Determination of redox reaction rates and orders by in situ liquid cell electron microscopy of Pd and Au solution growth
Abstract
In-situ liquid cell transmission and scanning transmission electron microscopy (TEM/STEM) experiments are important as they provide direct insight into processes in liquids, such as solution growth of nanoparticles among others. In liquid cell TEM/STEM redox reaction experiments the hydrated electrons e⁻aq created by the electron beam are responsible for the reduction of metal-ion complexes. Here we investigate the rate equation of redox reactions involving reduction by e⁻aq generated by the electron beam during in-situ liquid TEM/STEM. Specifically we consider the growth of Pd on Au seeds in aqueous solutions containing Pd-chloro complexes. From the quantification of the rate of Pd deposition at different electron beam currents and as a function of distance from a stationary, nanometer-sized exciting beam, we determine that the reaction is first order with respect to the concentration of hydrated electrons, [e⁻aq]. In addition, by comparing Pd- and Au-deposition, we further demonstrate that measurements of the local deposition rate on nanoparticles in the solution via real-time imaging can be used to measure not only [e⁻aq] but also the rate of reduction of a metal-ion complex to zero-valent metal atoms in solution.
- Authors:
-
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1182529
- Report Number(s):
- BNL-107596-2015-JA
Journal ID: ISSN 0002-7863; R&D Project: 16060; KC0403020
- Grant/Contract Number:
- SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 136; Journal Issue: 48; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; functional nanomaterials; liquid cell TEM/STEM; in-situ TEM/STEM; gold-palladium core-shell nanoparticles; solution growth of Pd and Au; diffusion of hydrated electrons; reaction rate; reaction order
Citation Formats
Sutter, Eli A., and Sutter, Peter W. Determination of redox reaction rates and orders by in situ liquid cell electron microscopy of Pd and Au solution growth. United States: N. p., 2014.
Web. doi:10.1021/ja508279v.
Sutter, Eli A., & Sutter, Peter W. Determination of redox reaction rates and orders by in situ liquid cell electron microscopy of Pd and Au solution growth. United States. https://doi.org/10.1021/ja508279v
Sutter, Eli A., and Sutter, Peter W. Wed .
"Determination of redox reaction rates and orders by in situ liquid cell electron microscopy of Pd and Au solution growth". United States. https://doi.org/10.1021/ja508279v. https://www.osti.gov/servlets/purl/1182529.
@article{osti_1182529,
title = {Determination of redox reaction rates and orders by in situ liquid cell electron microscopy of Pd and Au solution growth},
author = {Sutter, Eli A. and Sutter, Peter W.},
abstractNote = {In-situ liquid cell transmission and scanning transmission electron microscopy (TEM/STEM) experiments are important as they provide direct insight into processes in liquids, such as solution growth of nanoparticles among others. In liquid cell TEM/STEM redox reaction experiments the hydrated electrons e⁻aq created by the electron beam are responsible for the reduction of metal-ion complexes. Here we investigate the rate equation of redox reactions involving reduction by e⁻aq generated by the electron beam during in-situ liquid TEM/STEM. Specifically we consider the growth of Pd on Au seeds in aqueous solutions containing Pd-chloro complexes. From the quantification of the rate of Pd deposition at different electron beam currents and as a function of distance from a stationary, nanometer-sized exciting beam, we determine that the reaction is first order with respect to the concentration of hydrated electrons, [e⁻aq]. In addition, by comparing Pd- and Au-deposition, we further demonstrate that measurements of the local deposition rate on nanoparticles in the solution via real-time imaging can be used to measure not only [e⁻aq] but also the rate of reduction of a metal-ion complex to zero-valent metal atoms in solution.},
doi = {10.1021/ja508279v},
journal = {Journal of the American Chemical Society},
number = 48,
volume = 136,
place = {United States},
year = {Wed Nov 19 00:00:00 EST 2014},
month = {Wed Nov 19 00:00:00 EST 2014}
}
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