High crystallinity design of Ir-based catalysts drives catalytic reversibility for water electrolysis and fuel cells

Woong Hee Lee, Young-Jin Ko, Jung Hwan Kim, Chang Hyuck Choi, Keun Hwa Chae, Hansung Kim, Yun Jeong Hwang, Byoung Koun Min, Peter Strasser () and Hyung-Suk Oh ()
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Woong Hee Lee: Korea Institute of Science and Technology (KIST)
Young-Jin Ko: Korea Institute of Science and Technology (KIST)
Jung Hwan Kim: Yonsei University
Chang Hyuck Choi: Gwangju Institute of Science and Technology
Keun Hwa Chae: Korea Institute of Science and Technology (KIST)
Hansung Kim: Yonsei University
Yun Jeong Hwang: Seoul National University
Byoung Koun Min: Korea Institute of Science and Technology (KIST)
Peter Strasser: Technical University Berlin
Hyung-Suk Oh: Korea Institute of Science and Technology (KIST)

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract The voltage reversal of water electrolyzers and fuel cells induces a large positive potential on the hydrogen electrodes, followed by severe system degradation. Applying a reversible multifunctional electrocatalyst to the hydrogen electrode is a practical solution. Ir exhibits excellent catalytic activity for hydrogen evolution reactions (HER), and hydrogen oxidation reactions (HOR), yet irreversibly converts to amorphous IrOx at potentials > 0.8 V/RHE, which is an excellent catalyst for oxygen evolution reactions (OER), yet a poor HER and HOR catalyst. Harnessing the multifunctional catalytic characteristics of Ir, here we design a unique Ir-based electrocatalyst with high crystallinity for OER, HER, and HOR. Under OER operation, the crystalline nanoparticle generates an atomically-thin IrOx layer, which reversibly transforms into a metallic Ir at more cathodic potentials, restoring high activity for HER and HOR. Our analysis reveals that a metallic Ir subsurface under thin IrOx layer can act as a catalytic substrate for the reduction of Ir ions, creating reversibility. Our work not only uncovers fundamental, uniquely reversible catalytic properties of nanoparticle catalysts, but also offers insights into nanocatalyst design.

Date: 2021
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DOI: 10.1038/s41467-021-24578-8

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