Hydrogen migration at restructuring palladium–silver oxide boundaries dramatically enhances reduction rate of silver oxide

O’Connor, Christopher R.; van Spronsen, Matthijs A.; Egle, Tobias; Xu, Fang; Kersell, Heath R.; Oliver-Meseguer, Judit; Karatok, Mustafa; Salmeron, Miquel; Madix, Robert J.; Friend, Cynthia M.

doi:10.1038/s41467-020-15536-x

Hydrogen migration at restructuring palladium–silver oxide boundaries dramatically enhances reduction rate of silver oxide

Journal Article · Wed Apr 15 00:00:00 EDT 2020 · Nature Communications

DOI:https://doi.org/10.1038/s41467-020-15536-x· OSTI ID:1695723

^[1]; ^[2]; ^[1]; ^[1]; Kersell, Heath R. ^[3]; Oliver-Meseguer, Judit ^[3]; ^[1]; ^[4]; Madix, Robert J. ^[1]; ^[1]

Harvard Univ., Cambridge, MA (United States)
Harvard Univ., Cambridge, MA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)

Heterogeneous catalysts are complex materials with multiple interfaces. A critical proposition in exploiting bifunctionality in alloy catalysts is to achieve surface migration across interfaces separating functionally dissimilar regions. Herein, we demonstrate the enhancement of more than 10⁴ in the rate of molecular hydrogen reduction of a silver surface oxide in the presence of palladium oxide compared to pure silver oxide resulting from the transfer of atomic hydrogen from palladium oxide islands onto the surrounding surface formed from oxidation of a palladium-silver alloy. The palladium-silver interface also dynamically restructures during reduction, resulting in silver-palladium intermixing. This study clearly demonstrates the migration of reaction intermediates and catalyst material across surface interfacial boundaries in alloys with a significant effect on surface reactivity, having broad implications for the catalytic function of bimetallic materials.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC); Harvard Univ., Cambridge, MA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0012573

OSTI ID:: 1695723

Alternate ID(s):: OSTI ID: 1843584

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 11; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (67)

