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

Jun Hyuk Kim, Zhao Ying Chern, Seonyoung Yoo, Ben Deglee, Jenghan Wang, Meilin Liu

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2 引文 斯高帕斯(Scopus)

摘要

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. 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.

原文英語
頁(從 - 到)2370-2379
頁數10
期刊ACS Applied Materials and Interfaces
12
發行號2
DOIs
出版狀態已發佈 - 2020 一月 15

ASJC Scopus subject areas

  • Materials Science(all)

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