skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Controlling catalytic activity and selectivity for partial hydrogenation by tuning the environment around active sites in iridium complexes bonded to supports

Abstract

Enveloping atomically dispersed supported iridium with the choice of ionic liquid molecular sheaths and supports controls the catalytic performance.

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [3];  [3]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Koc Univ., Istanbul (Turkey)
  2. Univ. of California, Davis, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1491267
Alternate Identifier(s):
OSTI ID: 1505424
Grant/Contract Number:  
AC02-76SF00515; FG02-04ER15513; 113M552; Consortium for Operando and Advanced Catalyst Characterization
Resource Type:
Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Volume: 10; Journal Issue: 9; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Babucci, Melike, Fang, Chia -Yu, Perez-Aguilar, Jorge E., Hoffman, Adam S., Boubnov, Alexey, Guan, Erjia, Bare, Simon R., Gates, Bruce C., and Uzun, Alper. Controlling catalytic activity and selectivity for partial hydrogenation by tuning the environment around active sites in iridium complexes bonded to supports. United States: N. p., 2019. Web. doi:10.1039/c8sc05287e.
Babucci, Melike, Fang, Chia -Yu, Perez-Aguilar, Jorge E., Hoffman, Adam S., Boubnov, Alexey, Guan, Erjia, Bare, Simon R., Gates, Bruce C., & Uzun, Alper. Controlling catalytic activity and selectivity for partial hydrogenation by tuning the environment around active sites in iridium complexes bonded to supports. United States. doi:10.1039/c8sc05287e.
Babucci, Melike, Fang, Chia -Yu, Perez-Aguilar, Jorge E., Hoffman, Adam S., Boubnov, Alexey, Guan, Erjia, Bare, Simon R., Gates, Bruce C., and Uzun, Alper. Wed . "Controlling catalytic activity and selectivity for partial hydrogenation by tuning the environment around active sites in iridium complexes bonded to supports". United States. doi:10.1039/c8sc05287e.
@article{osti_1491267,
title = {Controlling catalytic activity and selectivity for partial hydrogenation by tuning the environment around active sites in iridium complexes bonded to supports},
author = {Babucci, Melike and Fang, Chia -Yu and Perez-Aguilar, Jorge E. and Hoffman, Adam S. and Boubnov, Alexey and Guan, Erjia and Bare, Simon R. and Gates, Bruce C. and Uzun, Alper},
abstractNote = {Enveloping atomically dispersed supported iridium with the choice of ionic liquid molecular sheaths and supports controls the catalytic performance.},
doi = {10.1039/c8sc05287e},
journal = {Chemical Science},
number = 9,
volume = 10,
place = {United States},
year = {2019},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1039/c8sc05287e

Citation Metrics:
Cited by: 5 works
Citation information provided by
Web of Science

Figures / Tables:

Table 1 Table 1: Summary of EXAFS fit parameters characterizing samples prepared by adsorption of Ir(CO)2(acac) on metal oxides having various electron-donor characteristics (quantified by the their corresponding PZC values)a

Save / Share:

Works referenced in this record:

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005


Isolated Metal Active Site Concentration and Stability Control Catalytic CO 2 Reduction Selectivity
journal, February 2015

  • Matsubu, John C.; Yang, Vanessa N.; Christopher, Phillip
  • Journal of the American Chemical Society, Vol. 137, Issue 8
  • DOI: 10.1021/ja5128133

Homogeneity of Surface Sites in Supported Single-Site Metal Catalysts: Assessment with Band Widths of Metal Carbonyl Infrared Spectra
journal, September 2016

  • Hoffman, Adam S.; Fang, Chia-Yu; Gates, Bruce C.
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 19
  • DOI: 10.1021/acs.jpclett.6b01825

Catalysis by Supported Single Metal Atoms
journal, November 2016


Nature of the metal-support interface in supported metal catalysts: Results from X-ray absorption spectroscopy
journal, January 1992

  • Koningsberger, D. C.; Gates, B. C.
  • Catalysis Letters, Vol. 14, Issue 3-4
  • DOI: 10.1007/BF00769664

Tuning selectivity in catalysis by controlling particle shape
journal, January 2009

  • Lee, Ilkeun; Delbecq, Françoise; Morales, Ricardo
  • Nature Materials, Vol. 8, Issue 2
  • DOI: 10.1038/nmat2371

