Dual-substrate synergistic catalysis for highly efficient water purification

Lu-Jia Shi, Gui-Xiang Huang, Zhao-Hua Wang, Yanghua Duan, Ying-Jie Zhang, Jie-Jie Chen, Wen-Wei Li, Han-Qing Yu, Menachem Elimelech
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Abstract

Non-radical oxidation of pollutants by direct electron transfer has gained heightened interest in water purification for its higher selectivity and efficiency and lower tendency for byproduct formation than traditional advanced oxidation processes. Engineering of catalysts for efficient activation of two substrates (that is, pollutant and oxidant) is essential to trigger the direct electron transfer reactions but is often hindered by the distinct properties of the co-present substrates. We investigated the individual interaction between the catalyst and each substrate and proposed a dual-substrate synergistic catalysis strategy to achieve separate optimization of each substrate activation process. Experimental and theoretical analyses reveal a strong synergistic effect between the two catalysts that preferentially activate the substrates and have smaller resistance for interfacial electron transfer, thus drastically improving the decontamination efficiency. The dual-substrate synergistic catalysis system offers a conceptual advancement in achieving green and efficient water purification by substrate-specific activation, facilitating flexible design and mechanistic exploration of complex heterogeneous catalytic processes. The dual-substrate catalysis strategy realizes synergistic activation of both oxidant and pollutant via direct oxidative transfer process by employing two catalysts, achieving efficient removal of pollutants with minimal oxidant consumption.

Abstract Image

双底物协同催化高效水净化
与传统的高级氧化工艺相比,直接电子转移法对污染物的非自由基氧化具有更高的选择性和效率以及更低的副产物生成趋势,因此在水净化领域受到了越来越多的关注。有效活化两种底物(即污染物和氧化剂)的催化剂工程对于触发直接电子转移反应至关重要,但通常受到共同存在的底物的不同性质的阻碍。我们研究了催化剂与每个底物之间的相互作用,并提出了双底物协同催化策略,以实现每个底物活化过程的单独优化。实验和理论分析表明,两种催化剂之间具有较强的协同效应,优先激活底物,并且具有较小的界面电子转移阻力,从而大大提高了去污效率。双底物协同催化系统在通过底物特异性活化实现绿色高效水净化方面提供了概念上的进步,促进了复杂非均相催化过程的灵活设计和机理探索。双底物催化策略采用两种催化剂,通过直接氧化转移过程实现氧化剂和污染物的协同活化,以最小的氧化剂消耗实现污染物的高效去除。
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