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A robust fuel cell operated on nearly dry methane at 500 °C enabled by synergistic thermal catalysis and electrocatalysis

Nature Energy volume 3, pages 1042–1050 (2018)Cite this article

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Abstract

Solid oxide fuel cells (SOFCs) are potentially the most efficient technology for direct conversion of hydrocarbons to electricity. While their commercial viability is greatest at operating temperatures of 300–500 °C, it is extremely difficult to run SOFCs on methane at these temperatures, where oxygen reduction and C–H activation are notoriously sluggish. Here we report a robust SOFC that enabled direct utilization of nearly dry methane (with ~3.5% H2O) at 500 °C (achieving a peak power density of 0.37 W cm−2) with no evidence of coking after ~550 h operation. The cell consists of a PrBa0.5Sr0.5Co1.5Fe0.5O5+δ nanofibre-based cathode and a BaZr0.1Ce0.7Y0.1Yb0.1O3–δ-based multifunctional anode coated with Ce0.90Ni0.05Ru0.05O2 (CNR) catalyst for reforming of CH4 to H2 and CO. The high activity and coking resistance of the CNR is attributed to a synergistic effect of cationic Ni and Ru sites anchored on the CNR surface, as confirmed by in situ/operando experiments and computations.

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Fig. 1: Structure and performance of an intermediate-temperature fuel cell.
Fig. 2: Catalytic performances of steam reforming on Ce0.90Ni0.05Ru0.05O2, Ce0.90Ni0.10O2 and Ce0.90Ru0.10O2 catalysts.
Fig. 3: Coordination environments of singly dispersed Ni atoms (Ni1) and Ru atoms (Ru1) of Ce0.90Ni0.05Ru0.05O2 during catalysis.
Fig. 4: AP-XPS analysis of singly dispersed Ni atoms (Ni1) and Ru atoms (Ru1) of Ce0.90Ni0.05Ru0.05O2 during catalysis.
Fig. 5: Understanding of reactions on the catalyst layer.

Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

This work was supported by the US Department of Energy Advanced Research Projects Agency-Energy (ARPA-E) REBELS program under award no. DE-AR0000502 and the SECA Core Technology Program under award no. DE-FE0031201. The in situ/operando studies, preparation and evaluation of catalysts and the instrumentation of AP-XPS were support by the Catalysis program, Office of Basic Energy Sciences, US Department of Energy, under grant no. DE-SC0014561, and the Division of Chemistry of the NSF under award no.1462121. A part of XAS studies were done at beam line 8-ID (ISS) of the National Synchrotron Light Source II, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laborotary, under Contract No. DE-SC0012704. F.F.T and Y.T. acknowledged E. Stavitski for assistance in XAS experiments.

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  1. These authors contributed equally: Yu Chen, Ben deGlee, Yu Tang.

Authors and Affiliations

  1. School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA, USA

    Yu Chen, Ben deGlee, Bote Zhao, Lei Zhang, Seonyoung Yoo, Kai Pei, Jun Hyuk Kim, Yong Ding & Meilin Liu

  2. Department of Chemical and Petroleum Engineering and Center for Environmentally Beneficial Catalysis, University of Kansas, Lawrence, KS, USA

    Yu Tang, Yuechang Wei & Franklin Feng Tao

  3. School of Chemistry and Chemical Engineering, The Queen’s University of Belfast, Belfast, UK

    Ziyun Wang & P. Hu

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Contributions

M.L. and F.F.T. conceived the concept and supervised the research. Y.C., B.d. and Y.T. contributed equally to this work. Y.C., S.Y. and L.Z. prepared the electrolyte powder. Y.C., B.d., B.Z. and J.H.K. synthesized and tested the cathode and oxygen reduction catalyst materials. Y.C., S.Y. and K.P. fabricated and tested anode-supported single cells with the anodes coated with methane reforming catalysts. Y.C. and Y.D. performed the microanalysis of the electrolyte, electrode and catalyst materials. F.F.T. conceived the concept of dual single-site catalysts of reforming methane to syngas and supervised the synthesis, test and characterization of the reforming catalyst. Y.T. and Y.W. synthesized, tested and characterized the catalysts. Z.W. and P.H. performed the DFT computations. Y.C., B.d., Y.T., F.F.T. and M.L. analysed all experimental data and wrote the paper.

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Correspondence to Franklin Feng Tao or Meilin Liu.

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Chen, Y., deGlee, B., Tang, Y. et al. A robust fuel cell operated on nearly dry methane at 500 °C enabled by synergistic thermal catalysis and electrocatalysis. Nat Energy 3, 1042–1050 (2018). https://doi.org/10.1038/s41560-018-0262-5

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