Particle Size Effects in the Catalytic Electroreduction of CO 2 on Cu Nanoparticles
journal, May 2014

  • Reske, Rulle; Mistry, Hemma; Behafarid, Farzad
  • Journal of the American Chemical Society, Vol. 136, Issue 19
  • DOI: 10.1021/ja500328k

Synthesis of a molecularly defined single-active site heterogeneous catalyst for selective oxidation of N-heterocycles
journal, April 2018


Selective hydrogenation of 1,3-butadiene on platinum–copper alloys at the single-atom limit
journal, October 2015

  • Lucci, Felicia R.; Liu, Jilei; Marcinkowski, Matthew D.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9550

Gold Atoms Stabilized on Various Supports Catalyze the Water–Gas Shift Reaction
journal, November 2013

  • Flytzani-Stephanopoulos, Maria
  • Accounts of Chemical Research, Vol. 47, Issue 3
  • DOI: 10.1021/ar4001845

Size-dependent catalytic activity of supported metal clusters
journal, November 1994

  • Xu, Z.; Xiao, F. -S.; Purnell, S. K.
  • Nature, Vol. 372, Issue 6504
  • DOI: 10.1038/372346a0

Thermally stable single atom Pt/m-Al2O3 for selective hydrogenation and CO oxidation
journal, July 2017

  • Zhang, Zailei; Zhu, Yihan; Asakura, Hiroyuki
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms16100

Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis
journal, April 2013

  • Yang, Xiao-Feng; Wang, Aiqin; Qiao, Botao
  • Accounts of Chemical Research, Vol. 46, Issue 8
  • DOI: 10.1021/ar300361m

Electronic Metal-Support Interactions in Single-Atom Catalysts
journal, March 2014

  • Hu, Pingping; Huang, Zhiwei; Amghouz, Zakariae
  • Angewandte Chemie International Edition, Vol. 53, Issue 13
  • DOI: 10.1002/anie.201309248

Tuning Catalytic Selectivity: Zeolite- and Magnesium Oxide-Supported Molecular Rhodium Catalysts for Hydrogenation of 1,3-Butadiene
journal, September 2012

  • Yardimci, Dicle; Serna, Pedro; Gates, Bruce C.
  • ACS Catalysis, Vol. 2, Issue 10
  • DOI: 10.1021/cs300475c

Single-atom catalysis of CO oxidation using Pt1/FeOx
journal, July 2011

  • Qiao, Botao; Wang, Aiqin; Yang, Xiaofeng
  • Nature Chemistry, Vol. 3, Issue 8
  • DOI: 10.1038/nchem.1095

Single-Site Zeolite-Anchored Organoiridium Carbonyl Complexes: Characterization of Structure and Reactivity by Spectroscopy and Computational Chemistry
journal, July 2015

  • Martinez-Macias, Claudia; Chen, Mingyang; Dixon, David A.
  • Chemistry - A European Journal, Vol. 21, Issue 33
  • DOI: 10.1002/chem.201501277

Crystal structure of (acetylacetonato) (dicarbonyl)iridium(I)
journal, June 2009

  • Zherikova, K. V.; Kuratieva, N. V.; Morozova, N. B.
  • Journal of Structural Chemistry, Vol. 50, Issue 3
  • DOI: 10.1007/s10947-009-0088-x

Selective Hydrogenation of 1,3-Butadiene to 1-Butene by Pd(0) Nanoparticles Embedded in Imidazolium Ionic Liquids
journal, August 2005

  • Umpierre, Alexandre P.; Machado, Giovanna; Fecher, Gerhard H.
  • Advanced Synthesis & Catalysis, Vol. 347, Issue 10
  • DOI: 10.1002/adsc.200404313

Two- and Three-Dimensional [IrSi] Networks in the Silicides Sm3Ir2Si2, HoIrSi, and YbIrSi
journal, August 2001


Low-temperature carbon monoxide oxidation catalysed by regenerable atomically dispersed palladium on alumina
journal, September 2014

  • Peterson, Eric J.; DeLaRiva, Andrew T.; Lin, Sen
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5885

Tuning the Selectivity of Single-Site Supported Metal Catalysts with Ionic Liquids
journal, September 2017


