Journal Article

PdMoPtCoNi High Entropy Nanoalloy with d Electron Self‐Complementation‐Induced Multisite Synergistic Effect for Efficient Nanozyme Catalysis

Han, Yaru, Pan, Yifan, Xie, Haijiao, Ping, Jianfeng, Li, Zhonghong, Wang, Jianlong, Tang, Wenzhi, Li, Yuechun, Feng, Jianxing, Yang, Xuewei, Zhu, Wenxin

2024

Overview

Engineering multimetallic nanocatalysts with the entropy‐mediated strategy to reduce reaction activation energy is regarded as an innovative and effective approach to facilitate efficient heterogeneous catalysis. Accordingly, conformational entropy‐driven high‐entropy alloys (HEAs) are emerging as a promising candidate to settle the catalytic efficiency limitations of nanozymes, attributed to their versatile active site compositions and synergistic effects. As proof of the high‐entropy nanozymes (HEzymes) concept, elaborate PdMoPtCoNi HEA nanowires (NWs) with abundant active sites and tuned electronic structures, exhibiting peroxidase‐mimicking activity comparable to that of natural horseradish peroxidase are reported. Density functional theory calculations demonstrate that the enhanced electron abundance of HEA NWs near the Fermi level (EF) is facilitated via the self‐complementation effect among the diverse transition metal sites, thereby boosting the electron transfer efficiency at the catalytic interface through the cocktail effect. Subsequently, the HEzymes are integrated with a portable electronic device that utilizes Internet of Things‐driven signal conversion and wireless transmission functions for point‐of‐care diagnosis to validate their applicability in digital biosensing of urinary biomarkers. The proposed HEzymes underscore significant potential in enhancing nanozymes catalysis through tunable electronic structures and synergistic effects, paving the way for reformative advancements in nano‐bio analysis. As a proof of concept for high‐entropy nanozymes (HEzymes), a class of PdMoPtCoNi nanowires with abundant active sites and tuned electronic structure are designed, and with density functional theory calculations it is demonstrated that their peroxidase‐mimicking activity is comparable to HRP originating from the d electrons self‐complementation effect. The HEzymes are combined with a portable electronic device to achieve IoT‐activated POC digital urinalysis.

• Publisher: John Wiley & Sons, Inc,John Wiley and Sons Inc,Wiley
• Subject: Adsorption / Alloys / Alloys - chemistry / Biosensing Techniques - methods / Catalysis / Design / DFT calculations / Efficiency / Electrons / Energy / Entropy / Enzymes / Fourier transforms / Glucose / heterogeneous catalysis / high‐entropy alloys / Internet of Things / Metals / Morphology / Nanomaterials / Nanoparticles / Nanowires - chemistry / nanozymes / Phase transitions / Solid solutions / Spectrum analysis / Temperature