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

Journal Article · · ACS Catalysis

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.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Scientific and Technological Research Council of Turkey (TUBITAK)
Grant/Contract Number:
AC02-76SF00515; FG02-04ER15513; 217M547
OSTI ID:
1598414
Journal Information:
ACS Catalysis, Vol. 9, Issue 11; ISSN 2155-5435
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 45 works
Citation information provided by
Web of Science

References (31)

Bridging homogeneous and heterogeneous catalysis by heterogeneous single-metal-site catalysts journal June 2018
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT journal June 2005
The electronic structure of iridium and its oxides: The electronic structure of iridium and its oxides journal December 2015
Probing the Thermal Deoxygenation of Graphene Oxide Using High-Resolution In Situ X-ray-Based Spectroscopies journal August 2011
Isolated Metal Atom Geometries as a Strategy for Selective Heterogeneous Hydrogenations journal March 2012
Operando study of iridium acetylacetonate decomposition on amorphous silica–alumina for bifunctional catalyst preparation journal January 2010
Homogeneity of Surface Sites in Supported Single-Site Metal Catalysts: Assessment with Band Widths of Metal Carbonyl Infrared Spectra journal September 2016
A new method for parameterization of phase shift and backscattering amplitude journal March 1995
Layer-by-Layer Grown Electrodes Composed of Cationic Fe 3 O 4 Nanoparticles and Graphene Oxide Nanosheets for Electrochemical Energy Storage Devices journal January 2019
Self-Assembled Three-Dimensional Graphene-Based Aerogel with Embedded Multifarious Functional Nanoparticles and Its Excellent Photoelectrochemical Activities journal January 2014
Oxide- and Zeolite-Supported Isostructural Ir(C 2 H 4 ) 2 Complexes: Molecular-Level Observations of Electronic Effects of Supports as Ligands journal August 2012
Catalysis by Supported Single Metal Atoms journal November 2016
Synthesis and Characterization of Highly Crystalline Graphene Aerogels journal October 2014
Nature of the metal-support interface in supported metal catalysts: Results from X-ray absorption spectroscopy journal January 1992
Report of the international workshop on standards and criteria in X-ray absorption spectroscopy journal June 1989
Stability investigation of a high number density Pt 1 /Fe 2 O 3 single-atom catalyst under different gas environments by HAADF-STEM journal March 2018
Beating Heterogeneity of Single-Site Catalysts: MgO-Supported Iridium Complexes journal March 2018
Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis journal April 2013
Fabrication of Single-Atom Catalysts with Precise Structure and High Metal Loading journal October 2018
Transmission and fluorescence X-ray absorption spectroscopy cell/flow reactor for powder samples under vacuum or in reactive atmospheres journal July 2016
Single-atom catalysis of CO oxidation using Pt1/FeOx journal July 2011
Multiple-scattering calculations of x-ray-absorption spectra journal July 1995
Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles journal April 2018
Unusual infrared-absorption mechanism in thermally reduced graphene oxide journal September 2010
The Role of Intercalated Water in Multilayered Graphene Oxide journal October 2010
Avogadro: an advanced semantic chemical editor, visualization, and analysis platform journal August 2012
High-rate capacitive performance of graphene aerogel with a superhigh C/O molar ratio journal January 2012
Self-Standing Reduced Graphene Oxide Papers Electrodeposited with Manganese Oxide Nanostructures as Electrodes for Electrochemical Capacitors journal February 2019
Tuning the Selectivity of Single-Site Supported Metal Catalysts with Ionic Liquids journal September 2017
Graphene Aerogel Supported Pt Electrocatalysts for Oxygen Reduction Reaction by Supercritical Deposition journal October 2017
Effects of interionic interactions in 1,3-dialkylimidazolium ionic liquids on the electronic structure of metal sites in solid catalysts with ionic liquid layer (SCILL) journal April 2016

Cited By (2)

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Figures / Tables (9)