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Title: Catalytically active Au-O(OH)x- species stabilized by alkali ions on zeolites and mesoporous oxides

Abstract

Here we report that the addition of alkali ions (sodium or potassium) to gold on KLTL-zeolite and mesoporous MCM-41 silica stabilizes mononuclear gold in Au-O(OH)x-(Na or K) ensembles. This single-site gold species is active for the low-temperature (<200°C) water-gas shift (WGS) reaction. Unexpectedly, gold is thus similar to platinum in creating –O linkages with more than eight alkali ions and establishing an active site on various supports. The intrinsic activity of the single-site gold species is the same on irreducible supports as on reducible ceria, iron oxide, and titania supports, apparently all sharing a common, similarly structured gold active site. This finding paves the way for using earth-abundant supports to disperse and stabilize precious metal atoms with alkali additives for the WGS and potentially other fuel-processing reactions.

Authors:
 [1];  [2];  [1];  [2];  [3];  [4];  [5];  [6];  [2];  [1]
+ Show Author Affiliations
  1. Tufts Univ., Medford, MA (United States). Dept. of Chemical and Biological Engineering
  2. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering
  3. Louisiana State Univ., Baton Rouge, LA (United States). Dept. of Chemical Engineering
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  5. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  6. Univ. of Sydney, NSW (Australia). School of Chemical and Biomolecular Engineering
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Contributing Org.:
EMSL; the Center for Nanoscale Materials at Argonne National Laboratory (ANL); the CNMS at ORNL; and the National Energy Research Scientific Computing Center (NERSC)
OSTI Identifier:
1398777
Grant/Contract Number:  
FG02-05ER15731; FG02-05ER15730; AC02-06CH11357; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 346; Journal Issue: 6216; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Yang, Ming, Li, Sha, Wang, Yuan, Herron, Jeffrey A., Xu, Ye, Allard, Lawrence F., Lee, Sungsik, Huang, Jun, Mavrikakis, Manos, and Flytzani-Stephanopoulos, Maria. Catalytically active Au-O(OH)x- species stabilized by alkali ions on zeolites and mesoporous oxides. United States: N. p., 2014. Web. doi:10.1126/science.1260526.
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Yang, Ming, Li, Sha, Wang, Yuan, Herron, Jeffrey A., Xu, Ye, Allard, Lawrence F., Lee, Sungsik, Huang, Jun, Mavrikakis, Manos, & Flytzani-Stephanopoulos, Maria. Catalytically active Au-O(OH)x- species stabilized by alkali ions on zeolites and mesoporous oxides. United States. https://doi.org/10.1126/science.1260526
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Yang, Ming, Li, Sha, Wang, Yuan, Herron, Jeffrey A., Xu, Ye, Allard, Lawrence F., Lee, Sungsik, Huang, Jun, Mavrikakis, Manos, and Flytzani-Stephanopoulos, Maria. Thu . "Catalytically active Au-O(OH)x- species stabilized by alkali ions on zeolites and mesoporous oxides". United States. https://doi.org/10.1126/science.1260526. https://www.osti.gov/servlets/purl/1398777.
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@article{osti_1398777,
title = {Catalytically active Au-O(OH)x- species stabilized by alkali ions on zeolites and mesoporous oxides},
author = {Yang, Ming and Li, Sha and Wang, Yuan and Herron, Jeffrey A. and Xu, Ye and Allard, Lawrence F. and Lee, Sungsik and Huang, Jun and Mavrikakis, Manos and Flytzani-Stephanopoulos, Maria},
abstractNote = {Here we report that the addition of alkali ions (sodium or potassium) to gold on KLTL-zeolite and mesoporous MCM-41 silica stabilizes mononuclear gold in Au-O(OH)x-(Na or K) ensembles. This single-site gold species is active for the low-temperature (<200°C) water-gas shift (WGS) reaction. Unexpectedly, gold is thus similar to platinum in creating –O linkages with more than eight alkali ions and establishing an active site on various supports. The intrinsic activity of the single-site gold species is the same on irreducible supports as on reducible ceria, iron oxide, and titania supports, apparently all sharing a common, similarly structured gold active site. This finding paves the way for using earth-abundant supports to disperse and stabilize precious metal atoms with alkali additives for the WGS and potentially other fuel-processing reactions.},
doi = {10.1126/science.1260526},
journal = {Science},
number = 6216,
volume = 346,
place = {United States},
year = {Thu Nov 27 00:00:00 EST 2014},
month = {Thu Nov 27 00:00:00 EST 2014}
}
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https://doi.org/10.1126/science.1260526
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    Synergetic interaction between neighboring platinum and ruthenium monomers boosts CO oxidation
    journal, January 2019

