The role of nanoparticle size and ligand coverage in size focusing of colloidal metal nanoparticles
Abstract
Controlling the size distribution of nanoparticles is important for many applications and typically involves the use of ligands during synthesis. In this study, we show that the mechanism of size focusing involves a dependence of the growth rate on the size of the nanoparticles and the ligand coverage on the surface of the nanoparticles. To demonstrate these effects, we used in situ small angle X-ray scattering (SAXS) and population balance kinetic modeling (PBM) to investigate the evolution of size distribution during the synthesis of colloidal Pd metal nanoparticles. Despite temporal overlap of nucleation and growth, our in situ SAXS show size focusing of the distribution under different synthetic conditions (different concentrations of metal and ligand as well as solvent type). To understand the mechanism of size focusing using PBM, we systematically studied how the evolution of the nanoparticle size distribution is affected by nucleation rate, and dependence of the growth rate constant on ligand surface coverage, and size of the nanoparticles. We show that continuous nucleation contributes to size defocusing. However, continuous nucleation results in different reaction times for the nanoparticle population leading to time and size-dependent ligand surface coverage. Using density functional theory (DFT) calculations and Brønsted–Evans–Polanyi relations, wemore »
- Authors:
-
[2];
[4];
[2];
[1]
- Department of Chemical Engineering, Virginia Polytechnic Institute and State University, Blacksburg, USA
- Department of Chemical Engineering, University of Pittsburgh, Pittsburgh, USA
- Advanced Photon Source, Argonne National Laboratory, Argonne, USA
- X-ray Science Division, Argonne National Laboratory, Argonne, USA
- Environmental Molecular Science Laboratory, Pacific Northwest National Laboratory, Richland, USA
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1562321
- Alternate Identifier(s):
- OSTI ID: 1781316
- Report Number(s):
- PNNL-SA-161898
Journal ID: ISSN 2516-0230; NAADAI
- Grant/Contract Number:
- AC02-06CH11357; AC05-76RL01830
- Resource Type:
- Published Article
- Journal Name:
- Nanoscale Advances
- Additional Journal Information:
- Journal Name: Nanoscale Advances Journal Volume: 1 Journal Issue: 10; Journal ID: ISSN 2516-0230
- Publisher:
- Royal Society of Chemistry (RSC)
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY
Citation Formats
Mozaffari, Saeed, Li, Wenhui, Dixit, Mudit, Seifert, Soenke, Lee, Byeongdu, Kovarik, Libor, Mpourmpakis, Giannis, and Karim, Ayman M. The role of nanoparticle size and ligand coverage in size focusing of colloidal metal nanoparticles. United Kingdom: N. p., 2019.
Web. doi:10.1039/C9NA00348G.
Mozaffari, Saeed, Li, Wenhui, Dixit, Mudit, Seifert, Soenke, Lee, Byeongdu, Kovarik, Libor, Mpourmpakis, Giannis, & Karim, Ayman M. The role of nanoparticle size and ligand coverage in size focusing of colloidal metal nanoparticles. United Kingdom. https://doi.org/10.1039/C9NA00348G
Mozaffari, Saeed, Li, Wenhui, Dixit, Mudit, Seifert, Soenke, Lee, Byeongdu, Kovarik, Libor, Mpourmpakis, Giannis, and Karim, Ayman M. Tue .
"The role of nanoparticle size and ligand coverage in size focusing of colloidal metal nanoparticles". United Kingdom. https://doi.org/10.1039/C9NA00348G.
@article{osti_1562321,
title = {The role of nanoparticle size and ligand coverage in size focusing of colloidal metal nanoparticles},
author = {Mozaffari, Saeed and Li, Wenhui and Dixit, Mudit and Seifert, Soenke and Lee, Byeongdu and Kovarik, Libor and Mpourmpakis, Giannis and Karim, Ayman M.},
abstractNote = {Controlling the size distribution of nanoparticles is important for many applications and typically involves the use of ligands during synthesis. In this study, we show that the mechanism of size focusing involves a dependence of the growth rate on the size of the nanoparticles and the ligand coverage on the surface of the nanoparticles. To demonstrate these effects, we used in situ small angle X-ray scattering (SAXS) and population balance kinetic modeling (PBM) to investigate the evolution of size distribution during the synthesis of colloidal Pd metal nanoparticles. Despite temporal overlap of nucleation and growth, our in situ SAXS show size focusing of the distribution under different synthetic conditions (different concentrations of metal and ligand as well as solvent type). To understand the mechanism of size focusing using PBM, we systematically studied how the evolution of the nanoparticle size distribution is affected by nucleation rate, and dependence of the growth rate constant on ligand surface coverage, and size of the nanoparticles. We show that continuous nucleation contributes to size defocusing. However, continuous nucleation results in different reaction times for the nanoparticle population leading to time and size-dependent ligand surface coverage. Using density functional theory (DFT) calculations and Brønsted–Evans–Polanyi relations, we show that as the population grows, larger nanoparticles grow more slowly than smaller ones due to lower intrinsic activity and higher ligand coverage on the surface. Therefore, despite continuous nucleation, the faster growth of smaller nanoparticles in the population leads to size focusing. The size focusing behaviour (due to faster growth of smaller nanoparticles) was found to be model independent and similar results were demonstrated under different nucleation and growth pathways (e.g. growth via ion reduction on the surface and/or monomer addition). Our results provide a microscopic connection between kinetics and thermodynamics of nanoparticle growth and metal–ligand binding, and their effect on the size distribution of colloidal nanoparticles.},
doi = {10.1039/C9NA00348G},
journal = {Nanoscale Advances},
number = 10,
volume = 1,
place = {United Kingdom},
year = {2019},
month = {10}
}
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