Unraveling the Mechanism of Water-Mediated Sulfur Tolerance via Operando Surface-Enhanced Raman Spectroscopy

Kim, Jun Hyuk; Chern, Zhao-Ying; Yoo, Seonyoung; deGlee, Ben; Wang, Jenghan; Liu, Meilin

doi:10.1021/acsami.9b17294

Title: Unraveling the Mechanism of Water-Mediated Sulfur Tolerance via Operando Surface-Enhanced Raman Spectroscopy

Journal Article · 16 December 2019 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.9b17294 · OSTI ID:1877395

Kim, Jun Hyuk ^[1]; Chern, Zhao-Ying ^[2]; Yoo, Seonyoung ^[3]; deGlee, Ben ^[3];

^[2];

^[3]

Georgia Inst. of Technology, Atlanta, GA (United States); School of Materials Science & Engineering, Georgia Institute of Technology
National Taiwan Normal Univ., Taipei (Taiwan)
Georgia Inst. of Technology, Atlanta, GA (United States)

While several proton-conducting anode materials have shown excellent tolerance to sulfur poisoning, the mechanism is still unclear due largely to the inability to probe miniscule amounts of sulfur-containing species using conventional surface characterization techniques. Here we present our findings in unraveling the mechanism of water-mediated sulfur tolerance of a proton conductor under operating conditions empowered by surface-sensitive, operando surface-enhanced Raman spectroscopy (SERS) coupled with impedance spectroscopy. Contrary to the conventional view that surface-adsorbed sulfur is removed mainly by oxygen anions, it is found that –SO₄ groups on the surface of the proton conductor are converted to SO₂ by a water-mediated process, as confirmed by operando SERS analysis and density functional theory (DFT)-based calculations. Furthermore, the combination of operando SERS performed on a model electrode and theoretical computation offers an effective approach to investigate into complex mechanisms of electrode processes in various electrochemical systems, providing information vital to achieve the rational design of better electrode materials.

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Research Organization:: Georgia Inst. of Technology, Atlanta, GA (United States)

Sponsoring Organization:: U.S. National Science Foundation; USDOE

Grant/Contract Number:: FE0031201

OSTI ID:: 1877395

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 2 Vol. 12; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
Raman spectroscopy
anode
electrodes
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fuels
oxides
solid oxide fuel cell
sulfur
sulfur poisoning

Title: Unraveling the Mechanism of Water-Mediated Sulfur Tolerance via Operando Surface-Enhanced Raman Spectroscopy

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