    • Zhou, Peng; Hou, Xingang; Chao, Yuguang
    • Chemical Science, Vol. 10, Issue 23
    • DOI: 10.1039/c9sc00658c

    Strong electrostatic adsorption of Pt onto SiO 2 partially overcoated Al 2 O 3 —Towards single atom catalysts
    journal, December 2019

    • Bo, Zhenyu; McCullough, Lauren R.; Dull, Samuel
    • The Journal of Chemical Physics, Vol. 151, Issue 21
    • DOI: 10.1063/1.5128934

    A sulfur-tethering synthesis strategy toward high-loading atomically dispersed noble metal catalysts
    journal, October 2019

    Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts
    journal, September 2015

    Photochemical route for synthesizing atomically dispersed palladium catalysts
    journal, May 2016

    Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction
    journal, June 2017

    Effect of Nickel Oxide Doping to Ceria-Supported Gold Catalyst for CO Oxidation and Water-Gas Shift Reactions
    journal, November 2018

    Acetylene in Organic Synthesis: Recent Progress and New Uses
    journal, September 2018

    • Voronin, Vladimir V.; Ledovskaya, Maria S.; Bogachenkov, Alexander S.
    • Molecules, Vol. 23, Issue 10
    • DOI: 10.3390/molecules23102442

    Single-Atom Pt as Co-Catalyst for Enhanced Photocatalytic H 2 Evolution
    journal, January 2016

    Low‐Temperature Conversion of Alcohols into Bulky Nanoporous Graphene and Pure Hydrogen with Robust Selectivity on CaO
    journal, February 2019

    • Han, Gao‐Feng; Chen, Zhi‐Wen; Jeon, Jong‐Pil
    • Advanced Materials, Vol. 31, Issue 16
    • DOI: 10.1002/adma.201807267

    Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis
    journal, July 2019

    • Li, Xuning; Yang, Xiaofeng; Huang, Yanqiang
    • Advanced Materials, Vol. 31, Issue 50
    • DOI: 10.1002/adma.201902031

    Single-Site Active Cobalt-Based Photocatalyst with a Long Carrier Lifetime for Spontaneous Overall Water Splitting
    journal, June 2017

    Isolated Platinum Atoms Stabilized by Amorphous Tungstenic Acid: Metal-Support Interaction for Synergistic Oxygen Activation
    journal, June 2018

    • Zhang, Qian; Qin, Xi-Xi; Duan-Mu, Fan-Peng
    • Angewandte Chemie, Vol. 130, Issue 30
    • DOI: 10.1002/ange.201804319

    Atomically Precise Multimetallic Semiconductive Nanoclusters with Optical Limiting Effects
    journal, May 2018

    Design of Single Gold Atoms on Nitrogen-Doped Carbon for Molecular Recognition in Alkyne Semi-Hydrogenation
    journal, November 2018

    Die facettenreiche Reaktivität heterogener Einzelatom‐Katalysatoren
    journal, November 2018

    • Mitchell, Sharon; Vorobyeva, Evgeniya; Pérez‐Ramírez, Javier
    • Angewandte Chemie, Vol. 130, Issue 47
    • DOI: 10.1002/ange.201806936

