Electrocatalytic Study of the Oxygen Reduction Reaction at Gold Nanoparticles in the Absence and Presence of Interactions with SnOx Supports

Ostojic, Nevena; Duan, Zhiyao; Galyamova, Aigerim; Henkelman, Graeme; Crooks, Richard M.

doi:10.1021/jacs.8b08036

Title: Electrocatalytic Study of the Oxygen Reduction Reaction at Gold Nanoparticles in the Absence and Presence of Interactions with SnO_x Supports

Journal Article · Fri Oct 12 00:00:00 EDT 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b08036· OSTI ID:1617148

Ostojic, Nevena ^[1]; Duan, Zhiyao ^[1]; Galyamova, Aigerim ^[1];

^[1];

^[1]

Univ. of Texas, Austin, TX (United States)

Here we report that density functional theory (DFT) can be used to accurately predict how Au nanoparticle (NP) catalysts cooperate with SnO_x (x = 1.9 or 2.0) supports to carry out the oxygen reduction reaction (ORR). Specifically, dendrimers were used to encapsulate AuNPs and prevent their interactions with the underlying SnO_x supports. After removal of the dendrimers, however, the AuNPs are brought into direct contact with the support and hence feel its effect. The results show that both SnO_1.9 and SnO_2.0 supports strongly enhance the electrocatalytic properties of AuNPs for the ORR. In the case of AuNP interaction with a SnO_1.9 support, the number of electrons involved in the ORR (n_eff) increases from 2.1 ± 0.2 to 2.9 ± 0.1 following removal of the dendrimers, indicating an increased preference for the desired four-electron product (water), while the overpotential decreases by 0.32 V. Similarly, direct interactions between AuNPs and a SnO_2.0 support result in an increase in n_eff from 2.2 ± 0.1 to 3.1 ± 0.1 and a reduction of the overpotential by 0.28 V. These experimental results are in excellent agreement with the theoretically predicted onset potential shift of 0.30 V. According to the DFT calculations, the observed activity enhancements are attributed to the existence of anionic Au resulting from electron transfer from surface oxygen vacancies within the SnO_x supports to the AuNPs. This theoretical finding was confirmed experimentally using X-ray photoelectron spectroscopy. Importantly, the calculations reported here were performed prior to the experiments. Furthermore, this study represents an unusual case of theory accurately predicting the electrocatalytic manifestation of strong metal support interactions.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Univ. of Texas, Austin, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Robert A. Welch Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0010576; F-0032; F-1841

OSTI ID:: 1617148

Alternate ID(s):: OSTI ID: 1496830

Journal Information:: Journal of the American Chemical Society, Vol. 140, Issue 42; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 35 works

Citation information provided by
Web of Science

References (60)