Investigation of the Support Effect in Atomically Dispersed Pt on WO _{3− x} for Utilization of Pt in the Hydrogen Evolution Reaction Park, Jinkyu; Lee, Seonggyu; Kim, Hee‐Eun Angewandte Chemie International Edition, Vol. 58, Issue 45 https://doi.org/10.1002/anie.201908122	journal	November 2019
Low-Temperature Oxidation of CO over Gold Supported on TiO2, α-Fe2O3, and Co3O4 Haruta, M.; Tsubota, S.; Kobayashi, T. Journal of Catalysis, Vol. 144, Issue 1 https://doi.org/10.1006/jcat.1993.1322	journal	November 1993
Bimetallic Particle Formation in Pt–Re/Al2O3Reforming Catalysts Revealed by Energy-Dispersive X-Ray Spectrometry in the Analytical Electron Microscope Prestvik, Rune; Tøtdal, Bård; Lyman, Charles E. Journal of Catalysis, Vol. 176, Issue 1 https://doi.org/10.1006/jcat.1998.2025	journal	May 1998
Influence of Pretreatment Temperature on the Bimetallic Interactions in Pt-Re/Al2O3 Reforming Catalysts Studied by X-Ray Absorption Spectroscopy Rønning, Magnus; Gjervan, Torbjørn; Prestvik, Rune Journal of Catalysis, Vol. 204, Issue 2 https://doi.org/10.1006/jcat.2001.3399	journal	December 2001
Hydrogen evolution reaction (h.e.r.) in an acidic or basic medium on nickel electrodeposited with PW12O 40 3- and Cu2+ Savadogo, O.; Ndzebet, E. Journal of Applied Electrochemistry, Vol. 23, Issue 9 https://doi.org/10.1007/BF00251027	journal	September 1993
The kinetics and mechanism of spillover Levy, R. Journal of Catalysis, Vol. 32, Issue 2 https://doi.org/10.1016/0021-9517(74)90080-3	journal	February 1974
The effect of drying temperature on the temperature-programmed reduction profile of a platinum/rhenium/alumina catalyst Isaacs, B. Journal of Catalysis, Vol. 77, Issue 1 https://doi.org/10.1016/0021-9517(82)90144-0	journal	September 1982
Surface mobility of Re2O7 in the system Re7+Pd0/$gamma;-Al2O3 Ziemecki, S. Journal of Catalysis, Vol. 99, Issue 1 https://doi.org/10.1016/0021-9517(86)90213-7	journal	May 1986
Gold catalysts prepared by coprecipitation for low-temperature oxidation of hydrogen and of carbon monoxide Haruta, M. Journal of Catalysis, Vol. 115, Issue 2 https://doi.org/10.1016/0021-9517(89)90034-1	journal	February 1989
Adsorption of hydrogen on palladium single crystal surfaces Conrad, H.; Ertl, G.; Latta, E. E. Surface Science, Vol. 41, Issue 2 https://doi.org/10.1016/0039-6028(74)90060-0	journal	February 1974
The reaction of atomic copper with chemisorbed hydrogen on ruthenium Goodman, D. W.; Yates, J. T.; Peden, C. H. F. Surface Science, Vol. 164, Issue 2-3 https://doi.org/10.1016/0039-6028(85)90756-3	journal	December 1985
Chemisorption of atomic hydrogen on clean and Cl-covered Ag(111) Zhou, X. -L.; White, J. M.; Koel, B. E. Surface Science, Vol. 218, Issue 1 https://doi.org/10.1016/0039-6028(89)90627-4	journal	August 1989
Mobility of Ag adatoms on Ag(100) Langelaar, M. H.; Breeman, M.; Boerma, D. O. Surface Science, Vol. 352-354 https://doi.org/10.1016/0039-6028(95)01208-7	journal	May 1996
Kinetic modelling of the H2O2 reaction on Pd and of its influence on the hydrogen response of a hydrogen sensitive Pd metal-oxide-semiconductor device Fogelberg, Joakim; Petersson, Lars-Gunnar Surface Science, Vol. 350, Issue 1-3 https://doi.org/10.1016/0039-6028(96)80059-8	journal	April 1996
Alloy formation and metal oxide segregation in PtRe/γ-AlO catalysts as investigated by temperature-programmed reduction Wagstaff, N.; Prins, R. Journal of Catalysis, Vol. 59, Issue 3 https://doi.org/10.1016/S0021-9517(79)80012-3	journal	October 1979
The adsorption of water and oxygen on Ag(110): A study of the interactions among water molecules, hydroxyl groups, and oxygen atoms Bange, K.; Madey, T. E.; Sass, J. K. Surface Science, Vol. 183, Issue 3 https://doi.org/10.1016/S0039-6028(87)80215-7	journal	May 1987
Alloy surfaces: segregation, reconstruction and phase transitions Tréglia, G.; Legrand, B.; Ducastelle, F. Computational Materials Science, Vol. 15, Issue 2 https://doi.org/10.1016/S0927-0256(99)00004-X	journal	June 1999