    Stabilizing a Platinum 1 Single-Atom Catalyst on Supported Phosphomolybdic Acid without Compromising Hydrogenation Activity
    journal, May 2016

    • Zhang, Bin; Asakura, Hiroyuki; Zhang, Jia
    • Angewandte Chemie International Edition, Vol. 55, Issue 29
    • DOI: 10.1002/anie.201602801

    The Role of Supported Atomically Distributed Metal Species in Electrochemistry and How to Create Them
    journal, May 2019

    • Ding, Yuxiao; Schlögl, Robert; Heumann, Saskia
    • ChemElectroChem, Vol. 6, Issue 15
    • DOI: 10.1002/celc.201900598

    Hydride Transfer to Gold: Yes or No? Exploring the Unexpected Versatility of Au⋅⋅⋅H−M Bonding in Heterobimetallic Dihydrides
    journal, June 2020

    • Rocchigiani, Luca; Klooster, Wim T.; Coles, Simon J.
    • Chemistry – A European Journal, Vol. 26, Issue 37
    • DOI: 10.1002/chem.202000016

    Atomically isolated nickel species anchored on graphitized carbon for efficient hydrogen evolution electrocatalysis
    journal, February 2016

    • Fan, Lili; Liu, Peng Fei; Yan, Xuecheng
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms10667

    Contributions of distinct gold species to catalytic reactivity for carbon monoxide oxidation
    journal, November 2016

    • Guo, Li-Wen; Du, Pei-Pei; Fu, Xin-Pu
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms13481

    Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst
    journal, December 2016

    • Wang, Liangbing; Zhang, Wenbo; Wang, Shenpeng
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms14036

    High performance platinum single atom electrocatalyst for oxygen reduction reaction
    journal, July 2017

    • Liu, Jing; Jiao, Menggai; Lu, Lanlu
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms15938

    Enhanced oxygen reduction with single-atomic-site iron catalysts for a zinc-air battery and hydrogen-air fuel cell
    journal, December 2018

    Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen
    journal, March 2019

    • Pereira-Hernández, Xavier Isidro; DeLaRiva, Andrew; Muravev, Valery
    • Nature Communications, Vol. 10, Issue 1
    • DOI: 10.1038/s41467-019-09308-5

    Unraveling the coordination structure-performance relationship in Pt1/Fe2O3 single-atom catalyst
    journal, October 2019

    Boosting the catalysis of gold by O2 activation at Au-SiO2 interface
    journal, January 2020

    Identification of the active complex for CO oxidation over single-atom Ir-on-MgAl2O4 catalysts
    journal, December 2018

    Single platinum atoms immobilized on an MXene as an efficient catalyst for the hydrogen evolution reaction
    journal, December 2018

    Towards ALD thin film stabilized single-atom Pd 1 catalysts
    journal, January 2016

    • Piernavieja-Hermida, Mar; Lu, Zheng; White, Anderson
    • Nanoscale, Vol. 8, Issue 33
    • DOI: 10.1039/c6nr04403d

    Towards highly active Pd/CeO 2 for alkene hydrogenation by tuning Pd dispersion and surface properties of the catalysts
    journal, January 2017

    Porous liquid zeolites: hydrogen bonding-stabilized H-ZSM-5 in branched ionic liquids
    journal, January 2019

    • Li, Peipei; Chen, Hao; Schott, Jennifer A.
    • Nanoscale, Vol. 11, Issue 4
    • DOI: 10.1039/c8nr07337f

    Insights into interface engineering in steam reforming reactions for hydrogen production
    journal, January 2019

    • Chen, Sai; Pei, Chunlei; Gong, Jinlong
    • Energy & Environmental Science, Vol. 12, Issue 12
    • DOI: 10.1039/c9ee02808k

    Hydroxyl group modification improves the electrocatalytic ORR and OER activity of graphene supported single and bi-metal atomic catalysts (Ni, Co, and Fe)
    journal, January 2019

