Hydrogen holds significance as a versatile energy carrier that can be used in various sectors. Recently, hydroxide exchange membrane electrolyzers (HEMELs) towards clean hydrogen production have gained intensive attention, due to the possibility to use low-cost platinum group metal (PGM)-free electrocatalysts and cheaper membranes, ionomers.1 Although a variety of PGM-free catalysts have shown promising activities towards the alkaline oxygen evolution reaction (OER), few of them delivered sufficient stability in the pure-water-fed HEMELs.2 In this work, metallic aerogel, featured with high porosity and amorphous metal oxide shells, was deployed as platform to study the structural-performance relationship in HEMELs. A poly(aryl piperidinium) membrane and ionomer with high hydroxide conductivity were integrated to study the evolution in the composition and structure of PGM-free anode catalysts.3 Owing to unique properties of the 3D metallic aerogel, the optimal aerogel anode outperformed the Ir-based anode in the KOH-fed HEMELs. A transition in the HEMEL performance with different anode catalyst was observed when shifting from alkaline electrolyte to pure water, implying a steering in the rate limiting steps in the different anode feedings. The limiting factor of pure-water-fed HEMEL was probed by deconvoluting the contributions from ohmic resistance, electrode kinetic, and mass transport. The optimal metallic aerogel anode showed no performance loss during the 580-hour stability test at an industrial electrolyzer-relevant current density of 1 A cm−2 in pure water feeding. The HEMEL performance was monitored, revealing the degradations of critical components in the membrane-electrode-assembly. The structural performance relationship in HEMEL was probed by linking the physical properties of the catalysts with HEMEL performance. The gained insight will shed light on the development of highly efficient PGM-free anode catalysts for viable pure-fed HEMELs.References R. Abbasi, B. P. Setzler, S. Lin, J. Wang, Y. Zhao, H. Xu, B. Pivovar, B. Tian, X. Chen, G. Wu and Y. Yan, Advanced Materials, 31, 1805876 (2019).M. Chatenet, B. G. Pollet, D. R. Dekel, F. Dionigi, J. Deseure, P. Millet, R. D. Braatz, M. Z. Bazant, M. Eikerling, I. Staffell, P. Balcombe, Y. Shao-Horn and H. Schäfer, Chemical Society Reviews, 51, 4583 (2022).J. Wang, Y. Zhao, B. P. Setzler, S. Rojas-Carbonell, C. Ben Yehuda, A. Amel, M. Page, L. Wang, K. Hu, L. Shi, S. Gottesfeld, B. Xu and Y. Yan, Nature Energy, 4, 392 (2019).
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