Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, Institute of Fine Chemicals, ECUST School of Carbon Neutrality Future Technology, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China.
National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery, School of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai 200237, China.
Proc Natl Acad Sci U S A. 2023 Feb 14;120(7):e2218813120. doi: 10.1073/pnas.2218813120. Epub 2023 Feb 6.
Efficient H harvesting from wastewater instead of pure water can minimize fresh water consumption, which is expected to solve the problem of water shortage in H production process and contribute to carbon neutrality in the environmental remediation, but the inevitable electron depletion caused by electron-consuming pollutants will result in an exhausted H evolution reaction (HER) performance. In this paper, by coupling piezocatalysis and advanced oxidation processes (AOPs) by a MoS/Fe/peroxymonosulfate (PMS) ternary system, extensive types of wastewater achieved considerable H generation, which exceeded the yield in pure water with synchronous advanced degradation of organic pollutants. In addition, profiting from the crucial bridging role of PMS, the H yield in nitrobenzene wastewater after the introduction of PMS-based AOPs increased 3.37-fold from 267.7 μmol·g·h to 901.0 μmol·g·h because the presence of PMS both thermodynamically benefited MoS piezocatalytic H evolution and eliminated the electron depletion caused by organic pollutants. By this way, the original repressed H evolution performance in substrate of wastewater not only was regained but even showed a significant enhancement than that in pure water (505.7 μmol·g·h). Additionally, the cyclonic piezoelectric reactor was preliminarily designed for future industrialization. This strategy provided a valuable path for the recycling of actual wastewater by fuel production and synchronous advanced treatment.
从废水中而不是纯净水中高效地提取氢气可以最小化淡水的消耗，这有望解决氢气生产过程中的缺水问题，并为环境修复中的碳中和做出贡献，但电子消耗污染物不可避免地会耗尽电子，从而导致氢气析出反应（HER）性能耗尽。在本文中，通过将压电催化与先进氧化工艺（AOPs）耦合，利用 MoS/Fe/过一硫酸盐（PMS）三元体系，实现了广泛类型的废水的可观产氢量，超过了在纯水中的产氢量，同时同步实现了有机污染物的高级降解。此外，由于 PMS 的关键桥接作用，在引入基于 PMS 的 AOPs 后，硝基苯废水中的 H 产量从 267.7 μmol·g·h 增加到 901.0 μmol·g·h，增加了 3.37 倍，因为 PMS 的存在从热力学上有利于 MoS 压电催化析氢，并消除了有机污染物引起的电子耗尽。通过这种方式，不仅恢复了废水中底物中原本受到抑制的析氢性能，甚至比在纯水中表现出了显著的增强（505.7 μmol·g·h）。此外，初步设计了旋流压电反应器，为未来的工业化提供了一条有价值的途径，实现了实际废水的回收利用和同步的高级处理。
