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Research Papers

Deactivation of Ni-YSZ Material in Dry Methane and Oxidation of Various Forms of Deposited Carbon

[+] Author and Article Information
Barbara Novosel

e-mail address: barbara.novosel@fkkt.uni-lj.si

Jadran Maček

Faculty of Chemistry and Chemical Technology and Center of Excellence Low-Carbon Technologies (CO NOT),
University of Ljubljana,
SI-1001 Ljubljana, Slovenia

1Corresponding author. Present address: University of Ljubljana, Faculty of Chemistry and Chemical Technology, POB 537, SI-1001 Ljubljana, Slovenia.

Contributed by the Advanced Energy Systems Division of ASME for publication in the JOURNAL OF FUEL CELL SCIENCE AND TECHNOLOGY. Manuscript received March 22, 2012; final manuscript received July 13, 2012; published online October 22, 2012. Assoc. Editor: Masashi Mori.

J. Fuel Cell Sci. Technol 9(6), 061003 (Oct 22, 2012) (7 pages) doi:10.1115/1.4007272 History: Received March 22, 2012; Revised July 13, 2012

Carbon deposits are the most probable mode of deactivation for solid oxide fuel cell (SOFCs) using methane or higher hydrocarbons as fuel. The deposition of various carbon allotropes on the anode material was studied under dynamic and isothermal conditions. The results show methane dissociation on Ni-YSZ (nickel-yttrium stabilized zirconia) under the temperature-programmed mode in three general steps. Under isothermal conditions, various carbon species formed depending on the temperature. The presence of amorphous, filamentous, pyrolitic, and graphitic carbon allotropes was determined by quadrupole mass spectroscopy (QMS), X-ray crystallography, field emission scanning electron microscopy (FE-SEM), and infrared spectroscopy (IR). Carbon allotropes were subsequently oxidized in the atmosphere with 20.0 vol% and 0.5 vol% of oxygen in argon. Complex oxidation mechanisms were detected and discussed.

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Figures

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Fig. 1

TPR of NiO-YSZ in a mixture of hydrogen/argon and pure hydrogen

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Fig. 2

TPD on the anode material single continuous run (1), sequential run up to 370 °C (2), sequential run up to 650 °C (3), and sequential run up to 900 °C (4) in argon/methane atmosphere

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Fig. 3

Scanning electron microscope images of the activated (TPR) and deactivated Ni-YSZ material (ITD) at different temperatures in dry argon methane atmosphere (96 vol% Ar – 4 vol% methane)

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Fig. 4

XRD patterns of carbon deposits

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Fig. 5

Results of TPO analysis of carbon deposits in oxygen-rich atmosphere

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Fig. 6

Results of TPO analysis of carbon deposits in oxygen-lean atmosphere

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Fig. 7

Scanning electron microscope images (a), (c), and (e) of sample ITD-600 prepared at 600 °C 20 h; (b), (d), and (f) sample ITD-600 after partial oxidation in oxygen lean atmosphere

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