Towards ALD thin film stabilized single-atom Pd 1 catalysts
Abstract
Supported precious metal single-atom catalysts have shown interesting activity and selectivity in recent studies. However, agglomeration of these highly mobile mononuclear surface species can eliminate their unique catalytic properties. Here we study a strategy for synthesizing thin film stabilized single-atom Pd1 catalysts using atomic layer deposition (ALD). The thermal stability of the Pd1 catalysts is significantly enhanced by creating a nanocavity thin film structure. In situ infrared spectroscopy and Pd K-edge X-ray absorption spectroscopy (XAS) revealed that the Pd1 was anchored on the surface through chlorine sites. The thin film stabilized Pd1 catalysts were thermally stable under both oxidation and reduction conditions. The catalytic performance in the methanol decomposition reaction is found to depend on the thickness of protecting layers. While Pd1 catalysts showed promising activity at low temperature in a methanol decomposition reaction, 14 cycle TiO2 protected Pd1 was less active at high temperature. Pd L3 edge XAS indicated that the low reactivity compared with Pd nanoparticles is due to the strong adsorption of carbon monoxide even at 250 °C. Furthermore, these results clearly show that the ALD nanocavities provide a basis for future design of single-atom catalysts that are highly efficient and stable.
- Authors:
-
- Univ. of Alabama in Huntsville, Huntsville, AL (United States). Dept. of Chemical and Materials Engineering
- Univ. of Illinois, Chicago, IL (United States). Research Resources Center
- Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
- Argonne National Lab. (ANL), Argonne, IL (United States). Energy Systems Division
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); ORAU; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22) - National Science Foundation (NSF)
- OSTI Identifier:
- 1319206
- Alternate Identifier(s):
- OSTI ID: 1337161
- Grant/Contract Number:
- AC05-00OR22725; CBET-1511820; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nanoscale
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 33; Journal ID: ISSN 2040-3364
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY
Citation Formats
Piernavieja-Hermida, Mar, Lu, Zheng, White, Anderson, Low, Ke-Bin, Wu, Tianpin, Elam, Jeffrey W., Wu, Zili, and Lei, Yu. Towards ALD thin film stabilized single-atom Pd 1 catalysts. United States: N. p., 2016.
Web. doi:10.1039/c6nr04403d.
Piernavieja-Hermida, Mar, Lu, Zheng, White, Anderson, Low, Ke-Bin, Wu, Tianpin, Elam, Jeffrey W., Wu, Zili, & Lei, Yu. Towards ALD thin film stabilized single-atom Pd 1 catalysts. United States. https://doi.org/10.1039/c6nr04403d
Piernavieja-Hermida, Mar, Lu, Zheng, White, Anderson, Low, Ke-Bin, Wu, Tianpin, Elam, Jeffrey W., Wu, Zili, and Lei, Yu. Wed .
"Towards ALD thin film stabilized single-atom Pd 1 catalysts". United States. https://doi.org/10.1039/c6nr04403d. https://www.osti.gov/servlets/purl/1319206.
@article{osti_1319206,
title = {Towards ALD thin film stabilized single-atom Pd 1 catalysts},
author = {Piernavieja-Hermida, Mar and Lu, Zheng and White, Anderson and Low, Ke-Bin and Wu, Tianpin and Elam, Jeffrey W. and Wu, Zili and Lei, Yu},
abstractNote = {Supported precious metal single-atom catalysts have shown interesting activity and selectivity in recent studies. However, agglomeration of these highly mobile mononuclear surface species can eliminate their unique catalytic properties. Here we study a strategy for synthesizing thin film stabilized single-atom Pd1 catalysts using atomic layer deposition (ALD). The thermal stability of the Pd1 catalysts is significantly enhanced by creating a nanocavity thin film structure. In situ infrared spectroscopy and Pd K-edge X-ray absorption spectroscopy (XAS) revealed that the Pd1 was anchored on the surface through chlorine sites. The thin film stabilized Pd1 catalysts were thermally stable under both oxidation and reduction conditions. The catalytic performance in the methanol decomposition reaction is found to depend on the thickness of protecting layers. While Pd1 catalysts showed promising activity at low temperature in a methanol decomposition reaction, 14 cycle TiO2 protected Pd1 was less active at high temperature. Pd L3 edge XAS indicated that the low reactivity compared with Pd nanoparticles is due to the strong adsorption of carbon monoxide even at 250 °C. Furthermore, these results clearly show that the ALD nanocavities provide a basis for future design of single-atom catalysts that are highly efficient and stable.},
doi = {10.1039/c6nr04403d},
journal = {Nanoscale},
number = 33,
volume = 8,
place = {United States},
year = {Wed Jul 27 00:00:00 EDT 2016},
month = {Wed Jul 27 00:00:00 EDT 2016}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 89 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Surface poisoning in the nucleation and growth of palladium atomic layer deposition with Pd(hfac)2 and formalin
journal, June 2011
- Goldstein, D. N.; George, S. M.