Some recent theoretical advances in the understanding of the catalytic activity of Au Molina, L. M.; Hammer, B. Applied Catalysis A: General, Vol. 291, Issue 1-2 https://doi.org/10.1016/j.apcata.2005.01.050	journal	September 2005
Observation and simulation of hydrogen storage via spillover Wang, Cheng-Yu; Chang, Cheng-Wei; Wu, Yi-Ju Current Opinion in Chemical Engineering, Vol. 21 https://doi.org/10.1016/j.coche.2018.10.005	journal	September 2018
A systematic theoretical study of water dissociation on clean and oxygen-preadsorbed transition metals Wang, G.; Tao, S.; Bu, X. Journal of Catalysis, Vol. 244, Issue 1 https://doi.org/10.1016/j.jcat.2006.07.034	journal	November 2006
Evolution of steady-state material properties during catalysis: Oxidative coupling of methanol over nanoporous Ag0.03Au0.97 Zugic, Branko; van Spronsen, Matthijs A.; Heine, Christian Journal of Catalysis, Vol. 380 https://doi.org/10.1016/j.jcat.2019.08.041	journal	December 2019
Direct evidence of hydrogen spillover from Ni to Cu on Ni–Cu bimetallic catalysts Yao, Yunxi; Goodman, D. Wayne Journal of Molecular Catalysis A: Chemical, Vol. 383-384 https://doi.org/10.1016/j.molcata.2013.12.013	journal	March 2014
Reactivity of methanol on TiO2 nanoparticles supported on the Au(111) surface Farfan-Arribas, Enrique; Biener, Jürgen; Friend, Cynthia M. Surface Science, Vol. 591, Issue 1-3 https://doi.org/10.1016/j.susc.2005.06.002	journal	October 2005
Surface composition of clean and oxidized Pd75Ag25(100) from photoelectron spectroscopy and density functional theory calculations Walle, L. E.; Grönbeck, H.; Fernandes, V. R. Surface Science, Vol. 606, Issue 23-24 https://doi.org/10.1016/j.susc.2012.07.006	journal	December 2012
Atomic and Molecular Adsorption on Ag(111) Chen, Benjamin W. J.; Kirvassilis, Demetrios; Bai, Yunhai The Journal of Physical Chemistry C, Vol. 123, Issue 13 https://doi.org/10.1021/acs.jpcc.7b11629	journal	January 2018
Dynamics of Surface Alloys: Rearrangement of Pd/Ag(111) Induced by CO and O ₂ van Spronsen, Matthijs A.; Daunmu, Kaining; O’Connor, Christopher R. The Journal of Physical Chemistry C, Vol. 123, Issue 13 https://doi.org/10.1021/acs.jpcc.8b08849	journal	October 2018
Inverse Oxide/Metal Catalysts in Fundamental Studies and Practical Applications: A Perspective of Recent Developments Rodriguez, José A.; Liu, Ping; Graciani, Jesús The Journal of Physical Chemistry Letters, Vol. 7, Issue 13 https://doi.org/10.1021/acs.jpclett.6b00499	journal	June 2016
Understanding Heterolytic H ₂ Cleavage and Water-Assisted Hydrogen Spillover on Fe ₃ O ₄ (001)-Supported Single Palladium Atoms Doudin, Nassar; Yuk, Simuck F.; Marcinkowski, Matthew D. ACS Catalysis, Vol. 9, Issue 9 https://doi.org/10.1021/acscatal.9b01425	journal	July 2019
Catalysis by alloys and bimetallic clusters Sinfelt, John H. Accounts of Chemical Research, Vol. 10, Issue 1 https://doi.org/10.1021/ar50109a003	journal	January 1977
Hydrogen Spillover. Facts and Fiction Prins, R. Chemical Reviews, Vol. 112, Issue 5 https://doi.org/10.1021/cr200346z	journal	February 2012
Catalysis Science of Bulk Mixed Oxides Wachs, Israel E.; Routray, Kamalakanta ACS Catalysis, Vol. 2, Issue 6 https://doi.org/10.1021/cs2005482	journal	April 2012
In Situ Spectroscopic Study of the Oxidation and Reduction of Pd(111) Ketteler, Guido; Ogletree, D. Frank; Bluhm, Hendrik Journal of the American Chemical Society, Vol. 127, Issue 51 https://doi.org/10.1021/ja055754y	journal	December 2005
CO Oxidation on Inverse CeO _x /Cu(111) Catalysts: High Catalytic Activity and Ceria-Promoted Dissociation of O ₂ Yang, Fan; Graciani, Jesús; Evans, Jaime Journal of the American Chemical Society, Vol. 133, Issue 10 https://doi.org/10.1021/ja1087979	journal	March 2011
Hydrogen Activation on Silver: A Computational Study on Surface and Subsurface Oxygen Species Mohammad, Amjad B.; Yudanov, Ilya V.; Lim, Kok Hwa The Journal of Physical Chemistry C, Vol. 112, Issue 5 https://doi.org/10.1021/jp0765190	journal	February 2008
