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Selective Atomic Layer Deposition of RuOx Catalysts on Shape-Controlled Pd Nanocrystals with Significantly Enhanced Hydrogen Evolution Activity

Abstract

The electrochemical hydrogen evolution reaction (HER) is an emerging route for producing clean hydrogen. Recently, Ru-based catalysts have exhibited good activity towards HER, making them attractive substitutes for Pt. However, the HER performance of Ru-based catalysts still can not reach the same level as commercial Pt/C in acid solution. The atomic layer deposition (ALD) technique has proved to be an effective route for the preparation of noble metal catalysts on substrates. Herein, we successfully deposited RuOx catalysts on octahedral and cubic Pd seeds through an ALD process. Interestingly, we found that RuOx were selectively deposited on Pd particles when the Pd/nitrogen-doped carbon nanotube (NCNT) were used as the substrate. Importantly, the as-prepared Pd@RuOx/NCNT showed comparable activity with state-of-the-art commercial Pt/C catalysts for the HER. The performance exceeds all of the current Ru-based nanocatalysts for HER in acid solution. The X-ray absorption spectroscy and X-ray photoemission spectroscopy analysis indicated that the RuOx shell consists of metallic Ru and Ru(IV). DFT calculation results indicated that the Gibbs free energy of the intermediate state H* of octahedral Pd@RuOx was much lower than that of cubic Pd@RuOx, which resulted in the superior HER activity. This paper provides an example in rational design of efficient catalysts through combination of shape-controlled synthesis and ALD technique.

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Publication details

The article was received on 13 Sep 2018, accepted on 07 Nov 2018 and first published on 07 Nov 2018


Article type: Paper
DOI: 10.1039/C8TA08931K
Citation: J. Mater. Chem. A, 2018, Accepted Manuscript
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    Selective Atomic Layer Deposition of RuOx Catalysts on Shape-Controlled Pd Nanocrystals with Significantly Enhanced Hydrogen Evolution Activity

    L. Zhang, Z. Zhao, M. Norouzi Banis, L. Li, Y. Zhao, Z. Song, Z. Wang, T. Sham, R. Li, M. Zheng, J. Gong and X. Sun, J. Mater. Chem. A, 2018, Accepted Manuscript , DOI: 10.1039/C8TA08931K

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