Efficient Electrochemical Water Splitting with PdSn4Dirac Nodal Arc Semimetal

Danil W. Boukhvalov, Chia Nung Kuo, Silvia Nappini, Andrea Marchionni, Gianluca D’Olimpio, Jonathan Filippi, Silvia Mauri, Piero Torelli, Chin Shan Lue, Francesco Vizza, Antonio Politano

研究成果: Article同行評審


Recently, several researchers have claimed the existence of superior catalytic activity associated with topological materials belonging to the class of Dirac/Weyl semimetals, owing to the high electron conductivity and charge carrier mobility in these topological materials. By means of X-ray photoelectron spectroscopy, electrocatalytic tests, and density functional theory, we have investigated the chemical reactivity (chemisorption of ambient gases), ambient stability, and catalytic properties of PdSn4, a topological semimetal showing Dirac node arcs. We find a Tafel slope of 83 mV in the hydrogen evolution reaction (HER) dec-1with an overpotential of 50 mV, with performances resembling those of pure Pd, regardless of its limited amount in the alloy, with a subsequent reduction in the cost of raw materials by ∼80%. Remarkably, the PdSn4-based electrode shows superior robustness to CO compared to pure Pd and Pt and high stability in water media, although the PdSn4surface is prone to oxidation with the formation of a sub-nanometric SnO2skin. Moreover, we also assessed the significance of the role of topological electronic states in the observed catalytic properties. Actually, the peculiar atomic structure of oxidized PdSn4enables the migration of hydrogen atoms through the Sn-O layer with a barrier comparable with the energy cost of the Heyrovsky step of HER over Pt(111) in acidic media (0.1 eV). On the other hand, the topological properties play a minor role, if existing, contrarily to the recent reports overestimating their contribution in catalytic properties.

頁(從 - 到)7311-7318
期刊ACS Catalysis
出版狀態Published - 2021 六月 18

All Science Journal Classification (ASJC) codes

  • 催化
  • 化學 (全部)


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