Direct observation of accelerating hydrogen spillover via surface-lattice-confinement effect.
basic_science · Level V
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- Record sourced from PubMed, PMID 36739275.
- Also identified by DOI 10.1038/s41467-023-36044-8 and PMC identifier 9899253.
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Abstract
Uncovering how hydrogen transfers and what factors control hydrogen conductivity on solid surface is essential for enhancing catalytic performance of H-involving reactions, which is however hampered due to the structural complexity of powder catalysts, in particular, for oxide catalysts. Here, we construct stripe-like MnO(001) and grid-like Mn<sub>3</sub>O<sub>4</sub>(001) monolayers on Pt(111) substrate and investigate hydrogen spillover atop. Atomic-scale visualization demonstrates that hydrogen species from Pt diffuse unidirectionally along the stripes on MnO(001), whereas it exhibits an isotropic pathway on Mn<sub>3</sub>O<sub>4</sub>(001). Dynamic surface imaging in H<sub>2</sub> atmosphere reveals that hydrogen diffuses 4 times more rapidly on MnO than the case on Mn<sub>3</sub>O<sub>4</sub>, which is promoted by one-dimension surface-lattice-confinement effect. Theoretical calculations indicate that a uniform and medium O-O distance favors hydrogen diffusion while low-coordinate surface O atom inhibits it. Our work illustrates the surface-lattice-confinement effect of oxide catalysts on hydrogen spillover and provides a promising route to improve the hydrogen spillover efficiency.