TY - JOUR
T1 - In Situ Depletion-Guided Engineering of Nanoshell-like Gold Nanocluster Assemblies with Enhanced Peroxidase-like Nanozyme Activity
AU - Bera, Debkumar
AU - Mukhopadhyay, Arun
AU - Nonappa, null
AU - Goswami, Nirmal
N1 - Funding Information:
D.B. thanks Council of Scientific & Industrial Research (CSIR) and A. M. thanks UGC for fellowship. N.G. acknowledges CSIR, New Delhi for financial support under Grant Number HCP-0030 and thanks the Director, CSIR-Institute of Minerals & Materials Technology (IMMT), Bhubaneswar for in-house financial support (Grant Number: OLP-110). We thank Dr. Y S Chaudhary for access to TCSPC facility, Dr. A Giri for the XPS measurements and acknowledge access to the central instrumental facilities led by the central characterization department (CCD) at CSIR IMMT. We acknowledge the Academy of Finland for Project Funding (No. 352900), Photonics Research and Innovation (PREIN) flagship and Tampere Microscopy Centre (TMC), Tampere University, Finland.
Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023
Y1 - 2023
N2 - Functional superstructures constructed from metal nanoclusters (MNCs) hold great promise in providing highly tunable photoluminescence (PL), catalytic activity, photothermal stability, and biological functionality. However, their controlled synthesis with well-defined size, structure, and properties remains a significant challenge. Herein, we introduce a novel approach that combines depletion attraction and thermal activation to induce the in situ formation of spherical superclusters (AuSCs) from Au(I)-thiolate complexes within the assembly. Extensive characterization and electron tomographic reconstruction reveal that Au(I)-thiolate complexes can be sequentially transitioned into metallic Au0, resulting in hollow nanoshell-like structures with consistent size (∼110 nm) and diverse shell configurations. Our results demonstrate that AuSCs with thinner shells, containing a high concentration of Au(I)-thiolate complexes, exhibit the highest PL, while AuSCs with thicker shells, containing high concentrations of metallic gold atoms and low ligand density, show remarkable peroxidase-like nanozyme activity in the 3,3′,5,5′-tetramethylbenzidine (TMB) oxidation reaction.
AB - Functional superstructures constructed from metal nanoclusters (MNCs) hold great promise in providing highly tunable photoluminescence (PL), catalytic activity, photothermal stability, and biological functionality. However, their controlled synthesis with well-defined size, structure, and properties remains a significant challenge. Herein, we introduce a novel approach that combines depletion attraction and thermal activation to induce the in situ formation of spherical superclusters (AuSCs) from Au(I)-thiolate complexes within the assembly. Extensive characterization and electron tomographic reconstruction reveal that Au(I)-thiolate complexes can be sequentially transitioned into metallic Au0, resulting in hollow nanoshell-like structures with consistent size (∼110 nm) and diverse shell configurations. Our results demonstrate that AuSCs with thinner shells, containing a high concentration of Au(I)-thiolate complexes, exhibit the highest PL, while AuSCs with thicker shells, containing high concentrations of metallic gold atoms and low ligand density, show remarkable peroxidase-like nanozyme activity in the 3,3′,5,5′-tetramethylbenzidine (TMB) oxidation reaction.
U2 - 10.1021/acs.jpclett.3c01837
DO - 10.1021/acs.jpclett.3c01837
M3 - Article
C2 - 37561008
AN - SCOPUS:85168235582
SN - 1948-7185
VL - 14
SP - 7299
EP - 7305
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 32
ER -