- Thin Solid Films, Vol. 519, Issue 16
Sub-10 nm Platinum Nanocrystals with Size and Shape Control: Catalytic Study for Ethylene and Pyrrole Hydrogenation
journal, April 2009
- Tsung, Chia-Kuang; Kuhn, John N.; Huang, Wenyu
- Journal of the American Chemical Society, Vol. 131, Issue 16
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
Acetylene Cyclotrimerization on Supported Size-Selected Pd n Clusters (1 ≤ n ≤ 30): One Atom Is Enough!
journal, April 2000
- Abbet, S.; Sanchez, A.; Heiz, U.
- Journal of the American Chemical Society, Vol. 122, Issue 14
CO Oxidation on Au n /TiO 2 Catalysts Produced by Size-Selected Cluster Deposition
journal, May 2004
- Lee, Sungsik; Fan, Chaoyang; Wu, Tianpin
- Journal of the American Chemical Society, Vol. 126, Issue 18
Direct propylene epoxidation over barium-promoted Au/Ti-TUD catalysts with H2 and O2: Effect of Au particle size
journal, September 2007
- Lu, J.; Zhang, X.; Bravosuarez, J.
- Journal of Catalysis, Vol. 250, Issue 2
Effects of Chlorine in Titanium Oxide on Palladium Atomic Layer Deposition
journal, September 2014
- Lei, Yu; Liu, Bin; Lu, Junling
- The Journal of Physical Chemistry C, Vol. 118, Issue 39
Role of Cluster Size in Catalysis: Spectroscopic Investigation of γ-Al 2 O 3 -Supported Ir 4 and Ir 6 during Ethene Hydrogenation
journal, June 2003
- Argo, Andrew M.; Odzak, Josip F.; Gates, Bruce C.
- Journal of the American Chemical Society, Vol. 125, Issue 23
Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects
journal, April 2010
- Lei, Y.; Mehmood, F.; Lee, S.
- Science, Vol. 328, Issue 5975, p. 224-228
In situ surface characterization of the intermetallic compound PdGa – A highly selective hydrogenation catalyst
journal, June 2009
- Kovnir, K.; Armbrüster, M.; Teschner, D.
- Surface Science, Vol. 603, Issue 10-12
Electronic Structure Controls Reactivity of Size-Selected Pd Clusters Adsorbed on TiO2 Surfaces
journal, November 2009
- Kaden, W. E.; Wu, T.; Kunkel, W. A.
- Science, Vol. 326, Issue 5954
CO Adsorption on Monometallic and Bimetallic Au−Pd Nanoparticles Supported on Oxide Thin Films
journal, July 2010
- Abbott, H. L.; Aumer, A.; Lei, Y.
- The Journal of Physical Chemistry C, Vol. 114, Issue 40
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
Catalysis and In Situ Studies of Rh 1 /Co 3 O 4 Nanorods in Reduction of NO with H 2
journal, April 2013
- Wang, Lei; Zhang, Shiran; Zhu, Yuan
- ACS Catalysis, Vol. 3, Issue 5
Fundamentals of Industrial Catalytic Processes
book, January 2005
- Bartholomew, Calvin H.; Farrauto, Robert J.
- John Wiley & Sons, Inc.
Effect of Particle Size and Adsorbates on the L3, L2 and L1 X-ray Absorption Near Edge Structure of Supported Pt Nanoparticles
journal, February 2011
- Lei, Yu; Jelic, Jelena; Nitsche, Ludwig C.
- Topics in Catalysis, Vol. 54, Issue 5-7
Catalytically active Au-O(OH) x - species stabilized by alkali ions on zeolites and mesoporous oxides
journal, November 2014
- Yang, Ming; Li, Sha; Wang, Yuan
- Science, Vol. 346, Issue 6216
Atomic layer deposition—Sequential self-limiting surface reactions for advanced catalyst “bottom-up” synthesis
journal, June 2016
- Lu, Junling; Elam, Jeffrey W.; Stair, Peter C.
- Surface Science Reports, Vol. 71, Issue 2
A View from the Inside: Complexity in the Atomic Scale Ordering of Supported Metal Nanoparticles
journal, December 2001
- Frenkel, Anatoly I.; Hills, Charles W.; Nuzzo, Ralph G.