Ligand Effects in SCILL Model Systems: Site-Specific Interactions with Pt and Pd Nanoparticles
journal, April 2011

  • Sobota, Marek; Happel, Markus; Amende, Max
  • Advanced Materials, Vol. 23, Issue 22-23
  • DOI: 10.1002/adma.201004064

Isostructural Zeolite-Supported Rhodium and Iridium Complexes: Tuning Catalytic Activity and Selectivity by Ligand Modification
journal, August 2015


Control of Metal Nanocrystal Size Reveals Metal-Support Interface Role for Ceria Catalysts
journal, July 2013


An atomic-scale view of single-site Pt catalysis for low-temperature CO oxidation
journal, March 2018

  • Therrien, Andrew J.; Hensley, Alyssa J. R.; Marcinkowski, Matthew D.
  • Nature Catalysis, Vol. 1, Issue 3
  • DOI: 10.1038/s41929-018-0028-2

Evidence for antisite disorder in YBa2Cu3O7
journal, June 1989


Bridging homogeneous and heterogeneous catalysis by heterogeneous single-metal-site catalysts
journal, June 2018


Solid Catalyst with Ionic Liquid Layer (SCILL) – A New Concept to Improve Selectivity Illustrated by Hydrogenation of Cyclooctadiene
journal, August 2007

  • Kernchen, U.; Etzold, B.; Korth, W.
  • Chemical Engineering & Technology, Vol. 30, Issue 8
  • DOI: 10.1002/ceat.200700050

Interaction trends between single metal atoms and oxide supports identified with density functional theory and statistical learning
journal, July 2018

  • O’Connor, Nolan J.; Jonayat, A. S. M.; Janik, Michael J.
  • Nature Catalysis, Vol. 1, Issue 7
  • DOI: 10.1038/s41929-018-0094-5

Effects of Cu–Ni Bimetallic Catalyst Composition and Support on Activity, Selectivity, and Stability for Furfural Conversion to 2-Methyfuran
journal, December 2017

  • Seemala, Bhogeswararao; Cai, Charles M.; Kumar, Rajeev
  • ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 2
  • DOI: 10.1021/acssuschemeng.7b03572

Isolated Metal Atom Geometries as a Strategy for Selective Heterogeneous Hydrogenations
journal, March 2012

  • Kyriakou, Georgios; Boucher, Matthew B.; Jewell, April D.
  • Science, Vol. 335, Issue 6073
  • DOI: 10.1126/science.1215864

Tuning the Catalytic Activity and Selectivity of Pd Nanoparticles Using Ligand-Modified Supports and Surfaces
journal, September 2017

  • da Silva, Fernanda Parra; Fiorio, Jhonatan Luiz; Rossi, Liane Marcia
  • ACS Omega, Vol. 2, Issue 9
  • DOI: 10.1021/acsomega.7b00836

A new method for parameterization of phase shift and backscattering amplitude
journal, March 1995

  • Vaarkamp, Marius; Linders, Johannes C.; Koningsberger, Diek C.
  • Physica B: Condensed Matter, Vol. 208-209
  • DOI: 10.1016/0921-4526(94)00658-I

Isoelectric points and points of zero charge of metal (hydr)oxides: 50years after Parks' review
journal, December 2016


Electronic perturbations
journal, July 2012


Supported Molecular Iridium Catalysts: Resolving Effects of Metal Nuclearity and Supports as Ligands
journal, October 2011

  • Lu, Jing; Serna, Pedro; Aydin, Ceren
  • Journal of the American Chemical Society, Vol. 133, Issue 40
  • DOI: 10.1021/ja206486j

Interactions Between the Room-Temperature Ionic Liquid [C 2 C 1 Im][OTf] and Pd(111), Well-Ordered Al 2 O 3 , and Supported Pd Model Catalysts from IR Spectroscopy
journal, January 2014

  • Schernich, Stefan; Kostyshyn, Dmytro; Wagner, Valentin
  • The Journal of Physical Chemistry C, Vol. 118, Issue 6
  • DOI: 10.1021/jp5006692

Interactions of [BMIM][BF 4 ] with Metal Oxides and Their Consequences on Stability Limits
journal, September 2016

