Reaction Chemistry at Discrete Organometallic Fragments on Black Phosphorus

Mitra, Kendahl L. Walz; Riehs, Michael; Draguicevic, Andrei; Swann, William A.; Li, Christina W.; Velian, Alexandra

doi:10.1002/anie.202311575

Title: Reaction Chemistry at Discrete Organometallic Fragments on Black Phosphorus

Journal Article · 01 November 2023 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202311575 · OSTI ID:2222508

Mitra, Kendahl L. Walz ^[1];

^[1];

^[1]; Swann, William A. ^[2];

^[2];

^[1]

Department of Chemistry University of Washington Seattle WA 98195 USA
Department of Chemistry Purdue University West Lafayette IN 47907 USA

Abstract Black phosphorus (bP) is a two‐dimensional van der Waals material unique in its potential to serve as a support for single‐site catalysts due to its similarity to molecular phosphines, ligands quintessential in homogeneous catalysis. However, there is a scarcity of synthetic methods to install single metal centers on the bP lattice. Here, we demonstrate the functionalization of bP nanosheets with molecular Re and Mo complexes. A suite of characterization techniques, including infrared, X‐ray photoelectron and X‐ray absorption spectroscopy as well as scanning transmission electron microscopy corroborate that the functionalized nanosheets contain a high density of discrete metal centers directly bound to the bP surface. Moreover, the supported metal centers are chemically accessible and can undergo ligand exchange transformations without detaching from the surface. The steric and electronic properties of bP as a ligand are estimated with respect to molecular phosphines. Sterically, bP resembles tri(tolyl)phosphine when monodentate to a metal center, and bis(diphenylphosphino)propane when bidentate, whereas electronically bP is a σ‐donor as strong as a trialkyl phosphine. This work is foundational in elucidating the nature of black phosphorus as a ligand and underscores the viability of using bP as a basis for single‐site catalysts.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; AC02-06CH11357

OSTI ID:: 2222508

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 49 Vol. 62; ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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