Borohydride oxidation electrocatalysis at individual, shape‐controlled Au nanoparticles

Abstract Nanostructured materials are frequently employed as active components in electrochemical devices for energy conversion and storage. Unfortunately, the complexity of nanostructured materials, which can exhibit significant heterogeneities in morphology and/or composition within a macroscopic...

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Main Authors: Partha Saha, Md. Maksudur Rahman, Caleb M. Hill
Format: Article
Language:English
Published: Wiley-VCH 2022-10-01
Series:Electrochemical Science Advances
Subjects:
Online Access:https://doi.org/10.1002/elsa.202100120
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author Partha Saha
Md. Maksudur Rahman
Caleb M. Hill
author_facet Partha Saha
Md. Maksudur Rahman
Caleb M. Hill
author_sort Partha Saha
collection DOAJ
description Abstract Nanostructured materials are frequently employed as active components in electrochemical devices for energy conversion and storage. Unfortunately, the complexity of nanostructured materials, which can exhibit significant heterogeneities in morphology and/or composition within a macroscopic sample, makes it difficult to generate fundamental insights into their operation using traditional experimental techniques. Analytical methods that can probe the behavior of individual, discrete reactive entities, such as nanoparticles (NPs), may serve as powerful tools for the study of complex, heterogeneous systems, but remain experimentally challenging. Here, the application of probe‐based electroanalytical methods is demonstrated to be a powerful, high‐throughput strategy for the characterization of electrocatalytic systems. A pipet‐based approach, Targeted Electrochemical Cell Microscopy (TECCM), was applied to characterize the electrocatalytic properties of individual, shape‐controlled Au NPs toward the borohydride oxidation reaction (BOR), a model fuel cell reaction. Using TECCM, the BOR could be quantitatively interrogated at individual NPs in a high‐throughput fashion, directly revealing significant NP‐to‐NP variations in reactivity and stability. BOR kinetics were found to exhibit a significant shape dependence, generally increasing in the order Triangles < Spheres ≈ Octahedra < Rods, and prominent voltammetric features were observed that could be attributed to surface deactivation/reactivation process occurring at individual NPs. Together, these results demonstrate the large degree to which catalytic behavior varies at the single NP level and the power of applying single NP analytical techniques to the study of these systems.
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spelling doaj.art-e722deb8681d46c3b3a32575981ba0842023-08-17T12:00:55ZengWiley-VCHElectrochemical Science Advances2698-59772022-10-0125n/an/a10.1002/elsa.202100120Borohydride oxidation electrocatalysis at individual, shape‐controlled Au nanoparticlesPartha Saha0Md. Maksudur Rahman1Caleb M. Hill2Department of Chemistry University of Wyoming Laramie Wyoming USADepartment of Chemistry University of Wyoming Laramie Wyoming USADepartment of Chemistry University of Wyoming Laramie Wyoming USAAbstract Nanostructured materials are frequently employed as active components in electrochemical devices for energy conversion and storage. Unfortunately, the complexity of nanostructured materials, which can exhibit significant heterogeneities in morphology and/or composition within a macroscopic sample, makes it difficult to generate fundamental insights into their operation using traditional experimental techniques. Analytical methods that can probe the behavior of individual, discrete reactive entities, such as nanoparticles (NPs), may serve as powerful tools for the study of complex, heterogeneous systems, but remain experimentally challenging. Here, the application of probe‐based electroanalytical methods is demonstrated to be a powerful, high‐throughput strategy for the characterization of electrocatalytic systems. A pipet‐based approach, Targeted Electrochemical Cell Microscopy (TECCM), was applied to characterize the electrocatalytic properties of individual, shape‐controlled Au NPs toward the borohydride oxidation reaction (BOR), a model fuel cell reaction. Using TECCM, the BOR could be quantitatively interrogated at individual NPs in a high‐throughput fashion, directly revealing significant NP‐to‐NP variations in reactivity and stability. BOR kinetics were found to exhibit a significant shape dependence, generally increasing in the order Triangles < Spheres ≈ Octahedra < Rods, and prominent voltammetric features were observed that could be attributed to surface deactivation/reactivation process occurring at individual NPs. Together, these results demonstrate the large degree to which catalytic behavior varies at the single NP level and the power of applying single NP analytical techniques to the study of these systems.https://doi.org/10.1002/elsa.202100120electrocatalysiselectrochemical microscopynanoparticlessingle‐entity analysis
spellingShingle Partha Saha
Md. Maksudur Rahman
Caleb M. Hill
Borohydride oxidation electrocatalysis at individual, shape‐controlled Au nanoparticles
Electrochemical Science Advances
electrocatalysis
electrochemical microscopy
nanoparticles
single‐entity analysis
title Borohydride oxidation electrocatalysis at individual, shape‐controlled Au nanoparticles
title_full Borohydride oxidation electrocatalysis at individual, shape‐controlled Au nanoparticles
title_fullStr Borohydride oxidation electrocatalysis at individual, shape‐controlled Au nanoparticles
title_full_unstemmed Borohydride oxidation electrocatalysis at individual, shape‐controlled Au nanoparticles
title_short Borohydride oxidation electrocatalysis at individual, shape‐controlled Au nanoparticles
title_sort borohydride oxidation electrocatalysis at individual shape controlled au nanoparticles
topic electrocatalysis
electrochemical microscopy
nanoparticles
single‐entity analysis
url https://doi.org/10.1002/elsa.202100120
work_keys_str_mv AT parthasaha borohydrideoxidationelectrocatalysisatindividualshapecontrolledaunanoparticles
AT mdmaksudurrahman borohydrideoxidationelectrocatalysisatindividualshapecontrolledaunanoparticles
AT calebmhill borohydrideoxidationelectrocatalysisatindividualshapecontrolledaunanoparticles