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Title: Atomically Dispersed Reduced Graphene Aerogel-Supported Iridium Catalyst with an Iridium Loading of 14.8 wt %

Abstract

Atomically dispersed iridium complexes were anchored on a reduced graphene aerogel (rGA) by the reaction of Ir(CO)2(acac) [acac = acetonylacetonato] with oxygen-containing groups on the rGA. Characterization by X-ray absorption, infrared, and X-ray photoelectron spectroscopies and atomic resolution aberration-corrected scanning transmission electron microscopy demonstrates atomically dispersed iridium, at the remarkably high loading of 14.8 wt %. The rGA support offers sites for metal bonding comparable to those of metal oxides, but with the advantages of high density and a relatively high degree of uniformity, as indicated by the same turnover frequencies for catalytic hydrogenation of ethylene at low and high iridium loadings. We note the atomic dispersion at a high metal loading—and the high density of catalytic sites per unit of reactor volume, a key criterion for practical catalysts—set this catalyst apart from those reported.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [3]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Koç Univ., Istanbul (Turkey)
  2. Univ. of California, Davis, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Scientific and Technological Research Council of Turkey (TUBITAK)
OSTI Identifier:
1598414
Grant/Contract Number:  
AC02-76SF00515; FG02-04ER15513; 217M547
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 9; Journal Issue: 11; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; single-site; catalyst; iridium; noble metal; graphene; high metal loading; atomic dispersion

Citation Formats

Babucci, Melike, Sarac Oztuna, F. Eylul, Debefve, Louise M., Boubnov, Alexey, Bare, Simon R., Gates, Bruce C., Unal, Ugur, and Uzun, Alper. Atomically Dispersed Reduced Graphene Aerogel-Supported Iridium Catalyst with an Iridium Loading of 14.8 wt %. United States: N. p., 2019. Web. doi:10.1021/acscatal.9b02231.
Babucci, Melike, Sarac Oztuna, F. Eylul, Debefve, Louise M., Boubnov, Alexey, Bare, Simon R., Gates, Bruce C., Unal, Ugur, & Uzun, Alper. Atomically Dispersed Reduced Graphene Aerogel-Supported Iridium Catalyst with an Iridium Loading of 14.8 wt %. United States. https://doi.org/10.1021/acscatal.9b02231
Babucci, Melike, Sarac Oztuna, F. Eylul, Debefve, Louise M., Boubnov, Alexey, Bare, Simon R., Gates, Bruce C., Unal, Ugur, and Uzun, Alper. Tue . "Atomically Dispersed Reduced Graphene Aerogel-Supported Iridium Catalyst with an Iridium Loading of 14.8 wt %". United States. https://doi.org/10.1021/acscatal.9b02231. https://www.osti.gov/servlets/purl/1598414.
@article{osti_1598414,
title = {Atomically Dispersed Reduced Graphene Aerogel-Supported Iridium Catalyst with an Iridium Loading of 14.8 wt %},
author = {Babucci, Melike and Sarac Oztuna, F. Eylul and Debefve, Louise M. and Boubnov, Alexey and Bare, Simon R. and Gates, Bruce C. and Unal, Ugur and Uzun, Alper},
abstractNote = {Atomically dispersed iridium complexes were anchored on a reduced graphene aerogel (rGA) by the reaction of Ir(CO)2(acac) [acac = acetonylacetonato] with oxygen-containing groups on the rGA. Characterization by X-ray absorption, infrared, and X-ray photoelectron spectroscopies and atomic resolution aberration-corrected scanning transmission electron microscopy demonstrates atomically dispersed iridium, at the remarkably high loading of 14.8 wt %. The rGA support offers sites for metal bonding comparable to those of metal oxides, but with the advantages of high density and a relatively high degree of uniformity, as indicated by the same turnover frequencies for catalytic hydrogenation of ethylene at low and high iridium loadings. We note the atomic dispersion at a high metal loading—and the high density of catalytic sites per unit of reactor volume, a key criterion for practical catalysts—set this catalyst apart from those reported.},
doi = {10.1021/acscatal.9b02231},
journal = {ACS Catalysis},
number = 11,
volume = 9,
place = {United States},
year = {2019},
month = {7}
}

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Figures / Tables:

Figure 1 Figure 1: FESEM images of bare rGA at a magnification of (a) 70 kX and (b) 550 kX.

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