    • Zhao, Xiaomei; Liu, Xia; Huang, Baoyu
    • Journal of Materials Chemistry A, Vol. 7, Issue 42
    • DOI: 10.1039/c9ta08661g

    Recent advances in the precise control of isolated single-site catalysts by chemical methods
    journal, June 2018

    • Li, Zhijun; Wang, Dehua; Wu, Yuen
    • National Science Review, Vol. 5, Issue 5
    • DOI: 10.1093/nsr/nwy056

    Single-atom catalyst: a rising star for green synthesis of fine chemicals
    journal, August 2018

    • Zhang, Leilei; Ren, Yujing; Liu, Wengang
    • National Science Review, Vol. 5, Issue 5
    • DOI: 10.1093/nsr/nwy077

    Gold(III)-CO and gold(III)-CO 2 complexes and their role in the water-gas shift reaction
    journal, October 2015

    • Roşca, Dragoş-Adrian; Fernandez-Cestau, Julio; Morris, James
    • Science Advances, Vol. 1, Issue 9
    • DOI: 10.1126/sciadv.1500761

    A pyrolysis-free path toward superiorly catalytic nitrogen-coordinated single atom
    journal, August 2019

    New Strategies for the Preparation of Sinter‐Resistant Metal‐Nanoparticle‐Based Catalysts
    journal, July 2019

    • Wang, Lingxiang; Wang, Liang; Meng, Xiangju
    • Advanced Materials, Vol. 31, Issue 50
    • DOI: 10.1002/adma.201901905

    Static Regulation and Dynamic Evolution of Single‐Atom Catalysts in Thermal Catalytic Reactions
    journal, November 2018

    Stabilizing a Platinum 1 Single-Atom Catalyst on Supported Phosphomolybdic Acid without Compromising Hydrogenation Activity
    journal, May 2016

    Cyclometalated Gold(III) Complexes: Synthesis, Reactivity, and Physicochemical Properties
    journal, January 2017

    • Kumar, Roopender; Nevado, Cristina
    • Angewandte Chemie International Edition, Vol. 56, Issue 8
    • DOI: 10.1002/anie.201607225

    Promoting Effect and Mechanism of Alkali Na on Pd/SBA‐15 for Room Temperature Formaldehyde Catalytic Oxidation
    journal, September 2019

    Atomic palladium on graphitic carbon nitride as a hydrogen evolution catalyst under visible light irradiation
    journal, February 2019

    Towards stable single-atom catalysts: strong binding of atomically dispersed transition metals on the surface of nanostructured ceria
    journal, January 2016

    • Figueroba, Alberto; Kovács, Gábor; Bruix, Albert
    • Catalysis Science & Technology, Vol. 6, Issue 18
    • DOI: 10.1039/c6cy00294c

    Direct formation of Au( iii ) acetyl, alkoxyl and alkynyl functionalities via halide free tricationic Au( iii ) precursors
    journal, January 2018

    • Corbo, Robert; Albayer, Mohammad; Hall, Neville B.
    • Dalton Transactions, Vol. 47, Issue 12
    • DOI: 10.1039/c7dt04675h

    Facile one-pot synthesis of MOF supported gold pseudo-single-atom catalysts for hydrogenation reactions
    journal, January 2018

    • Wang, Zumin; Gu, Lin; Song, Li
    • Materials Chemistry Frontiers, Vol. 2, Issue 5
    • DOI: 10.1039/c8qm00081f

    Alkali-driven active site shift of fast SCR with NH 3 on V 2 O 5 –WO 3 /TiO 2 catalyst via a novel Eley–Rideal mechanism
    journal, January 2019

    • Xiang, Jinyao; Du, Xuesen; Wan, Yuyi
    • Catalysis Science & Technology, Vol. 9, Issue 21
    • DOI: 10.1039/c9cy01565e

    Dynamic multinuclear sites formed by mobilized copper ions in NO x selective catalytic reduction
    journal, August 2017

    • Paolucci, Christopher; Khurana, Ishant; Parekh, Atish A.
    • Science, Vol. 357, Issue 6354
    • DOI: 10.1126/science.aan5630

