、快速和可控的方式构建单原子光催化剂并阐明它们的构效关系仍然至关重要但具有挑战性。在这里，首次使用介电势垒放电 （DBD） 等离子体和湿化学方法快速合成了一种单原子光催化剂 （Ni-TpBpy），该光催化剂具有原子分散的 Ni 位点，具有高负载量和特定的四配位 N 2-Ni-Cl ₂ 环境在基于联吡啶的 COF 中。可见光驱动的 Ni-TpBpy 可以在 30 分钟内在 0.177 ^min-1 时实现对乙酰氨基酚 97.8% 的光降解效率，优于其他先进的光催化剂。实验研究和密度泛函理论 （DFT） 计算阐明了分散良好的 Ni 活性位点在增强光降解中的作用，这不仅缩小了带隙，促进了载流子分离和迁移，还促进了反应性超氧自由基的产生。本研究首次将单原子 Ni-TpBpy 用于新兴污染物的高效光催化降解中，具有显著的稳定性和通用性，为基于 COF 的单原子材料在环境修复中的应用带来了新的见解。