Abstract

Nanozymes have broad applications in theranostics and point-of-care tests. To enhance the catalytic activity of nanozymes, the conventional strategy is doping metals to form highly active nanoalloys. However, high-quality and stable nanoalloys are hard to synthesize. Ligand modification is a powerful strategy to achieve chemoselectivity or bioactivity by changing the surface chemistry. Here, we explore different ligands to enhance the catalytic activity of nanozymes, e.g., gold nanoparticles (AuNPs). We systematically studied the impacts on the enzymatic activity of AuNPs by ligand engineering of surface chemistry (charge, group, and surface distance). Our work established critical guidelines for surface modification of nanozymes. The amine group favors higher activity of AuNPs than other groups. The flexible amine-rich ligand enhances the catalytic activity of AuNPs in contrast to other ligands and unmodified AuNPs. Using a proof-of-concept model, we screened many candidate ligands to obtain polyamine-AuNPs, which have strongly enhanced peroxidase-like activity and 100 times enhanced sensitivity compared to unmodified AuNPs. The strategy of enhancing the catalytic activity of AuNPs using ligands will facilitate the catalysis-related applications of nanozymes in biology and diagnostics.

Highlights

  • Gold nanoparticles (AuNPs), one of the most explored artificial enzymes, have multiple enzyme-mimic activities, such as peroxidase (POX), glucose oxidase (GOx), and catalase (Cat).[1, 2] The activities make AuNPs powerful tools for biological and analytical applications.[3,4,5,6,7,8,9,10,11] AuNPs have become the smart building block for the point-of-care test (POCT) and clinical diagnosis

  • We systematically studied the impacts on the enzymatic activity of AuNPs by ligand engineering of surface chemistry

  • Amine alkanethiols with different alkyl carbon numbers (2 ~ 11, 2N, 3N, 4N, 5N, 6N, 8N, and 11N) on surfaces of AuNPs allow angstrom scale adjustment of surface distance

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Summary

Introduction

Gold nanoparticles (AuNPs), one of the most explored artificial enzymes, have multiple enzyme-mimic activities, such as peroxidase (POX), glucose oxidase (GOx), and catalase (Cat).[1, 2] The activities make AuNPs powerful tools for biological and analytical applications.[3,4,5,6,7,8,9,10,11] AuNPs have become the smart building block for the point-of-care test (POCT) and clinical diagnosis. We explore different ligands to enhance the catalytic activity of nanozymes, e.g., gold nanoparticles (AuNPs). We systematically studied the impacts on the enzymatic activity of AuNPs by ligand engineering of surface chemistry (charge, group, and surface distance).

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