Electrocatalytic Isoxazoline–Nanocarbon Metal Complexes
Abstract
In this work, we report the synthesis of new carbon-nanomaterial-based metal chelates that enable effective electronic coupling to electrocatalytic transition metals. In particular, multiwalled carbon nanotubes (MWCNTs) and few-layered graphene (FLG) were covalently functionalized by a microwave-assisted cyclo-addition with nitrile oxides to form metal-binding isoxazoline functional groups with high densities. The covalent attachment was evidenced by Raman spectroscopy, and the chemical identity of the surface functional groups was confirmed by X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). The functional carbon nanomaterials effectively chelate precious metals Ir(III), Pt(II), and Ru(III), as well as earth-abundant metals such as Ni(II), to afford materials with metal contents as high as 3.0 atom %. The molecularly dispersed nature of the catalysts was confirmed by X-ray absorption spectroscopy (XAS) and energy-dispersive X-ray spectroscopy (STEM-EDS) elemental mapping. The interplay between the chelate structure on the graphene surface and its metal binding ability has also been investigated by a combination of experimental and computational studies. The defined ligands on the graphene surfaces enable the formation of structurally precise heterogeneous molecular catalysts. The direct attachment of the isoxazoline functional group on the graphene surfaces provides strong electronic coupling between the chelated metal species and themore »
- Authors:
-
[1];
[1];
[2];
[1]
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Inst. for Soldier Nanotechnologies
- Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- National Science Foundation (NSF); National Institutes of Health (NIH); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1864830
- Grant/Contract Number:
- AC02-06CH11357; P42 ES027707; DMR-1809740; 1541959; ECCS-202506
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 143; Journal Issue: 27; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carbon nanotubes; functionalization; metals; radiology; two dimensional materials
Citation Formats
Luo, Shao-Xiong Lennon, Liu, Richard Y., Lee, Sungsik, and Swager, Timothy M. Electrocatalytic Isoxazoline–Nanocarbon Metal Complexes. United States: N. p., 2021.
Web. doi:10.1021/jacs.1c05439.
Luo, Shao-Xiong Lennon, Liu, Richard Y., Lee, Sungsik, & Swager, Timothy M. Electrocatalytic Isoxazoline–Nanocarbon Metal Complexes. United States. https://doi.org/10.1021/jacs.1c05439
Luo, Shao-Xiong Lennon, Liu, Richard Y., Lee, Sungsik, and Swager, Timothy M. Fri .
"Electrocatalytic Isoxazoline–Nanocarbon Metal Complexes". United States. https://doi.org/10.1021/jacs.1c05439. https://www.osti.gov/servlets/purl/1864830.
@article{osti_1864830,
title = {Electrocatalytic Isoxazoline–Nanocarbon Metal Complexes},
author = {Luo, Shao-Xiong Lennon and Liu, Richard Y. and Lee, Sungsik and Swager, Timothy M.},
abstractNote = {In this work, we report the synthesis of new carbon-nanomaterial-based metal chelates that enable effective electronic coupling to electrocatalytic transition metals. In particular, multiwalled carbon nanotubes (MWCNTs) and few-layered graphene (FLG) were covalently functionalized by a microwave-assisted cyclo-addition with nitrile oxides to form metal-binding isoxazoline functional groups with high densities. The covalent attachment was evidenced by Raman spectroscopy, and the chemical identity of the surface functional groups was confirmed by X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). The functional carbon nanomaterials effectively chelate precious metals Ir(III), Pt(II), and Ru(III), as well as earth-abundant metals such as Ni(II), to afford materials with metal contents as high as 3.0 atom %. The molecularly dispersed nature of the catalysts was confirmed by X-ray absorption spectroscopy (XAS) and energy-dispersive X-ray spectroscopy (STEM-EDS) elemental mapping. The interplay between the chelate structure on the graphene surface and its metal binding ability has also been investigated by a combination of experimental and computational studies. The defined ligands on the graphene surfaces enable the formation of structurally precise heterogeneous molecular catalysts. The direct attachment of the isoxazoline functional group on the graphene surfaces provides strong electronic coupling between the chelated metal species and the conductive carbon nanomaterial support. We demonstrate that the metal-chelated carbon nanomaterials are effective heterogeneous catalysts in the oxygen evolution reaction with low overpotentials and tunable catalytic activity.},
doi = {10.1021/jacs.1c05439},
journal = {Journal of the American Chemical Society},
number = 27,
volume = 143,
place = {United States},
year = {Fri Jul 02 00:00:00 EDT 2021},
month = {Fri Jul 02 00:00:00 EDT 2021}
}
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