Embedding Monodisperse LaO <i> <sub>x</sub> </i> Into Pt Nanoclusters for Ultra‐Stable and Efficient Hydrogen Isotope Oxidation

Catalytic oxidation plays a crucial role in the efficient treatment of hydrogen isotopes, with the key technical challenge being the development of high-performance catalysts to enhance isotope removal efficiency, thereby reducing environmental pollution and ensuring public radiation safety. Herein, the strategic control of platinum nanoclusters confined within silicalite-1 zeolites is reported to enhance the high removal efficiency for hydrogen isotopes under low-temperature conditions for the first time. Incorporating a single lanthanum oxide (LaO<sub>x</sub>) into Pt nanoclusters adapts the local charge of adjacent Pt atoms, significantly altering their electronic structure. The existence of individual LaO<sub>x</sub> species is confirmed by X-ray absorption spectroscopy and aberration-corrected electron microscopy, and the performance enhancement mechanism is further probed by theoretical calculations. This embedded single LaO<sub>x</sub> both facilitates local charge adjustment and supplies abundant active oxygen species, leading to performance enhancement by reducing the energy barrier of rate-determining step (O<sup>*</sup> + H → OH<sup>*</sup>), in accordance with the Mars-van Krevelen mechanism. Consequently, during a surprisingly long-term restart performance test (≈267 d), the PtLaOx@S-1 maintained a high conversion rate over 99% at 50 °C and a space velocity of 48,000 mL·g<sup>-1</sup>·h<sup>-1</sup>. This study highlights the potential of individual LaO<sub>x</sub> sites for enhancing hydrogen isotope oxidation.

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Publication Details

Journal
Advanced Science
Published
2025-05-29
DOI
https://doi.org/10.1002/advs.202504224
Primary Topic
Catalytic Processes in Materials Science
Type
article
Field-Weighted Citation Impact
0.00

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article

Embedding Monodisperse LaO x Into Pt Nanoclusters for Ultra‐Stable and Efficient Hydrogen Isotope Oxidation

Junhong Luo, Xingwen Feng, Feize Li, Linsen Zhou et al.
Advanced Science
Catalytic Processes in Materials Science
article

Embedding Monodisperse LaO x Into Pt Nanoclusters for Ultra‐Stable and Efficient Hydrogen Isotope Oxidation

Junhong Luo, Xingwen Feng, Feize Li, Linsen Zhou, Jiangfeng Song, Xiaoyan Shi, Xianglin Wang, Guilin Wei, Ning Liu
article en

Abstract

Catalytic oxidation plays a crucial role in the efficient treatment of hydrogen isotopes, with the key technical challenge being the development of high-performance catalysts to enhance isotope removal efficiency, thereby reducing environmental pollution and ensuring public radiation safety. Herein, the strategic control of platinum nanoclusters confined within silicalite-1 zeolites is reported to enhance the high removal efficiency for hydrogen isotopes under low-temperature conditions for the first time. Incorporating a single lanthanum oxide (LaO<sub>x</sub>) into Pt nanoclusters adapts the local charge of adjacent Pt atoms, significantly altering their electronic structure. The existence of individual LaO<sub>x</sub> species is confirmed by X-ray absorption spectroscopy and aberration-corrected electron microscopy, and the performance enhancement mechanism is further probed by theoretical calculations. This embedded single LaO<sub>x</sub> both facilitates local charge adjustment and supplies abundant active oxygen species, leading to performance enhancement by reducing the energy barrier of rate-determining step (O<sup>*</sup> + H → OH<sup>*</sup>), in accordance with the Mars-van Krevelen mechanism. Consequently, during a surprisingly long-term restart performance test (≈267 d), the PtLaOx@S-1 maintained a high conversion rate over 99% at 50 °C and a space velocity of 48,000 mL·g<sup>-1</sup>·h<sup>-1</sup>. This study highlights the potential of individual LaO<sub>x</sub> sites for enhancing hydrogen isotope oxidation.

Advanced ScienceVol. 12(30)
Sichuan University (CN), China Academy of Engineering Physics (CN)
National Natural Science Foundation of China
Openalex Percentile: Top 92%
Catalytic Processes in Materials Science
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