文献类型：期刊文献

英文题名：Rational Design of Mnconicuznfe-Based High-Entropy Nanozyme for Cascade Catalysis and Point-of-Care Testing Of Glutathione

作者：Lin, Hua[1]; Li, Ruoke[1]; Xu, Weixin[3]; Ke, Li[1]; Zhou, Shengmin[1]; Zhang, Lin[1]; Pang, Huan[2]; Liu, Yueling[1]

机构：[1] State Key Laboratory of Bioreactor Engineering, School of Biotechnology, East China University of Science and Technology, Shanghai, 200237, China; [2] School of Chemistry and Chemical Engineering, Yangzhou University, Jiangsu, 225009, China; [3] Department of Laboratory Medicine, Jiading District Central Hospital Affiliated Shanghai University of Medicine & Health Sciences, Shanghai, 201800, China

年份：2025

外文期刊名：SSRN

收录：EI(收录号：20250245356)

语种：英文

外文关键词：Analytic equipment - Binary alloys - Density functional theory - Design for testability - Dissociation - Entropy - Free energy - Gibbs free energy - Iron alloys - Manganese alloys - Metal recovery - Microfluidics - Oxygen - Paper

摘要：Prussian blue analogues (PBA) has sparked considerable interest owing to the versatile advantages such as diverse compositions, tunable structure and low price. However, most of the studies previously relied on conventional empirical and trial-and-error methods for identifying the effective catalytic activity. Recent advancements in theory-guided design using predictive models of catalytic performance are leading a new revolution in the field of nanozymes, which has yet to focus on PBA. Herein, a series of PBAs including binary, ternary, quaternary, quinary, and high-entropy were firstly investigated by density functional theory (DFT) calculations. The experimental results and DFT calculations proved the superior catalytic activity of high-entropy (MnCoNiCuZnFe) than medium- and low-entropy PBAs, mainly owing to the enhanced d-band center near Fermi energy level (EF), which strengthened the adsorption of intermediates and subsequently boosted the catalytic efficiency. When combined with 3,3',5,5'-tetramethylbenzidine (TMB) and H2O2, reactive oxygen species (ROS) was produced which oxidized colorless TMB to blue oxTMB. In the presence of glutathione (GSH), the high-entropy PBA oxide (HEO) based colorimetric system exhibited a low detection limit of 0.07 μM, a linear range of 0.10-70.0 μM together with a good recovery ratio in spiked serum samples. Moreover, DFT calculations elucidated the electronic structure by revealing the Gibbs free energy of H2O2 dissociation on individual transition-metal sites, indicating the multi-element synergistic effects underlying the enhanced catalytic performance. Besides, the HEO demonstrated multi-enzymatic activities including oxidase (OXD) and glutathione oxidase (GSHOx). As a proof-of-concept, a microfluidic paper-based analytical device (μPAD) for the point-of-care testing (POCT) of GSH was successfully developed. This study not only provides a rational design strategy for multi-metallic nanomaterials, but also expands the application of high-entropy PBA nanozymes. ? 2025, The Authors. All rights reserved.