    Recover the activity of sintered supported catalysts by nitrogen-doped carbon atomization
    journal, January 2020

    Recent Advances in the Gold-Catalysed Low-Temperature Water–Gas Shift Reaction
    journal, December 2018

    Design of Single Gold Atoms on Nitrogen-Doped Carbon for Molecular Recognition in Alkyne Semi-Hydrogenation
    journal, November 2018

    • Lin, Ronghe; Albani, Davide; Fako, Edvin
    • Angewandte Chemie International Edition, Vol. 58, Issue 2
    • DOI: 10.1002/anie.201805820

    The Multifaceted Reactivity of Single-Atom Heterogeneous Catalysts
    text, January 2018

    Static Regulation and Dynamic Evolution of Single‐Atom Catalysts in Thermal Catalytic Reactions
    journal, November 2018

    Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles
    journal, April 2018

    Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst
    journal, March 2016

    • Choi, Chang Hyuck; Kim, Minho; Kwon, Han Chang
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms10922

    Contributions of distinct gold species to catalytic reactivity for carbon monoxide oxidation
    journal, November 2016

    • Guo, Li-Wen; Du, Pei-Pei; Fu, Xin-Pu
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms13481

    Platinum single-atom and cluster catalysis of the hydrogen evolution reaction
    journal, November 2016

    • Cheng, Niancai; Stambula, Samantha; Wang, Da
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms13638

    Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst
    journal, December 2016

    • Wang, Liangbing; Zhang, Wenbo; Wang, Shenpeng
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms14036

    High performance platinum single atom electrocatalyst for oxygen reduction reaction
    journal, July 2017

    • Liu, Jing; Jiao, Menggai; Lu, Lanlu
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms15938

    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

    Atomic engineering of high-density isolated Co atoms on graphene with proximal-atom controlled reaction selectivity
    journal, August 2018

    Breaking the scaling relationship via thermally stable Pt/Cu single atom alloys for catalytic dehydrogenation
    journal, October 2018

    Enhanced oxygen reduction with single-atomic-site iron catalysts for a zinc-air battery and hydrogen-air fuel cell
    journal, December 2018

    Construction of stabilized bulk-nano interfaces for highly promoted inverse CeO2/Cu catalyst
    journal, August 2019

    Reversing the charge transfer between platinum and sulfur-doped carbon support for electrocatalytic hydrogen evolution
    journal, October 2019

    Titania supported synergistic palladium single atoms and nanoparticles for room temperature ketone and aldehydes hydrogenation
    journal, January 2020

    Heterolytic bond activation at gold: evidence for gold( iii ) H–B, H–Si complexes, H–H and H–C cleavage
    journal, January 2019

    • Rocchigiani, Luca; Budzelaar, Peter H. M.; Bochmann, Manfred
    • Chemical Science, Vol. 10, Issue 9
    • DOI: 10.1039/c8sc05229h

    A pyrolysis-free path toward superiorly catalytic nitrogen-coordinated single atom
    journal, August 2019

    A sulfur-tethering synthesis strategy toward high-loading atomically dispersed noble metal catalysts
    journal, October 2019

    The Success Story of Gold-Based Catalysts for Gas- and Liquid-Phase Reactions: A Brief Perspective and Beyond
    journal, October 2019

    • Price, Cameron A. H.; Pastor-Pérez, Laura; Ivanova, Svetlana
    • Frontiers in Chemistry, Vol. 7
    • DOI: 10.3389/fchem.2019.00691

    On the High Sensitivity of the Electronic States of 1 nm Gold Particles to Pretreatments and Modifiers
    journal, March 2016

    Acetylene in Organic Synthesis: Recent Progress and New Uses
    journal, September 2018

    • Voronin, Vladimir V.; Ledovskaya, Maria S.; Bogachenkov, Alexander S.
    • Molecules, Vol. 23, Issue 10
    • DOI: 10.3390/molecules23102442
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