Dissociative Adsorption of Hydrogen on PdO(101) Studied by HRCLS and DFT Martin, N. M.; Van den Bossche, M.; Grönbeck, H. The Journal of Physical Chemistry C, Vol. 117, Issue 26 https://doi.org/10.1021/jp4036698	journal	June 2013
Mechanisms for H ₂ Reduction on the PdO{101} Surface and the Pd{100}-(√5 × √5) R 27°-O Surface Oxide Blanco-Rey, M.; Wales, D. J.; Jenkins, S. J. The Journal of Physical Chemistry C, Vol. 113, Issue 38 https://doi.org/10.1021/jp904693t	journal	August 2009
Hydrogen Dissociation, Spillover, and Desorption from Cu-Supported Co Nanoparticles Lewis, Emily A.; Marcinkowski, Matthew D.; Murphy, Colin J. The Journal of Physical Chemistry Letters, Vol. 5, Issue 19 https://doi.org/10.1021/jz5016789	journal	September 2014
Catalyst support effects on hydrogen spillover Karim, Waiz; Spreafico, Clelia; Kleibert, Armin Nature, Vol. 541, Issue 7635 https://doi.org/10.1038/nature20782	journal	January 2017
Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts Matsubu, John C.; Zhang, Shuyi; DeRita, Leo Nature Chemistry, Vol. 9, Issue 2 https://doi.org/10.1038/nchem.2607	journal	September 2016
Highly porous non-precious bimetallic electrocatalysts for efficient hydrogen evolution Lu, Qi; Hutchings, Gregory S.; Yu, Weiting Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7567	journal	March 2015
Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts Zugic, Branko; Wang, Lucun; Heine, Christian Nature Materials, Vol. 16, Issue 5 https://doi.org/10.1038/nmat4824	journal	December 2016
Structural evolution of atomically dispersed Pt catalysts dictates reactivity DeRita, Leo; Resasco, Joaquin; Dai, Sheng Nature Materials, Vol. 18, Issue 7 https://doi.org/10.1038/s41563-019-0349-9	journal	April 2019
Catalyst deactivation via decomposition into single atoms and the role of metal loading Goodman, Emmett D.; Johnston-Peck, Aaron C.; Dietze, Elisabeth M. Nature Catalysis, Vol. 2, Issue 9 https://doi.org/10.1038/s41929-019-0328-1	journal	August 2019
A computational study of H ₂ dissociation on silver surfaces: The effect of oxygen in the added row structure of Ag(110) Mohammad, Amjad B.; Hwa Lim, Kok; Yudanov, Ilya V. Phys. Chem. Chem. Phys., Vol. 9, Issue 10 https://doi.org/10.1039/B616675J	journal	January 2007
New approaches to hydrogen storage Graetz, Jason Chem. Soc. Rev., Vol. 38, Issue 1 https://doi.org/10.1039/B718842K	journal	January 2009
Thermodynamic and spectroscopic properties of oxygen on silver under an oxygen atmosphere Jones, Travis E.; Rocha, Tulio C. R.; Knop-Gericke, Axel Physical Chemistry Chemical Physics, Vol. 17, Issue 14 https://doi.org/10.1039/C5CP00342C	journal	January 2015
Generalized nano-thermodynamic model for capturing size-dependent surface segregation in multi-metal alloy nanoparticles Divi, Srikanth; Chatterjee, Abhijit RSC Advances, Vol. 8, Issue 19 https://doi.org/10.1039/C8RA00945G	journal	January 2018
Bimetallic catalysts for hydrogen generation Wei, Zhehao; Sun, Junming; Li, Yan Chemical Society Reviews, Vol. 41, Issue 24 https://doi.org/10.1039/c2cs35201j	journal	January 2012
Alloys in catalysis: phase separation and surface segregation phenomena in response to the reactive environment Zafeiratos, Spiros; Piccinin, Simone; Teschner, Detre Catalysis Science & Technology, Vol. 2, Issue 9 https://doi.org/10.1039/c2cy00487a	journal	January 2012
Single atom alloy surface analogs in Pd0.18Cu15 nanoparticles for selective hydrogenation reactions Boucher, Matthew B.; Zugic, Branko; Cladaras, George Physical Chemistry Chemical Physics, Vol. 15, Issue 29 https://doi.org/10.1039/c3cp51538a	journal	January 2013
A scanning tunneling microscopy study of the reaction between hydrogen and oxygen to form water on Pd(111) Mitsui, T.; Rose, M. K.; Fomin, E. The Journal of Chemical Physics, Vol. 117, Issue 12 https://doi.org/10.1063/1.1502655	journal	September 2002
Density functional calculations of hydrogen adsorption on palladium–silver alloy surfaces Løvvik, O. M.; Olsen, R. A. The Journal of Chemical Physics, Vol. 118, Issue 7 https://doi.org/10.1063/1.1536955	journal	February 2003
