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Direct Observation of Structural Evolution of Metal Chalcogenide in Electrocatalytic Water Oxidation
Beijing Univ Technol, Inst Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China..
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2018 (English)In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 12, no 12, p. 12369-12379Article in journal (Refereed) Published
Abstract [en]

As one of the most remarkable oxygen evolution reaction (OER) electrocatalysts, metal chalcogenides have been intensively reported during the past few decades because of their high OER activities. It has been reported that electron-chemical conversion of metal OER chalcogenides into oxides/hydroxides would take place after the OER. However, the transition mechanism of such unstable structures, as well as the real active sites and catalytic activity during the OER for these electrocatalysts, has not been understood yet; therefore a direct observation for the electrocatalytic water oxidation process, especially at nano or even angstrom scale, is urgently needed. In this research, by employing advanced Cs-corrected transmission electron microscopy (TEM), a step by step oxidational evolution of amorphous electrocatalyst CoSx into crystallized CoOOH in the OER has been in situ captured: irreversible conversion of CoSx to crystallized CoOOH is initiated on the surface of the electrocatalysts with a morphology change via Co(OH)(2) intermediate during the OER measurement, where CoOOH is confirmed as the real active species. Besides, this transition process has also been confirmed by multiple applications of X-ray photoelectron spectroscopy (XPS), in situ Fourier-transform infrared spectroscopy (FTIR), and other ex situ technologies. Moreover, on the basis of this discovery, a high-efficiency electrocatalyst of a nitrogen-doped graphene foam (NGF) coated by CoSx has been explored through a thorough structure transformation of CoOOH. We believe this in situ and in-depth observation of structural evolution in the OER measurement can provide insights into the fundamental understanding of the mechanism for the OER catalysts, thus enabling the more rational design of low-cost and high-efficient electrocatalysts for water splitting.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2018. Vol. 12, no 12, p. 12369-12379
Keywords [en]
in situ TEM, water oxidation, cobalt chalcogenide, structural evolution, XPS
National Category
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-241337DOI: 10.1021/acsnano.8b06312ISI: 000454567500060PubMedID: 30508382Scopus ID: 2-s2.0-85058499382OAI: oai:DiVA.org:kth-241337DiVA, id: diva2:1280807
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QC 20190121

Available from: 2019-01-21 Created: 2019-01-21 Last updated: 2019-01-21Bibliographically approved

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Sun, Licheng

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