School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, Jiangsu 225002, China.
Hubei Key Laboratory of Pollutant Analysis & Reuse Technology College of Chemistry and Chemical Engineering, Hubei Normal University, Huangshi, Hubei 435002, China.
Nano Lett. 2024 Jun 5;24(22):6634-6643. doi: 10.1021/acs.nanolett.4c01193. Epub 2024 May 14.
The effect of strong metal-support interaction (SMSI) has never been systematically studied in the field of nanozyme-based catalysis before. Herein, by coupling two different Pd crystal facets with MnO, i.e., (100) by Pd cube (Pd) and (111) by Pd icosahedron (Pd), we observed the reconstruction of Pd atomic structure within the Pd-MnO interface, with the reconstructed Pd (100) facet more disordered than Pd (111), verifying the existence of SMSI in such coupled system. The rearranged Pd atoms in the interface resulted in enhanced uricase-like catalytic activity, with Pd@MnO demonstrating the best catalytic performance. Theoretical calculations suggested that a more disordered Pd interface led to stronger interactions with intermediates during the uricolytic process. cell experiments and therapy results demonstrated excellent biocompatibility, therapeutic effect, and biosafety for their potential hyperuricemia treatment. Our work provides a brand-new perspective for the design of highly efficient uricase-mimic catalysts.
在此之前,强金属-载体相互作用(SMSI)在基于纳米酶的催化领域从未被系统地研究过。在此,通过将 MnO 与两种不同的 Pd 晶面(Pd 立方体中的(100)和 Pd 二十面体中的(111))耦合,我们观察到 Pd-MnO 界面内 Pd 原子结构的重构,其中重构的 Pd(100)面比 Pd(111)面更无序,验证了这种耦合体系中存在 SMSI。界面中重新排列的 Pd 原子导致尿酸酶样催化活性增强,其中 Pd@MnO 表现出最佳的催化性能。理论计算表明,界面中更无序的 Pd 与尿酸降解过程中的中间产物之间存在更强的相互作用。细胞实验和治疗结果表明,它们具有优异的生物相容性、治疗效果和生物安全性,有望用于高尿酸血症的治疗。我们的工作为设计高效的尿酸酶模拟催化剂提供了全新的视角。