Reactivity mapping of nanoscale defect chemistry under electrochemical reaction conditions

Electrocatalysts often show increased conversion at nanoscale chemical or topographic surface inhomogeneities, resulting in spatially heterogeneous reactivity. Identifying reacting species locally with nanometer precision during chemical conversion is one of the biggest quests in electrochemical sur...

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Bibliographic Details
Published in:Nature communications 2019-12, Vol.10 (1), p.5702-8, Article 5702
Main Authors: Pfisterer, Jonas H. K., Baghernejad, Masoud, Giuzio, Giovanni, Domke, Katrin F.
Format: Article
Language:English
Subjects:
140/133
639/638/161
639/638/542/971
639/766/930/12
Defects
Electrochemistry
Humanities and Social Sciences
Mapping
multidisciplinary
Organic chemistry
Oxidation
Science
Science (multidisciplinary)
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Summary:Electrocatalysts often show increased conversion at nanoscale chemical or topographic surface inhomogeneities, resulting in spatially heterogeneous reactivity. Identifying reacting species locally with nanometer precision during chemical conversion is one of the biggest quests in electrochemical surface science to advance (electro)catalysis and related fields. Here, we demonstrate that electrochemical tip-enhanced Raman spectroscopy can be used for combined topography and reactivity imaging of electro-active surface sites under reaction conditions. We map the electrochemical oxidation of Au nanodefects, a showcase energy conversion and corrosion reaction, with a chemical spatial sensitivity of about 10 nm. The results indicate the reversible, concurrent formation of spatially separated Au 2 O 3 and Au 2 O species at defect-terrace and protrusion sites on the defect, respectively. Active-site chemical nano-imaging under realistic working conditions is expected to be pivotal in a broad range of disciplines where quasi-atomistic reactivity understanding could enable strategic engineering of active sites to rationally tune (electro)chemical device properties. Identifying reacting species locally with nanometer precision is a major challenge in electrochemical surface science. Using operando Raman nanoscopy, authors image the reversible, concurrent formation of nanometer-spatially separated Au 2 O 3 and Au 2 O species during Au nanodefect oxidation.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-019-13692-3