4.8 Article

Strong Metal-Support Interaction for 2D Materials: Application in Noble Metal/TiB2 Heterointerfaces and their Enhanced Catalytic Performance for Formic Acid Dehydrogenation

期刊

ADVANCED MATERIALS
卷 33, 期 32, 页码 -

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202101536

关键词

formic acid dehydrogenation; hydrogen production; MBenes; noble metals; strong metal-support interaction

资金

  1. National Natural Science Foundation of China [21872123, 21902027, U19B2003]
  2. Zhejiang Provincial Natural Science Foundation of China [LY18B030007]
  3. National Research Foundation of Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) programme
  4. National Supercomputing Centre, Singapore [12001868]

向作者/读者索取更多资源

In the study of strong metal-support interaction (SMSI) between noble metal and 2D TiB2 supports, direct evidence of encapsulating metal nanoparticles with TiB2 overlayers to form sintering-resistant core-shell structures is reported. This newly created TiB2-based SMSI promotes catalytic activity and stability simultaneously, optimizing hydrogen production and selectivity. The theoretical and experimental results suggest that the interaction between transition metals and TiB2 overlayers plays a crucial role in creating thermally stable and catalytically active metal/support interfaces for scalable chemical and energy applications.
Strong metal-support interaction (SMSI) is a phenomenon commonly observed on heterogeneous catalysts. Here, direct evidence of SMSI between noble metal and 2D TiB2 supports is reported. The temperature-induced TiB2 overlayers encapsulate the metal nanoparticles, resulting in core-shell nanostructures that are sintering-resistant with metal loadings as high as 12.0 wt%. The TiOx-terminated TiB2 surfaces are the active sites catalyzing the dehydrogenation of formic acid at room temperature. In contrast to the trade-off between stability and activity in conventional SMSI, TiB2-based SMSI promotes catalytic activity and stability simultaneously. By optimizing the thickness and coverage of the overlayer, the Pt/TiB2 catalyst displays an outstanding hydrogen productivity of 13.8 mmol g(cat)(-1) h(-1) in 10.0 m aqueous solution without any additive or pH adjustment, with >99.9% selectivity toward CO2 and H-2. Theoretical studies suggest that the TiB2 overlayers are stabilized on different transition metals through an interplay between covalent and electrostatic interactions. Furthermore, the computationally determined trends in metal-TiB2 interactions are fully consistent with the experimental observations regarding the extent of SMSI on different transition metals. The present research introduces a new means to create thermally stable and catalytically active metal/support interfaces for scalable chemical and energy applications.

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