Shandong Key Laboratory of Water Pollution Control and Resource Reuse, School of Environmental Science and Engineering, Shandong University, Jinan 250100, P. R. China.
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA 5005, Australia.
Chem Soc Rev. 2021 Apr 26;50(8):5281-5322. doi: 10.1039/d0cs01032d.
Emerging single atom catalysts (SACs), especially carbon-based SACs are appealing materials in environmental catalysis because of their ultrahigh performances, environmental friendliness, structural/chemical robustness, and the maximum utilization of active metal sites. The metal centres, carbon matrixes, and coordination characteristics collectively determine the electronic features of carbon-based SACs, and their behaviours in catalysing peroxide activation and efficiencies in advanced oxidation processes (AOPs). However, there is lack of a comprehensive and critical review reporting the successful marriage of carbon-based SACs in AOP-based remediation technologies. It is particularly necessary to systematically compare and reveal the catalytic sites and the associated mechanisms of carbon-based SACs in diverse AOP systems. In this review, we highlight the synthetic strategies, characterisation, and computation of carbon-based SACs, and for the first time, showcase their innovative applications in AOP technologies. We unveil the origins of versatile catalytic oxidation pathways in different AOP systems and the mechanisms of micropollutant degradation over carbon-based SACs, distinguished from the upsized counterparts (metals/oxides and carbon substrates). We also provide directions to the rational design of on-demand SACs for green chemistry and environmental sustainability. Also, we suggest a designated and integrated experimental/theoretical protocol for revealing the structure-catalysis relations of SACs in AOP applications, and propose the prospects for future opportunities and challenges.
新兴的单原子催化剂（SACs），尤其是基于碳的 SACs，因其超高的性能、环境友好性、结构/化学稳定性以及最大限度地利用活性金属位点，而在环境催化中备受关注。金属中心、碳基质和配位特性共同决定了基于碳的 SACs 的电子特性，以及它们在过氧化物活化和高级氧化过程（AOPs）中的催化效率。然而，目前缺乏全面而批判性的综述来报道基于碳的 SACs 在基于 AOP 的修复技术中的成功结合。系统地比较和揭示不同 AOP 体系中基于碳的 SACs 的催化位点和相关机制是非常必要的。在这篇综述中，我们重点介绍了基于碳的 SACs 的合成策略、特性和计算，并首次展示了它们在 AOP 技术中的创新应用。我们揭示了不同 AOP 体系中多功能催化氧化途径的起源，以及基于碳的 SACs 降解微量污染物的机制，这与传统的大尺寸对应物（金属/氧化物和碳基底）有所不同。我们还为按需设计绿色化学和环境可持续性的 SACs 提供了方向。此外，我们建议了一个指定的、综合的实验/理论方案，以揭示 SACs 在 AOP 应用中的结构-催化关系，并提出了未来的机遇和挑战。
