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Intermetallic Nanocatalysts from Heterobimetallic Group 10–14 Pyridine-2-thiolate Precursors
Organometallics
  • Carena L. Daniels, Iowa State University
  • Megan Knobeloch, Iowa State University
  • Philip Yox, Iowa State University
  • Marquix A.S. Adamson, Iowa State University
  • Yunhua Chen, Iowa State University
  • Rick W. Dorn, Iowa State University and Ames Laboratory
  • Hao Wu, Ningbo University of Technology
  • Guoquan Zhou, Sichuan University of Science and Engineering
  • Huajun Fan, Ningbo University of Technology
  • Aaron J. Rossini, Iowa State University and Ames Laboratory
  • Javier Vela, Iowa State University and Ames Laboratory
Document Type
Article
Publication Version
Submitted Manuscript
Publication Date
3-3-2020
DOI
10.1021/acs.organomet.9b00803
Abstract

Intermetallic compounds are atomically ordered inorganic materials containing two or more transition metals and main-group elements in unique crystal structures. Intermetallics based on group 10 and group 14 metals have shown enhanced activity, selectivity, and durability in comparison to simple metals and alloys in many catalytic reactions. While high-temperature solid-state methods to prepare intermetallic compounds exist, softer synthetic methods can provide key advantages, such as enabling the preparation of metastable phases or of smaller particles with increased surface areas for catalysis. Here, we study a generalized family of heterobimetallic precursors to binary intermetallics, each containing a group 10 metal and a group 14 tetrel bonded together and supported by pincer-like pyridine-2-thiolate ligands. Upon thermal decomposition, these heterobimetallic complexes form 10–14 binary intermetallic nanocrystals. Experiments and density functional theory (DFT) computations help in better understanding the reactivity of these precursors toward the synthesis of specific intermetallic binary phases. Using Pd2Sn as an example, we demonstrate that nanoparticles made in this way can act as uniquely selective catalysts for the reduction of nitroarenes to azoxyarenes, which highlights the utility of the intermetallics made by our method. Employing heterobimetallic pincer complexes as precursors toward binary nanocrystals and other metal-rich intermetallics provides opportunities to explore the fundamental chemistry and applications of these materials.

Comments

This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Organometallics, copyright © American Chemical Society after peer review. To access the final edited and published work see DOI: 10.1021/acs.organomet.9b00803. Posted with permission.

Copyright Owner
American Chemical Society
Language
en
File Format
application/pdf
Citation Information
Carena L. Daniels, Megan Knobeloch, Philip Yox, Marquix A.S. Adamson, et al.. "Intermetallic Nanocatalysts from Heterobimetallic Group 10–14 Pyridine-2-thiolate Precursors" Organometallics Vol. 39 Iss. 7 (2020) p. 1092 - 1104
Available at: http://works.bepress.com/javier_vela-becerra/55/