Yu Fengbo, Jia Chao, Wu Xuan, Sun Liming, Shi Zhijian, Teng Tao, Lin Litao, He Zhelin, Gao Jie, Zhang Shicheng, Wang Liang, Wang Shaobin, Zhu Xiangdong
Shanghai Technical Service Platform for Pollution Control and Resource Utilization of Organic Wastes, Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, 200092, Shanghai, China.
Shanghai Institute of Pollution Control and Ecological Security, 200092, Shanghai, China.
Nat Commun. 2023 Aug 17;14(1):4975. doi: 10.1038/s41467-023-40691-2.
Iron-based catalysts are promising candidates for advanced oxidation process-based wastewater remediation. However, the preparation of these materials often involves complex and energy intensive syntheses. Further, due to the inherent limitations of the preparation conditions, it is challenging to realise the full potential of the catalyst. Herein, we develop an iron-based nanomaterial catalyst via soft carbon assisted flash joule heating (FJH). FJH involves rapid temperature increase, electric shock, and cooling, the process simultaneously transforms a low-grade iron mineral (FeS) and soft carbon into an electron rich nano Fe/FeS heterostructure embedded in thin-bedded graphene. The process is energy efficient and consumes 34 times less energy than conventional pyrolysis. Density functional theory calculations indicate that the electron delocalization of the FJH-derived heterostructure improves its binding ability with peroxydisulfate via bidentate binuclear model, thereby enhancing ·OH yield for organics mineralization. The Fe-based nanomaterial catalyst exhibits strong catalytic performance over a wide pH range. Similar catalysts can be prepared using other commonly available iron precursors. Finally, we also present a strategy for continuous and automated production of the iron-based nanomaterial catalysts.
铁基催化剂是基于高级氧化工艺的废水修复的有前途的候选材料。然而，这些材料的制备通常涉及复杂且耗能的合成过程。此外，由于制备条件的固有局限性，要充分发挥催化剂的潜力具有挑战性。在此，我们通过软碳辅助闪速焦耳加热（FJH）开发了一种铁基纳米材料催化剂。FJH涉及快速升温、电冲击和冷却，该过程同时将低品位铁矿物（FeS）和软碳转化为嵌入薄层石墨烯中的富电子纳米Fe/FeS异质结构。该过程具有能源效率，比传统热解消耗的能量少34倍。密度泛函理论计算表明，FJH衍生的异质结构的电子离域通过双齿双核模型提高了其与过二硫酸盐的结合能力，从而提高了用于有机物矿化的·OH产率。铁基纳米材料催化剂在很宽的pH范围内都表现出很强的催化性能。使用其他常见的铁前驱体也可以制备类似的催化剂。最后，我们还提出了一种铁基纳米材料催化剂的连续自动化生产策略。