- The Journal of Physical Chemistry B, Vol. 105, Issue 51
Reactivity and stability of Au in and on TS-1 for epoxidation of propylene with H2 and O2
journal, August 2004
- Yap, N.
- Journal of Catalysis, Vol. 226, Issue 1
Size- and support-dependency in the catalysis of gold
journal, April 1997
- Haruta, Masatake
- Catalysis Today, Vol. 36, Issue 1
Catalyst Design with Atomic Layer Deposition
journal, February 2015
- O’Neill, Brandon J.; Jackson, David H. K.; Lee, Jechan
- ACS Catalysis, Vol. 5, Issue 3
CO Oxidation Catalyzed by Supported Gold: Cooperation between Gold and Nanocrystalline Rare-Earth Supports Forms Reactive Surface Superoxide and Peroxide Species
journal, July 2005
- Guzman, Javier; Carrettin, Silvio; Fierro-Gonzalez, Juan C.
- Angewandte Chemie International Edition, Vol. 44, Issue 30
Intact Size-Selected Au n Clusters on a TiO 2 (110)-(1 × 1) Surface at Room Temperature
journal, October 2005
- Tong, Xiao; Benz, Lauren; Kemper, Paul
- Journal of the American Chemical Society, Vol. 127, Issue 39
Alumina Over-coating on Pd Nanoparticle Catalysts by Atomic Layer Deposition: Enhanced Stability and Reactivity
journal, January 2011
- Feng, Hao; Lu, Junling; Stair, Peter C.
- Catalysis Letters, Vol. 141, Issue 4
The Production of Propene Oxide: Catalytic Processes and Recent Developments
journal, May 2006
- Nijhuis, T. Alexander; Makkee, Michiel; Moulijn, Jacob A.
- Industrial & Engineering Chemistry Research, Vol. 45, Issue 10
Precisely Applying TiO 2 Overcoat on Supported Au Catalysts Using Atomic Layer Deposition for Understanding the Reaction Mechanism and Improved Activity in CO Oxidation
journal, December 2015
- Wang, Chunlei; Wang, Hengwei; Yao, Qi
- The Journal of Physical Chemistry C, Vol. 120, Issue 1
Catalytic Oxidation of Carbon Monoxide on Monodispersed Platinum Clusters: Each Atom Counts
journal, April 1999
- Heiz, U.; Sanchez, A.; Abbet, S.
- Journal of the American Chemical Society, Vol. 121, Issue 13
Imaging Isolated Gold Atom Catalytic Sites in Zeolite NaY
journal, March 2012
- Lu, Jing; Aydin, Ceren; Browning, Nigel D.
- Angewandte Chemie International Edition, Vol. 51, Issue 24
Carbon monoxide-induced adatom sintering in a Pd–Fe3O4 model catalyst
journal, June 2013
- Parkinson, Gareth S.; Novotny, Zbynek; Argentero, Giacomo
- Nature Materials, Vol. 12, Issue 8
Atomically Dispersed Au–(OH) x Species Bound on Titania Catalyze the Low-Temperature Water-Gas Shift Reaction
journal, March 2013
- Yang, Ming; Allard, Lawrence F.; Flytzani-Stephanopoulos, Maria
- Journal of the American Chemical Society, Vol. 135, Issue 10
Spectroscopic study of the interaction of carbon monoxide with cationic and metallic palladium in palladium–alumina catalysts
journal, January 1992
- Tessier, Didier; Rakai, Ahmed; Bozon-Verduraz, François
- J. Chem. Soc., Faraday Trans., Vol. 88, Issue 5
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
Single-atom Catalysis Using Pt/Graphene Achieved through Atomic Layer Deposition
journal, May 2013
- Sun, Shuhui; Zhang, Gaixia; Gauquelin, Nicolas
- Scientific Reports, Vol. 3, Issue 1
Palladium Nanoparticle Formation on TiO 2 (110) by Thermal Decomposition of Palladium(II) Hexafluoroacetylacetonate
journal, August 2014
- Gharachorlou, Amir; Detwiler, Michael D.; Nartova, Anna V.
- ACS Applied Materials & Interfaces, Vol. 6, Issue 16
Resolving Precursor Deligation, Surface Species Evolution, and Nanoparticle Nucleation during Palladium Atomic Layer Deposition
journal, May 2013
- Lei, Yu; Lu, Junling; Zhao, Haiyan
- The Journal of Physical Chemistry C, Vol. 117, Issue 21
Atomic Layer Deposition: An Overview
journal, January 2010
- George, Steven M.
