Construction of highly-active nanozymes featuring merits of enzymes and nanomaterials is challenging for biomimetic catalysis. Herein, “confined coordination” strategy was proposed to engineer a novel laccase-nanozyme supported on mesoporous COF-OMe (Cu-Cys@COF-OMe) for the effective degradation of phenolic pollutants. In-situ L-Cysteine modification and confined Cu-coordination implanted unique Cys-multicopper (Cu⁺/Cu²⁺) cluster in COF-OMe mesopores, and engineered biomimetic active pockets to which achieved efficient synergistic diffusion-adsorption-catalysis. Cu-Cys@COF-OMe realized 1.9 times higher enzymatic activity than that of laccase and 2.1–17.0 times higher monatomic copper activity than that of reported state-of-the-art laccase nanozymes, respectively. Besides, Cu-Cys@COF-OMe displayed catalytic merits of nano-materials over laccase, which demonstrated enhanced catalytic activity with temperature and excellent stability under variable reaction conditions. Cu-Cys@COF-OMe nanozyme exhibited 1.4 times faster degradation kinetics (of laccase) for phenolic pollutants, which was further intensified (3.4 times) after exposure to NaCl. This work opens a promising avenue for better design of laccase nanozymes to realize effective phenolic pollutants degradation for large-scale applications.

构建具有酶和纳米材料优点的高活性纳米酶对于仿生催化具有挑战性。在此，提出了“受限配位”策略来设计一种新型漆酶纳米酶，支持介孔 COF-OMe (Cu-Cys@COF-OMe)，以有效降解酚类污染物。原位L-半胱氨酸修饰和受限铜配位植入独特的 Cys-多铜 (Cu ⁺ /Cu ²⁺）在COF-OMe介孔中聚集，并设计了仿生活性口袋，从而实现了有效的协同扩散-吸附-催化。Cu-Cys@COF-OMe 的酶活性是漆酶的 1.9 倍，单原子铜活性是报道的最先进的漆酶纳米酶的 2.1-17.0 倍。此外，Cu-Cys@COF-OMe 与漆酶相比，表现出纳米材料的催化优势，在不同的反应条件下表现出更高的催化活性和优异的稳定性。Cu-Cys@COF-OMe 纳米酶对酚类污染物的降解动力学（漆酶）提高了 1.4 倍，暴露于 NaCl 后进一步增强（3.4 倍）。