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Understanding the Impact of Sulfur Poisoning on the Methane-Reforming Activity of a Solid Oxide Fuel Cell Anode

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    Research Article

    Understanding the Impact of Sulfur Poisoning on the Methane-Reforming Activity of a Solid Oxide Fuel Cell Anode
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    • Jun Hyuk Kim
      Jun Hyuk Kim
      School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
      More by Jun Hyuk Kim
    • Mingfei Liu
      Mingfei Liu
      Energy Research & Innovation, Phillips 66 Company, 2331 CityWest Blvd., Houston, Texas 77042, United States
      More by Mingfei Liu
    • Yu Chen
      Yu Chen
      School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
      More by Yu Chen
      Orcidhttps://orcid.org/0000-0001-9890-9551
    • Ryan Murphy
      Ryan Murphy
      School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
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    • YongMan Choi*
      YongMan Choi
      College of Photonics, National Yang Ming Chiao Tung University, Tainan 71150, Taiwan
      *Email: [email protected]
      More by YongMan Choi
    • Ying Liu
      Ying Liu
      Energy Research & Innovation, Phillips 66 Company, 2331 CityWest Blvd., Houston, Texas 77042, United States
      More by Ying Liu
    • Meilin Liu*
      Meilin Liu
      School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
      *Email: [email protected]
      More by Meilin Liu
      Orcidhttps://orcid.org/0000-0002-6188-2372
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    ACS Catalysis

    Cite this: ACS Catal. 2021, 11, 21, 13556–13566
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    https://doi.org/10.1021/acscatal.1c02470
    Published October 25, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    Natural gas is one of the most attractive fuels for solid oxide fuel cells (SOFCs) because of the existing fuel distribution infrastructure. Unfortunately, natural gas routinely contains small concentrations of sulfur-containing compounds, which may result in degradation in performance of fuel cells due to sulfur poisoning of Ni-based anodes. To date, the deactivation mechanism of anodes by sulfur remains poorly understood, making it extremely challenging to mitigate the problem. Here, we report our findings in unveiling the mechanism of the electrode processes on a Ni-yttria-stabilized-zirconia (Ni-YSZ) anode, enabled by highly surface-sensitive, in situ surface-enhanced Raman spectroscopy (SERS). While two different configurations of CO reformates were observed on the Ni-YSZ surface during steam methane-reforming (SMR) processes, the accumulation of S–S bonds at the sulfur-contaminated solid–gas interface significantly hinders the subsequent methane-reforming process. The identification of the key steps responsible for sulfur poisoning is vital to the development of effective strategies for minimizing the impact of sulfur on robust SOFC operations.

    Copyright © 2021 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.1c02470.

    • Experimental section, a schematic of the experimental setup for electrochemical measurements (Figure S1); IV characterization of a Ni-YSZ anode-supported cell with H2 at 700 °C (Figure S2); gas composition analysis of the anode exhaust when sulfur-free CH4 is fed (Figure S3); calculated equilibrium gas compositions using HSC chemistry 5 program (Figure S4, Table S1); DRT analyses of impedance spectra (Figure S5); SEM and EDS taken from the anodes after the sulfur-laden methane operation (Figure S6); structural characterization of the model electrode (Figure S7); Raman intensity comparison of 1mM R6G solution between ordinary Raman and SERS (Figure S8); SEM images of the Ag@SiO2 (Figure S9); UV-vis extinction spectra of Ag@SiO2 (Figure S10); temperature-dependent SERS measurements of Ni-YSZ model electrode measured under a reducing atmosphere (1:1 = H2/Ar) (Figure S11); CO stretching frequency on different adsorption site on nickel metal (Figure S12); comparison of S−S bond intensity between sulfur/Ni/YSZ mixture and Ni-YSZ model cell measured at 500 °C with 100 ppm H2S/H2 (Figure S13); in situ SERS analysis of Ni-YSZ model electrode upon exposure to 100 ppm H2S in H2 followed by steam reforming of CH4 at 500 °C (Figure S14); ex situ Raman spectrum of a sulfur-contaminated Ni-YSZ electrode focused on Ni-YSZ interface (Figure S15); comparison of DFT-calculated vibrational frequencies of CO bond (cm–1) on Ni(111) surface (Table S2); and comparison of the vibrational frequencies of CO using Raman spectroscopy under different conditions (Table S3) (PDF)

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    Cited By

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    This article is cited by 21 publications.

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    ACS Catalysis

    Cite this: ACS Catal. 2021, 11, 21, 13556–13566
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acscatal.1c02470
    Published October 25, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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