Solid Acid Electrochemical Cell for the Production of Hydrogen from Ammonia

Creators: Lim, Dae-Kwang; Plymill, Austin B.; Paik, Haemin; Qian, Xin; Zecevic, Strahinja; Chisholm, Calum R. I.; Haile, Sossina M.

Abstract

Production of high-purity hydrogen by thermal-electrochemical decomposition of ammonia at an intermediate temperature of 250°C is demonstrated. The process is enabled by use of a solid-acid-based electrochemical cell (SAEC) in combination with a bilayered anode, comprising a thermal-cracking catalyst layer and a hydrogen electrooxidation catalyst layer. Cs-promoted Ru on carbon nanotubes (Ru/CNT) serves as the thermal decomposition catalyst, and Pt on carbon black mixed with CsH₂PO₄ is used to catalyze hydrogen electrooxidation. Cells were operated at 250°C with humidified dilute ammonia supplied to the anode and humidified hydrogen supplied to the counter electrode. A current density of 435 mA/cm² was achieved at a potential of 0.4 V and ammonia flow rate of 30 sccm. With a demonstrated faradic efficiency for hydrogen production of 100%, the process yields hydrogen at a rate of 1.48 mol H₂/g_(cat)h.

Additional Information

© 2020 Elsevier Inc. Received 29 June 2020, Revised 16 September 2020, Accepted 8 October 2020, Available online 3 November 2020. The information, data, or work presented herein was funded in large part by the Advanced Research Projects Agency – Energy (ARPA-E), U.S. Department of Energy, under award number DE-AR0000813 of the REFUELS program. This work made use of the EPIC Facility of Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the MRSEC program (NSF DMR-1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. Additionally, this work made use of the Jerome B. Cohen X-Ray Diffraction Facility supported by the MRSEC program of the National Science Foundation (DMR-1720139) at the Materials Research Center of Northwestern University. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States government or any agency thereof. Author Contributions: C.R.I.C. and S.M.H. conceived the project, with S.M.H. providing overall supervision. D.-K.L., A.B.P., H.P., X.Q., and S.Z. designed and carried out experiments. D.-K.L., A.B.P., and S.M.H. analyzed the data. D.-K.L., A.B.P., H.P., S.Z., C.R.I.C., and S.M.H. added conceptual contributions. D.-K.L., A.B.P., H.P., C.R.I.C., and S.M.H. prepared and edited the manuscript. Declaration of Interests: D.-K.L., A.B.P., C.R.I.C., S.Z., and S.M.H. have filed the provisional US patent "solid acid electrochemical cells for the production of hydrogen from liquid fuels." C.R.I.C. and S.Z. are employed by SAFCell, Inc., which aims to develop the technology described here. D.-K.L. is currently affiliated with the Korean Advanced Institute of Science and Technology, Yuseong-gu, Daejeon, Republic of Korea. H.P. is currently affiliated with the Massachusetts Institute of Technology, Cambridge, MA, USA.

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