Structural transformation and catalytic hydrogenation activity of amidinate-protected copper hydride clusters

Chun-Yu Liu, Shang-Fu Yuan, Song Wang, Zong-Jie Guan, Jiang De-en and Quan-Ming Wang ()
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Chun-Yu Liu: Tsinghua University
Shang-Fu Yuan: Tsinghua University
Song Wang: University of California
Zong-Jie Guan: Tsinghua University
Jiang De-en: University of California
Quan-Ming Wang: Tsinghua University

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract Copper hydrides are important hydrogenation catalysts, but their poor stability hinders the practical applications. Ligand engineering is an effective strategy to tackle this issue. An amidinate ligand, N,N′-Di(5-trifluoromethyl-2-pyridyl)formamidinate (Tf-dpf) with four N-donors has been applied as a protecting agent in the synthesis of stable copper hydride clusters: Cu11H3(Tf-dpf)6(OAc)2 (Cu11) with three interfacial μ5-H and [Cu12H3(Tf-dpf)6(OAc)2]·OAc (Cu12) with three interstitial μ6-H. A solvent-triggered reversible interconversion between Cu11 and Cu12 has been observed thanks to the flexibility of Tf-dpf. Cu11 shows high activity in the reduction of 4-nitrophenol to 4-aminophenol, while Cu12 displays very low activity. Deuteration experiments prove that the type of hydride is the key in dictating the catalytic activity, for the interfacial μ5-H species in Cu11 are involved in the catalytic cycle whereas the interstitial μ6-H species in Cu12 are not. This work highlights the role of hydrides with regard to catalytic hydrogenation activity.

Date: 2022
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DOI: 10.1038/s41467-022-29819-y

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