Thermo-electrochemical production of compressed hydrogen from methane with near-zero energy loss

Abstract

Conventional production of hydrogen requires large industrial plants to minimize energy losses and capital costs associated with steam reforming, water–gas shift, product separation and compression. Here we present a protonic membrane reformer (PMR) that produces high-purity hydrogen from steam methane reforming in a single-stage process with near-zero energy loss. We use a BaZrO3-based proton-conducting electrolyte deposited as a dense film on a porous Ni composite electrode with dual function as a reforming catalyst. At 800 °C, we achieve full methane conversion by removing 99% of the formed hydrogen, which is simultaneously compressed electrochemically up to 50 bar. A thermally balanced operation regime is achieved by coupling several thermo-chemical processes. Modelling of a small-scale (10 kg H2 day−1) hydrogen plant reveals an overall energy efficiency of >87%. The results suggest that future declining electricity prices could make PMRs a competitive alternative for industrial-scale hydrogen plants integrating CO2 capture.

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Fig. 1: Schematic of the protonic membrane reformer.
Fig. 2: Protonic membrane reformer for production of compressed hydrogen.
Fig. 3: Breakdown of voltage losses and microthermal integration at 800 °C.
Fig. 4: Thermo-fluid dynamic simulations.
Fig. 5: Techno-economic evaluation of centralized hydrogen production plant.
Fig. 6: Techno-economic evaluation of distributed hydrogen production.

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Acknowledgements

This work was supported by the Research Council of Norway (grant 256264) and the Spanish Government (SEV-2016-0683 grant). NORTEM is acknowledged for access to transmission electron microscopes.

Author contributions

H.M.-F., D.C., R.Z. and C.K. performed the experiments. H.M.-F., J.M.S., R.H., D.C., P.K.V., T.N. and C.K. designed the experiments. D.B. fabricated the tubular membrane electrode assembly. H.M.-F., C.K., R.H., T.N. and J.M.S. analysed electrochemical data. H.M.-F., J.M.S., S.H.M., R.Z. and C.K. analysed the catalytic data. I.Y.-T. and D.C.-M. designed and performed modelling studies. D.C. collected scanning and transmission electron microscope data. P.K.V. and C.K. initiated the project. H.M.-F., D.C., I.Y.-T., D.C.-M., D.B., S.H.M., P.K.V., T.N., R.H., J.M.S. and C.K. wrote the manuscript, while all authors discussed the results and commented on the manuscript.

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Correspondence to José M. Serra or Christian Kjølseth.

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H.M.-F., D.C., I.Y.-T, D.B., S.H.M., P.K.V. and C.K. are employed by CoorsTek Membrane Sciences (CTMS). T.N. is member of the CTMS board. D.C. postdoctoral research at University of Oslo is partially funded by CTMS. The other authors declare no competing financial interests.

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Supplementary Methods, Supplementary Figures 1–15, Supplementary Tables 1–2 and Supplementary References

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Malerød-Fjeld, H., Clark, D., Yuste-Tirados, I. et al. Thermo-electrochemical production of compressed hydrogen from methane with near-zero energy loss. Nat Energy 2, 923–931 (2017). https://doi.org/10.1038/s41560-017-0029-4

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