Mesoscopic restructuring and mass transport of metal atoms during reduction of the Ag(111)-p(4×4)-O surface with CO Klust, Andreas; Madix, Robert J. The Journal of Chemical Physics, Vol. 126, Issue 8 https://doi.org/10.1063/1.2483919	journal	February 2007
Density functional theory in surface chemistry and catalysis Norskov, J. K.; Abild-Pedersen, F.; Studt, F. Proceedings of the National Academy of Sciences, Vol. 108, Issue 3 https://doi.org/10.1073/pnas.1006652108	journal	January 2011
Temperature Programmed Reduction Hurst, Nicholas W.; Gentry, Stephen J.; Jones, Alan Catalysis Reviews, Vol. 24, Issue 2 https://doi.org/10.1080/03602458208079654	journal	January 1982
Many-electron singularity in X-ray photoemission and X-ray line spectra from metals Doniach, S.; Sunjic, M. Journal of Physics C: Solid State Physics, Vol. 3, Issue 2 https://doi.org/10.1088/0022-3719/3/2/010	journal	February 1970
Collective excitations in x-ray spectra of metals Mahan, G. D. Physical Review B, Vol. 11, Issue 12 https://doi.org/10.1103/PhysRevB.11.4814	journal	June 1975
High-Resolution X-Ray Photoemission Spectrum of the Valence Bands of Gold Shirley, D. A. Physical Review B, Vol. 5, Issue 12 https://doi.org/10.1103/PhysRevB.5.4709	journal	June 1972
Direct observation of mobility and interactions of oxygen molecules chemisorbed on the Ag(110) surface Barth, J. V.; Zambelli, T.; Wintterlin, J. Physical Review B, Vol. 55, Issue 19 https://doi.org/10.1103/PhysRevB.55.12902	journal	May 1997
Phase diagrams for surface alloys Christensen, A.; Ruban, A. V.; Stoltze, P. Physical Review B, Vol. 56, Issue 10 https://doi.org/10.1103/PhysRevB.56.5822	journal	September 1997
Alloy surface segregation in reactive environments: First-principles atomistic thermodynamics study of Ag 3 Pd ( 111 ) in oxygen atmospheres Kitchin, John R.; Reuter, Karsten; Scheffler, Matthias Physical Review B, Vol. 77, Issue 7 https://doi.org/10.1103/PhysRevB.77.075437	journal	February 2008
Hydrogen Dissociation and Spillover on Individual Isolated Palladium Atoms Tierney, Heather L.; Baber, Ashleigh E.; Kitchin, John R. Physical Review Letters, Vol. 103, Issue 24 https://doi.org/10.1103/PhysRevLett.103.246102	journal	December 2009
Catalytic Role of Metal Oxides in Gold-Based Catalysts: A First Principles Study of CO Oxidation on T i O 2 Supported Au Liu, Zhi-Pan; Gong, Xue-Qing; Kohanoff, Jorge Physical Review Letters, Vol. 91, Issue 26 https://doi.org/10.1103/PhysRevLett.91.266102	journal	December 2003
Activity of CeOx and TiOx Nanoparticles Grown on Au(111) in the Water-Gas Shift Reaction Rodriguez, J. A.; Ma, S.; Liu, P. Science, Vol. 318, Issue 5857 https://doi.org/10.1126/science.1150038	journal	December 2007
Reaction-Driven Restructuring of Rh-Pd and Pt-Pd Core-Shell Nanoparticles Tao, F.; Grass, M. E.; Zhang, Y. Science, Vol. 322, Issue 5903 https://doi.org/10.1126/science.1164170	journal	November 2008
Spectroscopic Observation of Dual Catalytic Sites During Oxidation of CO on a Au/TiO2 Catalyst Green, I. X.; Tang, W.; Neurock, M. Science, Vol. 333, Issue 6043 https://doi.org/10.1126/science.1207272	journal	August 2011
Activation of Cu(111) surface by decomposition into nanoclusters driven by CO adsorption Eren, B.; Zherebetskyy, D.; Patera, L. L. Science, Vol. 351, Issue 6272 https://doi.org/10.1126/science.aad8868	journal	January 2016

Similar Records

Facilitating hydrogen atom migration via a dense phase on palladium islands to a surrounding silver surface

Journal Article · Tue Sep 01 20:00:00 EDT 2020 · Proceedings of the National Academy of Sciences of the United States of America · OSTI ID:1657616

Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts

Journal Article · Sun Dec 18 19:00:00 EST 2016 · Nature Materials · OSTI ID:1414360

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Hydrogen migration at restructuring palladium–silver oxide boundaries dramatically enhances reduction rate of silver oxide

Citation Formats

References (67)

Similar Records

Related Subjects