2D Metastable-Phase Hafnium Oxide Triggers Hydrogen Spillover for Boosting Hydrogen Production.
basic_science · Level V
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- Record sourced from PubMed, PMID 40012464.
- Also identified by DOI 10.1002/adma.202415978.
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Abstract
Hydrogen (H) manipulation plays a significantly important role in many important applications, in which the occurrence of hydrogen spillover generally shows substrate-dependent behavior. It therefore remains an open question about how to trigger the hydrogen spillover on the substrates that are generally hydrogen spillover forbidden. Here a new metastable-phase 2D edge-sharing oxide: six-hexagonal phase-hafnium oxide (Hex-HfO<sub>2</sub>, space group: P6<sub>3</sub>mc (186)) with the coordination number of six is demonstrated, which serves as an ideal platform for activating efficient hydrogen spillover after loading Ru nanoclusters (Ru/Hex-HfO<sub>2</sub>). For a stark comparison, the hydrogen spillover is strongly forbidden when using stable monoclinic phase HfO<sub>2</sub> (M-HfO<sub>2</sub>, space group: P2<sub>1</sub>/c (14), coordination number: seven) as the substrate. When applied in an acidic hydrogen evolution reaction (HER), Ru/Hex-HfO<sub>2</sub> exhibits a low overpotential of 8 mV at 10 mA cm<sup>-2</sup> and a high Ru utilization activity of 14.37 A mg<sub>Ru</sub> <sup>-1</sup> at 30 mV. Detailed mechanism reveals the positive H adsorption free energy on Hex-HfO<sub>2</sub>, indicating that H is more likely to spillover on Hex-HfO<sub>2</sub>. Furthermore, the strong interaction between Ru and Hex-HfO<sub>2</sub> optimizes the desorption of hydrogen intermediate, thus facilitating the surface H spillover. The discovery provides new guidance for developing metastable-phase oxide substrates for advanced catalysis.