Determination of redox reaction rates and orders by in situ liquid cell electron microscopy of Pd and Au solution growth

Sutter, Eli A.; Sutter, Peter W.

doi:10.1021/ja508279v

Title: Determination of redox reaction rates and orders by in situ liquid cell electron microscopy of Pd and Au solution growth

Journal Article · Wed Nov 19 00:00:00 EST 2014 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/ja508279v· OSTI ID:1182529

Sutter, Eli A. ^[1]; Sutter, Peter W. ^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States)

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.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC00112704

OSTI ID:: 1182529

Report Number(s):: BNL-107596-2015-JA; R&D Project: 16060; KC0403020

Journal Information:: Journal of the American Chemical Society, Vol. 136, Issue 48; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 39 works

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In situ electron microscopy of the self-assembly of single-stranded DNA-functionalized Au nanoparticles in aqueous solution Sutter, Eli; Zhang, Bo; Sutter, Stephan Nanoscale, Vol. 11, Issue 1 https://doi.org/10.1039/c8nr08421a	journal	January 2019
Current Status of Liquid-cell Transmission Electron Microscopy Hong, Jaeyoung; Chun, Dong Won Ceramist, Vol. 22, Issue 4 https://doi.org/10.31613/ceramist.2019.22.4.10	journal	December 2019
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Title: Determination of redox reaction rates and orders by in situ liquid cell electron microscopy of Pd and Au solution growth

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