- Chemical Reviews, Vol. 110, Issue 1, p. 111-131
Single-atom catalysis of CO oxidation using Pt1/FeOx
journal, July 2011
- Qiao, Botao; Wang, Aiqin; Yang, Xiaofeng
- Nature Chemistry, Vol. 3, Issue 8
The Surface Chemistry of Atomic Layer Depositions of Solid Thin Films
journal, May 2012
- Zaera, Francisco
- The Journal of Physical Chemistry Letters, Vol. 3, Issue 10
The adsorption and oxidation of methanol on thin palladium films
journal, August 1996
- Francis, S. M.; Corneille, J.; Goodman, D. W.
- Surface Science, Vol. 364, Issue 1
Titanium isopropoxide as a precursor for atomic layer deposition: characterization of titanium dioxide growth process
journal, July 2000
- Aarik, Jaan; Aidla, Aleks; Uustare, Teet
- Applied Surface Science, Vol. 161, Issue 3-4
Adsorbate-Induced Structural Changes in 1–3 nm Platinum Nanoparticles
journal, June 2014
- Lei, Yu; Zhao, Haiyan; Rivas, Rosa Diaz
- Journal of the American Chemical Society, Vol. 136, Issue 26
Design and synthesis of model and practical palladium catalysts using atomic layer deposition
journal, January 2016
- Lu, Zheng; Kizilkaya, Orhan; Kropf, A. Jeremy
- Catalysis Science & Technology, Vol. 6, Issue 18
Mononuclear Zeolite-Supported Iridium: Kinetic, Spectroscopic, Electron Microscopic, and Size-Selective Poisoning Evidence for an Atomically Dispersed True Catalyst at 22 °C
journal, August 2012
- Bayram, Ercan; Lu, Jing; Aydin, Ceren
- ACS Catalysis, Vol. 2, Issue 9
Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts
journal, September 2015
- Ding, K.; Gulec, A.; Johnson, A. M.
- Science, Vol. 350, Issue 6257
Cluster Chemistry: Size-Dependent Reactivity Induced by Reverse Spill-Over
journal, August 2007
- Röttgen, Martin A.; Abbet, Stephane; Judai, Ken
- Journal of the American Chemical Society, Vol. 129, Issue 31
Selective Vapor-Phase Epoxidation of Propylene over Au/TiO2Catalysts in the Presence of Oxygen and Hydrogen
journal, September 1998
- Hayashi, Toshio; Tanaka, Koji; Haruta, Masatake
- Journal of Catalysis, Vol. 178, Issue 2
CO Oxidation Catalyzed by Supported Gold: Cooperation between Gold and Nanocrystalline Rare-Earth Supports Forms Reactive Surface Superoxide and Peroxide Species
journal, July 2005
- Guzman, Javier; Carrettin, Silvio; Fierro-Gonzalez, Juan C.
- Angewandte Chemie, Vol. 117, Issue 30
Imaging Isolated Gold Atom Catalytic Sites in Zeolite NaY
journal, March 2012
- Lu, Jing; Aydin, Ceren; Browning, Nigel D.
- Angewandte Chemie, Vol. 124, Issue 24
A nanostructured cathode architecture for low charge overpotential in lithium-oxygen batteries
journal, August 2013
- Lu, Jun; Lei, Yu; Lau, Kah Chun
- Nature Communications, Vol. 4, Issue 1
Works referencing / citing this record:
Recent Advances in Atomic Metal Doping of Carbon-based Nanomaterials for Energy Conversion
journal, April 2017
- Bayatsarmadi, Bita; Zheng, Yao; Vasileff, Anthony
- Small, Vol. 13, Issue 21
Strategies for Stabilizing Atomically Dispersed Metal Catalysts
journal, December 2017
- Qin, Ruixuan; Liu, Pengxin; Fu, Gang
- Small Methods, Vol. 2, Issue 1
Recent Advances for MOF‐Derived Carbon‐Supported Single‐Atom Catalysts
journal, February 2019
- Han, Aijuan; Wang, Bingqing; Kumar, Anuj
- Small Methods, Vol. 3, Issue 9
C 2 N-graphene supported single-atom catalysts for CO 2 electrochemical reduction reaction: mechanistic insight and catalyst screening
journal, January 2018
- Cui, Xudong; An, Wei; Liu, Xiaoyang
- Nanoscale, Vol. 10, Issue 32
Atmosphere-dependent stability and mobility of catalytic Pt single atoms and clusters on γ-Al 2 O 3
journal, January 2019
- Dessal, Caroline; Sangnier, Alexis; Chizallet, Céline
- Nanoscale, Vol. 11, Issue 14