Synergize Strong and Reactive Metal-Support Interactions to Construct Sub-2 nm Metal Phosphide Cluster for Enhanced Selective Hydrogenation Activities.

Strong metal-support interactions (SMSI) are crucial for stabilizing sub-2 nm metal sites, e.g. single atom (M1) or cluster (Mn). However, further optimizing sub-2 nm sites to break the activity-stability trade-off due to excessive interactions remains significant challenges. Accordingly, for the first time, we propose synergizing SMSI with reactive metal-support interactions (RMSI). Comprehensive characterization confirms that the SMSI stabilizes the metal and regulates the aggregation of Ni1 into Nin site within sub-2 nm. Meanwhile, RMSI modulates Nin through sufficiently activating P in the support and eventually generates sub-2 nm metal phosphide Ni2P cluster (Ni2Pn). The synergetic metal-support interactions triggered the adaptive coordination and electronic structure optimization of Ni2Pn, leading to the desired substrate adsorption-desorption kinetics. Consequently, the activity of Ni2Pn site greatly enhanced towards the selective hydrogenations of p-chloronitrobenzene and alkynyl alcohol. The formation rates of target products are up to 20.2 and 3.0 times greater than that of Ni1 and Nin site, respectively. This work may open a new direction for metal-support interactions and promote innovation and application of active sites below 2 nm.

• Publication year

  2024

• Venue

  Angewandte Chemie

• Publication date

  2024-09-23

• Fields of study

  Medicine, Materials Science, Chemistry

• Identifiers
  DOI 10.1002/anie.202413788PMID 39313750
• External record

  Open on Semantic Scholar

• Source metadata

  Semantic Scholar, PubMed

• No claims are published for this paper.

• No concepts are published for this paper.

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