Paper Publications
Release time: 2024-11-23Hits:
- Affiliation of Author(s):材料科学与工程学院
- Journal:ACS CATALYSIS
- Key Words:Chemistry, Physical
- Abstract:While some early transition metals, such as Ti, can efficiently adsorb and dissociate hydrogen, they have rarely been utilized in hydrogenation and dehydrogenation (de/hydrogenation) reactions because their strong Cat–H bond results in a high hydrogen diffusion barrier. This limitation is known as the macroscopic scaling relation. Herein, using de/hydrogenation reactions of Mg/MgH2 as the example, we report that the hydrogen dissociation and diffusion barrier can be scaled by the Ti valence state, leading to the establishment of a “microscopic” scaling relation. The reaction rates of TiTM-MgO/MgH2 are improved by 69–72 times compared to that of MgH2 under the same conditions, which are even 10 times higher than those of Pd- and Pt-based catalysts. Kinetic analyses and density functional theory (DFT) calculations confirm that the electron transfer properties between catalysts and hydrogens can be systematically controlled as a function of Ti valence states, optimizing the Ti–H bond stability. Significantly, the chemical and structural properties of the TiTM-MgO catalyst remained largely unchanged during and after de/hydrogenation reactions. Our results revealed a “microscopic” scaling relation within a single element governed by its valence state, offering a blueprint for the application of early transition metals in de/hydrogenation reactions.
- Co-author:刘江(学),Yuchuan Ye(外)
- First Author:关浩天(学)
- Indexed by:Journal paper
- Correspondence Author:鲁杨帆,李谦,潘复生
- Document Code:273618
- Page Number:-
- ISSN No.:2155-5435
- Translation or Not:no
- Date of Publication:2024-01-01
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