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Title: Adsorption and Catalytic Activity of Gold Nanoparticles in Mesoporous Silica: Effect of Pore Size and Dispersion Salinity

Abstract

The assembled state of nanoparticles (NPs) within porous matrices plays a governing role in directing their biological, electronic, and catalytic properties. However, the effects of the spatial confinement and environmental factors, such as salinity, on the NP assemblies within the pores are poorly understood. In this study, we use adsorption isotherms, spectrophotometry, and small-angle neutron scattering to develop a better understanding of the effect of spatial confinement on the assembled state and catalytic performance of gold (Au) NPs in propylamine-functionalized SBA-15 and MCM-41 mesoporous silica materials (mSiO2). We carry out a detailed investigation of the effect of pore diameter and ionic strength on the packing and spatial distribution of AuNPs within mSiO2 to get a comprehensive insight into the structure, functioning, and activity of these NPs. We demonstrate the ability of the adsorbed AuNPs to withstand aggregation under high salinity conditions. We attribute the observed preservation of the adsorbed state of AuNPs to the strong electrostatic attraction between oppositely charged pore walls and AuNPs. The preservation of the structure allows the AuNPs to retain their catalytic activity for a model reaction in high salinity aqueous solution, here, the reduction of p-nitrophenol to p-aminophenol, which otherwise is significantly diminished due tomore » bulk aggregation of the AuNPs. This fundamental study demonstrates the critical role of confinement and dispersion salinity on the adsorption and catalytic performance of NPs.« less

Authors:
 [1]; ORCiD logo [2];  [3];  [4]; ORCiD logo [1]; ORCiD logo [1]
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  1. Louisiana State Univ., Baton Rouge, LA (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Louisiana State Univ., Baton Rouge, LA (United States). Center for Advanced Microstructures and Devices
  4. Ivy Tech Community College of Indiana, Valparaiso, IN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1863296
Grant/Contract Number:  
AC05-00OR22725; CBET-1943986
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 126; Journal Issue: 5; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; adsorption; metal nanoparticles; mixtures; silica; transfer reactions

Citation Formats

Ma, Yingzhen, Nagy, Gergely, Siebenbürger, Miriam, Kaur, Ravneet, Dooley, Kerry M., and Bharti, Bhuvnesh. Adsorption and Catalytic Activity of Gold Nanoparticles in Mesoporous Silica: Effect of Pore Size and Dispersion Salinity. United States: N. p., 2022. Web. doi:10.1021/acs.jpcc.1c09573.
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Ma, Yingzhen, Nagy, Gergely, Siebenbürger, Miriam, Kaur, Ravneet, Dooley, Kerry M., & Bharti, Bhuvnesh. Adsorption and Catalytic Activity of Gold Nanoparticles in Mesoporous Silica: Effect of Pore Size and Dispersion Salinity. United States. https://doi.org/10.1021/acs.jpcc.1c09573
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Ma, Yingzhen, Nagy, Gergely, Siebenbürger, Miriam, Kaur, Ravneet, Dooley, Kerry M., and Bharti, Bhuvnesh. Wed . "Adsorption and Catalytic Activity of Gold Nanoparticles in Mesoporous Silica: Effect of Pore Size and Dispersion Salinity". United States. https://doi.org/10.1021/acs.jpcc.1c09573. https://www.osti.gov/servlets/purl/1863296.
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@article{osti_1863296,
title = {Adsorption and Catalytic Activity of Gold Nanoparticles in Mesoporous Silica: Effect of Pore Size and Dispersion Salinity},
author = {Ma, Yingzhen and Nagy, Gergely and Siebenbürger, Miriam and Kaur, Ravneet and Dooley, Kerry M. and Bharti, Bhuvnesh},
abstractNote = {The assembled state of nanoparticles (NPs) within porous matrices plays a governing role in directing their biological, electronic, and catalytic properties. However, the effects of the spatial confinement and environmental factors, such as salinity, on the NP assemblies within the pores are poorly understood. In this study, we use adsorption isotherms, spectrophotometry, and small-angle neutron scattering to develop a better understanding of the effect of spatial confinement on the assembled state and catalytic performance of gold (Au) NPs in propylamine-functionalized SBA-15 and MCM-41 mesoporous silica materials (mSiO2). We carry out a detailed investigation of the effect of pore diameter and ionic strength on the packing and spatial distribution of AuNPs within mSiO2 to get a comprehensive insight into the structure, functioning, and activity of these NPs. We demonstrate the ability of the adsorbed AuNPs to withstand aggregation under high salinity conditions. We attribute the observed preservation of the adsorbed state of AuNPs to the strong electrostatic attraction between oppositely charged pore walls and AuNPs. The preservation of the structure allows the AuNPs to retain their catalytic activity for a model reaction in high salinity aqueous solution, here, the reduction of p-nitrophenol to p-aminophenol, which otherwise is significantly diminished due to bulk aggregation of the AuNPs. This fundamental study demonstrates the critical role of confinement and dispersion salinity on the adsorption and catalytic performance of NPs.},
doi = {10.1021/acs.jpcc.1c09573},
journal = {Journal of Physical Chemistry. C},
number = 5,
volume = 126,
place = {United States},
year = {Wed Jan 26 00:00:00 EST 2022},
month = {Wed Jan 26 00:00:00 EST 2022}
}
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