  • Babucci, Melike; Balci, Volkan; Akçay, Aslı
  • The Journal of Physical Chemistry C, Vol. 120, Issue 36
  • DOI: 10.1021/acs.jpcc.6b03975

A New Type of Strong Metal–Support Interaction and the Production of H 2 through the Transformation of Water on Pt/CeO 2 (111) and Pt/CeO x /TiO 2 (110) Catalysts
journal, May 2012

  • Bruix, Albert; Rodriguez, José A.; Ramírez, Pedro J.
  • Journal of the American Chemical Society, Vol. 134, Issue 21
  • DOI: 10.1021/ja302070k

Well-Defined Noble Metal Single Sites in Zeolites as an Alternative to Catalysis by Insoluble Metal Salts
journal, September 2015

  • Rubio-Marqués, Paula; Rivero-Crespo, Miguel A.; Leyva-Pérez, Antonio
  • Journal of the American Chemical Society, Vol. 137, Issue 36
  • DOI: 10.1021/jacs.5b07304

Single-Atom Pd 1 /Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene
journal, August 2015

  • Yan, Huan; Cheng, Hao; Yi, Hong
  • Journal of the American Chemical Society, Vol. 137, Issue 33
  • DOI: 10.1021/jacs.5b06485

Interfacial electronic effects control the reaction selectivity of platinum catalysts
journal, January 2016

  • Chen, Guangxu; Xu, Chaofa; Huang, Xiaoqing
  • Nature Materials, Vol. 15, Issue 5
  • DOI: 10.1038/nmat4555

Transmission and fluorescence X-ray absorption spectroscopy cell/flow reactor for powder samples under vacuum or in reactive atmospheres
journal, July 2016

  • Hoffman, A. S.; Debefve, L. M.; Bendjeriou-Sedjerari, A.
  • Review of Scientific Instruments, Vol. 87, Issue 7
  • DOI: 10.1063/1.4958824

Surface Science and Model Catalysis with Ionic Liquid-Modified Materials
journal, April 2011

  • Steinrück, H. -P.; Libuda, J.; Wasserscheid, P.
  • Advanced Materials, Vol. 23, Issue 22-23
  • DOI: 10.1002/adma.201100211

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


Remarkable Performance of Ir 1 /FeO x Single-Atom Catalyst in Water Gas Shift Reaction
journal, October 2013

  • Lin, Jian; Wang, Aiqin; Qiao, Botao
  • Journal of the American Chemical Society, Vol. 135, Issue 41
  • DOI: 10.1021/ja408574m

Dynamic Structural Changes in a Molecular Zeolite-Supported Iridium Catalyst for Ethene Hydrogenation
journal, November 2009

  • Uzun, Alper; Gates, Bruce C.
  • Journal of the American Chemical Society, Vol. 131, Issue 43
  • DOI: 10.1021/ja906553n

Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C–H activation
journal, January 2018

  • Marcinkowski, Matthew D.; Darby, Matthew T.; Liu, Jilei
  • Nature Chemistry, Vol. 10, Issue 3
  • DOI: 10.1038/nchem.2915

Reactive surface organometallic complexes observed using dynamic nuclear polarization surface enhanced NMR spectroscopy
journal, January 2017

  • Pump, Eva; Viger-Gravel, Jasmine; Abou-Hamad, Edy
  • Chemical Science, Vol. 8, Issue 1
  • DOI: 10.1039/C6SC02379G

The Multifaceted Reactivity of Single-Atom Heterogeneous Catalysts
journal, October 2018

  • Mitchell, Sharon; Vorobyeva, Evgeniya; Pérez-Ramírez, Javier
  • Angewandte Chemie International Edition, Vol. 57, Issue 47
  • DOI: 10.1002/anie.201806936

Mild oxidation of methane to methanol or acetic acid on supported isolated rhodium catalysts
journal, November 2017

  • Shan, Junjun; Li, Mengwei; Allard, Lawrence F.
  • Nature, Vol. 551, Issue 7682
  • DOI: 10.1038/nature24640

Surface organometallic chemistry in heterogeneous catalysis
journal, January 2018

  • Samantaray, Manoja K.; Pump, Eva; Bendjeriou-Sedjerari, Anissa
  • Chemical Society Reviews, Vol. 47, Issue 22
  • DOI: 10.1039/C8CS00356D

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.