Gu Chao-Hai, Wang Song, Zhang Ai-Yong, Liu Chang, Jiang Jun, Yu Han-Qing
CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China.
Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, China.
Nat Commun. 2024 Jul 10;15(1):5771. doi: 10.1038/s41467-024-50240-0.
Developing eco-friendly catalysts for effective water purification with minimal oxidant use is imperative. Herein, we present a metal-free and nitrogen/fluorine dual-site catalyst, enhancing the selectivity and utilization of singlet oxygen (O) for water decontamination. Advanced theoretical simulations reveal that synergistic fluorine-nitrogen interactions modulate electron distribution and polarization, creating asymmetric surface electron configurations and electron-deficient nitrogen vacancies. These properties trigger the selective generation of O from peroxymonosulfate (PMS) and improve the utilization of neighboring reactive oxygen species, facilitated by contaminant enrichment at the fluorine-carbon Lewis-acid adsorption sites. Utilizing these insights, we synthesize the catalyst through montmorillonite (MMT)-assisted pyrolysis (NFC/M). This method leverages the role of MMT as an in-situ layer-stacked template, enabling controlled decomposition of carbon, nitrogen, and fluorine precursors and resulting in a catalyst with enhanced structural adaptability, reactive site accessibility, and mass-transfer capacity. The NFC/M demonstrates an impressive 290.5-fold increase in phenol degradation efficiency than the single-site analogs, outperforming most of metal-based catalysts. This work not only underscores the potential of precise electronic and structural manipulations in catalyst design but also advances the development of efficient and sustainable solutions for water purification.
开发对环境友好的催化剂以在最少使用氧化剂的情况下实现有效的水净化势在必行。在此，我们展示了一种无金属且具有氮/氟双位点的催化剂，可增强单重态氧（O）用于水净化的选择性和利用率。先进的理论模拟表明，氟 - 氮协同相互作用调节电子分布和极化，形成不对称的表面电子构型和缺电子的氮空位。这些特性触发了过一硫酸盐（PMS）选择性生成O，并通过氟 - 碳路易斯酸吸附位点处的污染物富集促进了相邻活性氧物种的利用。利用这些见解，我们通过蒙脱石（MMT）辅助热解合成了该催化剂（NFC/M）。这种方法利用了MMT作为原位层状堆叠模板的作用，实现了碳、氮和氟前驱体的可控分解，从而得到一种具有增强的结构适应性、反应位点可及性和传质能力的催化剂。NFC/M的苯酚降解效率比单位点类似物提高了令人印象深刻的290.5倍，优于大多数金属基催化剂。这项工作不仅强调了在催化剂设计中进行精确电子和结构调控的潜力，还推动了高效且可持续的水净化解决方案的发展。
