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Title: Ligand-Free Noble Metal Nanocluster Catalysts on Carbon Supports via “Soft” Nitriding

We report a robust, universal "soft" nitriding method to grow in situ ligand-free ultrasmall noble metal nanocatalysts (UNMN; e.g., Au, Pd, and Pt) onto carbon. Using low-temperature urea pretreatment at 300 °C, soft nitriding enriches nitrogen-containing species on the surface of carbon supports and enhances the affinity of noble metal precursors onto these supports. We demonstrated sub-2-nm, ligand-free UNMNs grown in situ on seven different types of nitrided carbons with no organic ligands via chemical reduction or thermolysis. Ligand-free UNMNs supported on carbon showed superior electrocatalytic activity for methanol oxidation compared to counterparts with surface capping agents or larger nanocrystals on the same carbon supports. Our method is expected to provide guidelines for the preparation of ligand-free UNMNs on a variety of supports and, additionally, to broaden their applications in energy conversion and electrochemical catalysis.
Authors:
 [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [3] ;  [4] ;  [4]
  1. Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry
  2. Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry; Department of Chemistry, NingXia Medical University, Yinchuan 750004, China
  3. Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry, Inst. of Materials Science, and Green Emulsions, Micelles, and Surfactants Center; Univ. of Connecticut Health Center, Farmington, CT (United States). Dept. of Surgery and Neag Cancer Center; Univ.of Ireland, Galway (Ireland). School of Chemistry
  4. Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry, Inst. of Materials Science, and Green Emulsions, Micelles, and Surfactants Center
Publication Date:
Grant/Contract Number:
FG02-86ER13622
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal Issue: 14; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1467441

Liu, Ben, Yao, Huiqin, Song, Wenqiao, Jin, Lei, Mosa, Islam M., Rusling, James F., Suib, Steven L., and He, Jie. Ligand-Free Noble Metal Nanocluster Catalysts on Carbon Supports via “Soft” Nitriding. United States: N. p., Web. doi:10.1021/jacs.6b01702.
Liu, Ben, Yao, Huiqin, Song, Wenqiao, Jin, Lei, Mosa, Islam M., Rusling, James F., Suib, Steven L., & He, Jie. Ligand-Free Noble Metal Nanocluster Catalysts on Carbon Supports via “Soft” Nitriding. United States. doi:10.1021/jacs.6b01702.
Liu, Ben, Yao, Huiqin, Song, Wenqiao, Jin, Lei, Mosa, Islam M., Rusling, James F., Suib, Steven L., and He, Jie. 2016. "Ligand-Free Noble Metal Nanocluster Catalysts on Carbon Supports via “Soft” Nitriding". United States. doi:10.1021/jacs.6b01702. https://www.osti.gov/servlets/purl/1467441.
@article{osti_1467441,
title = {Ligand-Free Noble Metal Nanocluster Catalysts on Carbon Supports via “Soft” Nitriding},
author = {Liu, Ben and Yao, Huiqin and Song, Wenqiao and Jin, Lei and Mosa, Islam M. and Rusling, James F. and Suib, Steven L. and He, Jie},
abstractNote = {We report a robust, universal "soft" nitriding method to grow in situ ligand-free ultrasmall noble metal nanocatalysts (UNMN; e.g., Au, Pd, and Pt) onto carbon. Using low-temperature urea pretreatment at 300 °C, soft nitriding enriches nitrogen-containing species on the surface of carbon supports and enhances the affinity of noble metal precursors onto these supports. We demonstrated sub-2-nm, ligand-free UNMNs grown in situ on seven different types of nitrided carbons with no organic ligands via chemical reduction or thermolysis. Ligand-free UNMNs supported on carbon showed superior electrocatalytic activity for methanol oxidation compared to counterparts with surface capping agents or larger nanocrystals on the same carbon supports. Our method is expected to provide guidelines for the preparation of ligand-free UNMNs on a variety of supports and, additionally, to broaden their applications in energy conversion and electrochemical catalysis.},
doi = {10.1021/jacs.6b01702},
journal = {Journal of the American Chemical Society},
number = 14,
volume = 138,
place = {United States},
year = {2016},
month = {3}
}