Hu Guishan, Zhou Binyu, Zhen Yu, Zhu Junyong, Hou Jingwei, Zhang Yatao, Wang Yong, Van der Bruggend Bart
School of Chemical Engineering, Zhengzhou University Zhengzhou 450001 P. R. China
School of Chemical Engineering, The University of Queensland St Lucia QLD 4072 Australia.
Chem Sci. 2025 Sep 2. doi: 10.1039/d5sc04204f.
Heterogeneous catalysis has emerged as a promising approach for sustainable and efficient water purification due to its high catalytic efficacy and low energy consumption. However, the complex nature of nontraditional water resources (, trace toxic metals, organic molecules, and high salinity) leads to gradual catalyst deactivation, hindering large-scale implementation. Here we introduce the concept of sieving-coupled nanoconfined catalytic water pollutant conversion for rapid purification of complex water sources. This dual-function system was achieved by integrating recycled palladium nanoclusters within covalent organic framework (COF) membranes. The strong interaction between Pd and the pyrazine nitrogen in the COF facilitates the formation of a Pd layer within a 40 nm-thick COF nanofilm. The resultant Pd-TpPz membrane exhibited a high permeability of 85.4 L m h bar while achieving 99.8% for Eriochrome black T. This precise-sieving effect of the membrane enables the efficient catalytic reduction of various pollutants such as rhodamine B (RhB), Cr(vi), and 4-nitroaniline in complex systems. The reported Pd-TpPz membrane evinced favorable long-term stability, recyclability, antimicrobial activity, and acid-base resistance (pH = 2-12), demonstrating its high potential for water treatment. This work paves the way towards the development of sieving-coupled nanoconfined catalysis for rapid water purification.
由于具有高催化效率和低能耗，多相催化已成为一种有前景的可持续高效水净化方法。然而，非传统水资源的复杂性质（如痕量有毒金属、有机分子和高盐度）会导致催化剂逐渐失活，阻碍其大规模应用。在此，我们引入了筛分耦合纳米受限催化水污染物转化的概念，用于快速净化复杂水源。这种双功能系统是通过将回收的钯纳米团簇整合到共价有机框架（COF）膜中实现的。钯与COF中吡嗪氮之间的强相互作用促进了在40纳米厚的COF纳米膜内形成钯层。所得的Pd-TpPz膜表现出85.4 L m h bar的高渗透率，同时对铬黑T的去除率达到99.8%。该膜的这种精确筛分效应能够在复杂体系中高效催化还原各种污染物，如罗丹明B（RhB）、Cr(vi)和4-硝基苯胺。所报道的Pd-TpPz膜表现出良好的长期稳定性、可回收性、抗菌活性和耐酸碱性能（pH = 2-12），证明了其在水处理方面的巨大潜力。这项工作为开发用于快速水净化的筛分耦合纳米受限催化铺平了道路。
