Institute of Environmental Engineering & Nano-Technology, Institute of Environment and Ecology, Guangdong Provincial Engineering Research Centre for Urban Water Recycling and Environmental Safety, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, China.
College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, 518060, China.
Nat Commun. 2022 Jul 11;13(1):4010. doi: 10.1038/s41467-022-31807-1.
The freshwater scarcity and inadequate access to clean water globally have rallied tremendous efforts in developing robust technologies for water purification and decontamination, and heterogeneous catalysis is a highly-promising solution. Sub-nanometer-confined reaction is the ultimate frontier of catalytic chemistry, yet it is challenging to form the angstrom channels with distributed atomic catalytic centers within, and to match the internal mass transfer and the reactive species' lifetimes. Here, we resolve these issues by applying the concept of the angstrom-confined catalytic water contaminant degradation to achieve unprecedented reaction rates within 4.6 Å channels of two-dimensional laminate membrane assembled from monolayer cobalt-doped titanium oxide nanosheets. The demonstrated degradation rate constant of the target pollutant ranitidine (1.06 ms) is 5-7 orders of magnitude faster compared with the state-of-the-art, achieving the 100% degradation over 100 h continuous operation. This approach is also ~100% effective against diverse water contaminates with a retention time of <30 ms, and the strategy developed can be also extended to other two-dimensional material-assembled membranes. This work paves the way towards the generic angstrom-confined catalysis and unravels the importance of utilizing angstrom-confinement strategy in the design of efficient catalysts for water purification.
全球范围内存在淡水资源短缺和清洁水获取不足的问题，这促使人们大力开发强大的水净化和去污技术，多相催化是一种极具前景的解决方案。亚纳米限域反应是催化化学的终极前沿，但在其中形成具有分布式原子催化中心的埃米通道，并匹配内部传质和反应物种寿命具有挑战性。在这里，我们通过应用埃米限域催化水污染物降解的概念来解决这些问题，在由单层钴掺杂氧化钛纳米片组装而成的二维层状膜的 4.6Å 通道内实现了前所未有的反应速率。目标污染物雷尼替丁的降解速率常数（1.06ms）比最先进的技术快 5-7 个数量级，在 100 小时的连续运行中实现了 100%的降解。这种方法对停留时间<30ms 的多种水污染物的有效率也达到了 100%，所开发的策略还可以扩展到其他二维材料组装膜。这项工作为通用埃米限域催化铺平了道路，并揭示了在设计用于水净化的高效催化剂时利用埃米限域策略的重要性。
