Minor Impact of Ligand Shell Steric Profile on Colloidal Nanocarbon Catalysis

The catalytic activity of a colloidal nanoparticle is typically inhibited by the very capping agents that are required to maintain colloidal stability and catalyst dispersion. However, the relative importance of steric contributions to the observed attenuation in catalytic activity is poorly underst...

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Main Authors: Chu, Sterling B, Fukushima, Tomohiro, Surendranath, Yogesh
Other Authors: Massachusetts Institute of Technology. Department of Chemistry
Format: Article
Language:en_US
Published: American Chemical Society (ACS) 2018
Online Access:http://hdl.handle.net/1721.1/114224
https://orcid.org/0000-0003-4783-4734
https://orcid.org/0000-0002-6556-3571
https://orcid.org/0000-0003-1016-3420
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author Chu, Sterling B
Fukushima, Tomohiro
Surendranath, Yogesh
author2 Massachusetts Institute of Technology. Department of Chemistry
author_facet Massachusetts Institute of Technology. Department of Chemistry
Chu, Sterling B
Fukushima, Tomohiro
Surendranath, Yogesh
author_sort Chu, Sterling B
collection MIT
description The catalytic activity of a colloidal nanoparticle is typically inhibited by the very capping agents that are required to maintain colloidal stability and catalyst dispersion. However, the relative importance of steric contributions to the observed attenuation in catalytic activity is poorly understood. Herein, we prepare colloidal graphitic carbon nanoparticles featuring covalent amide linkages to aliphatic surface capping agents of varying length. Using aerobic benzylamine oxidation as a test reaction, we find that the steric profile of the ligand shell plays a negligible role in suppressing catalytic activity relative to chemisorption interactions that alter the surface chemistry of the catalyst. The work suggests that heterostructured nanoparticles that provide distinct surface sites for ligand binding and substrate activation should allow for high colloidal stability and robust catalytic activity
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spelling mit-1721.1/1142242022-10-01T11:19:22Z Minor Impact of Ligand Shell Steric Profile on Colloidal Nanocarbon Catalysis Chu, Sterling B Fukushima, Tomohiro Surendranath, Yogesh Massachusetts Institute of Technology. Department of Chemistry Surendranath, Yogesh Chu, Sterling B Fukushima, Tomohiro Surendranath, Yogesh The catalytic activity of a colloidal nanoparticle is typically inhibited by the very capping agents that are required to maintain colloidal stability and catalyst dispersion. However, the relative importance of steric contributions to the observed attenuation in catalytic activity is poorly understood. Herein, we prepare colloidal graphitic carbon nanoparticles featuring covalent amide linkages to aliphatic surface capping agents of varying length. Using aerobic benzylamine oxidation as a test reaction, we find that the steric profile of the ligand shell plays a negligible role in suppressing catalytic activity relative to chemisorption interactions that alter the surface chemistry of the catalyst. The work suggests that heterostructured nanoparticles that provide distinct surface sites for ligand binding and substrate activation should allow for high colloidal stability and robust catalytic activity National Science Foundation (U.S.). Materials Research Science and Engineering Centers (Program) (DMR – 1419807) Massachusetts Institute of Technology. Department of Chemistry 2018-03-19T19:11:19Z 2018-03-19T19:11:19Z 2017-01 2016-11 Article http://purl.org/eprint/type/JournalArticle 0897-4756 1520-5002 http://hdl.handle.net/1721.1/114224 Chu, Sterling B., et al. “Minor Impact of Ligand Shell Steric Profile on Colloidal Nanocarbon Catalysis.” Chemistry of Materials, vol. 29, no. 2, Jan. 2017, pp. 495–98. © 2017 American Chemical Society https://orcid.org/0000-0003-4783-4734 https://orcid.org/0000-0002-6556-3571 https://orcid.org/0000-0003-1016-3420 en_US http://dx.doi.org/10.1021/acs.chemmater.6b04930 Chemistry of Materials Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf American Chemical Society (ACS) Prof. Surendranath via Erja Kajosalo
spellingShingle Chu, Sterling B
Fukushima, Tomohiro
Surendranath, Yogesh
Minor Impact of Ligand Shell Steric Profile on Colloidal Nanocarbon Catalysis
title Minor Impact of Ligand Shell Steric Profile on Colloidal Nanocarbon Catalysis
title_full Minor Impact of Ligand Shell Steric Profile on Colloidal Nanocarbon Catalysis
title_fullStr Minor Impact of Ligand Shell Steric Profile on Colloidal Nanocarbon Catalysis
title_full_unstemmed Minor Impact of Ligand Shell Steric Profile on Colloidal Nanocarbon Catalysis
title_short Minor Impact of Ligand Shell Steric Profile on Colloidal Nanocarbon Catalysis
title_sort minor impact of ligand shell steric profile on colloidal nanocarbon catalysis
url http://hdl.handle.net/1721.1/114224
https://orcid.org/0000-0003-4783-4734
https://orcid.org/0000-0002-6556-3571
https://orcid.org/0000-0003-1016-3420
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