Nanozyme has emerged as promising alternative to natural enzyme during recent years. Currently, laccase nanozyme is mainly limited to Cu-containing materials with catalytic Cu as active site. Noncopper laccase nanozyme, however, has not attracted extensive attention. Herein, inspired by multicopper active site and redox Cu²⁺/Cu⁺ electron transfer pathway of natural laccase, a range of multivalent cerium-based metal-organic frameworks (Ce-MOFs) with considerable laccase-mimicking activity were designed, where the internal cerium redox (Ce⁴⁺/Ce³⁺) reactivity could mimic the active center and catalytic function of natural laccase. Compared with natural laccase, Ce-UiO-66 and Ce-MOF-808 exhibited not only better catalytic efficiency (at identical mass concentration) but also superior stability and recyclability toward the oxidation of phenolic compounds. Accordingly, they were applied for detection of mercaptan contaminants and degradation of bisphenol A, showing great potential in environmental catalysis. This work provides new deep insights for rational design of advanced nanozymes and demonstrates the huge potential of applying nanozymes for environmental remediation.

近年来，纳米酶已成为天然酶的有希望的替代品。目前，漆酶纳米酶主要局限于以催化Cu为活性位点的含Cu材料。然而，非铜漆酶纳米酶并未引起广泛关注。在此，受天然漆酶的多铜活性位点和氧化还原 Cu ²⁺ /Cu ⁺电子传递途径的启发，设计了一系列具有相当大的漆酶模拟活性的多价铈基金属有机骨架（Ce-MOFs），其中内部铈氧化还原（Ce ⁴⁺ /Ce ³⁺) 反应性可以模拟天然漆酶的活性中心和催化功能。与天然漆酶相比，Ce-UiO-66 和 Ce-MOF-808 不仅表现出更好的催化效率（在相同的质量浓度下），而且对酚类化合物的氧化具有优异的稳定性和可回收性。因此，它们被应用于硫醇污染物的检测和双酚A的降解，在环境催化方面显示出巨大的潜力。这项工作为先进纳米酶的合理设计提供了新的深刻见解，并展示了将纳米酶应用于环境修复的巨大潜力。