Synthesis and catalytic properties of metal nanoparticles: Size, shape, support, composition, and oxidation state effects Cuenya, Beatriz Roldan Thin Solid Films, Vol. 518, Issue 12 https://doi.org/10.1016/j.tsf.2010.01.018	journal	April 2010
Advanced Electron Microscopy of Metal-Support Interactions in Supported Metal Catalysts Liu, Jingyue Jimmy ChemCatChem, Vol. 3, Issue 6 https://doi.org/10.1002/cctc.201100090	journal	June 2011
Promotion, Electrochemical Promotion and Metal–Support Interactions: Their Common Features Vayenas, Costas G. Catalysis Letters, Vol. 143, Issue 11 https://doi.org/10.1007/s10562-013-1128-x	journal	October 2013
A Case of Strong Metal-Support Interactions: Combining Advanced Microscopy and Model Systems to Elucidate the Atomic Structure of Interfaces Willinger, Marc G.; Zhang, Wei; Bondarchuk, Oleksandr Angewandte Chemie International Edition, Vol. 53, Issue 23 https://doi.org/10.1002/anie.201400290	journal	May 2014
Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide Tauster, S. J.; Fung, S. C.; Garten, R. L. Journal of the American Chemical Society, Vol. 100, Issue 1 https://doi.org/10.1021/ja00469a029	journal	January 1978
Strong metal-support interactions Tauster, S. J. Accounts of Chemical Research, Vol. 20, Issue 11 https://doi.org/10.1021/ar00143a001	journal	November 1987
Systematic study of transition-metal (Fe, Co, Ni, Cu) phthalocyanines as electrocatalysts for oxygen reduction and their evaluation by DFT Zhang, Zhengping; Yang, Shaoxuan; Dou, Meiling RSC Advances, Vol. 6, Issue 71 https://doi.org/10.1039/C6RA12426G	journal	January 2016
CO Oxidation at the Au/TiO ₂ Boundary: The Role of the Au/Ti _5c Site Duan, Zhiyao; Henkelman, Graeme ACS Catalysis, Vol. 5, Issue 3 https://doi.org/10.1021/cs501610a	journal	February 2015
CO Oxidation Mechanism on CeO ₂ -Supported Au Nanoparticles Kim, Hyun You; Lee, Hyuck Mo; Henkelman, Graeme Journal of the American Chemical Society, Vol. 134, Issue 3 https://doi.org/10.1021/ja207510v	journal	January 2012
Oxygen Reduction in Alkaline Media: From Mechanisms to Recent Advances of Catalysts Ge, Xiaoming; Sumboja, Afriyanti; Wuu, Delvin ACS Catalysis, Vol. 5, Issue 8 https://doi.org/10.1021/acscatal.5b00524	journal	July 2015
Au–metal oxide support interface as catalytic active sites Wu, Yi Y.; Mashayekhi, Neema A.; Kung, Harold H. Catalysis Science & Technology, Vol. 3, Issue 11 https://doi.org/10.1039/c3cy00243h	journal	January 2013
CO Oxidation on Gold-Supported Iron Oxides: New Insights into Strong Oxide–Metal Interactions Yu, Liang; Liu, Yun; Yang, Fan The Journal of Physical Chemistry C, Vol. 119, Issue 29 https://doi.org/10.1021/acs.jpcc.5b03315	journal	July 2015
Tuning metal support interactions enhances the activity and durability of TiO2-supported Pt nanocatalysts Hsieh, Bing-Jen; Tsai, Meng-Che; Pan, Chun-Jern Electrochimica Acta, Vol. 224 https://doi.org/10.1016/j.electacta.2016.12.020	journal	January 2017
Metal–Support Interactions between Nanosized Pt and Metal Oxides (WO ₃ and TiO ₂ ) Studied Using X-ray Photoelectron Spectroscopy Lewera, Adam; Timperman, Laure; Roguska, Agata The Journal of Physical Chemistry C, Vol. 115, Issue 41 https://doi.org/10.1021/jp2068446	journal	September 2011
CO oxidation on nanostructured SnOx/Pt(111) surfaces: unique properties of reduced SnOx Axnanda, Stephanus; Zhou, Wei-Ping; White, Michael G. Physical Chemistry Chemical Physics, Vol. 14, Issue 29 https://doi.org/10.1039/c2cp41601h	journal	January 2012
Niobium oxide-supported platinum ultra-low amount electrocatalysts for oxygen reduction Sasaki, K.; Zhang, L.; Adzic, R. R. Phys. Chem. Chem. Phys., Vol. 10, Issue 1 https://doi.org/10.1039/B709893F	journal	January 2008
Support effects on the oxidation of ethanol at Pt nanoparticles Moghaddam, Reza B.; Pickup, Peter G. Electrochimica Acta, Vol. 65 https://doi.org/10.1016/j.electacta.2012.01.042	journal	March 2012
Electrochemically enhanced metal-support interaction of highly dispersed Ru nanoparticles with a CeO2 support Dole, H. A. E.; Safady, L. F.; Ntais, S. Journal of Catalysis, Vol. 318 https://doi.org/10.1016/j.jcat.2014.07.003	journal	October 2014
Influence of TiO ₂ Bulk Defects on CO Adsorption and CO Oxidation on Au/TiO ₂ : Electronic Metal–Support Interactions (EMSIs) in Supported Au Catalysts Wang, Yuchen; Widmann, Daniel; Behm, R. Juergen ACS Catalysis, Vol. 7, Issue 4 https://doi.org/10.1021/acscatal.7b00251	journal	February 2017
Enhancement in Ethanol Electrooxidation by SnO _x Nanoislands Grown on Pt(111): Effect of Metal Oxide–Metal Interface Sites Zhou, Wei-Ping; Axnanda, Stephanus; White, Michael G. The Journal of Physical Chemistry C, Vol. 115, Issue 33 https://doi.org/10.1021/jp203770x	journal	August 2011
Ternary Pt/Rh/SnO₂ electrocatalysts for oxidizing ethanol to CO₂ Kowal, A.; Li, M.; Shao, M. Nature Materials, Vol. 8, Issue 4, p. 325-330 https://doi.org/10.1038/nmat2359	journal	January 2009
Strong metal–support interaction improves activity and stability of Pt electrocatalysts on doped metal oxides Jiménez-Morales, Ignacio; Cavaliere, Sara; Jones, Deborah Physical Chemistry Chemical Physics, Vol. 20, Issue 13 https://doi.org/10.1039/C8CP00176F	journal	January 2018
Nanostructured platinum becomes alloyed at oxide-composite substrate Timperman, L.; Lewera, A.; Vogel, W. Electrochemistry Communications, Vol. 12, Issue 12 https://doi.org/10.1016/j.elecom.2010.10.020	journal	December 2010
Enhanced Oxygen Reduction Reaction Activity Due to Electronic Effects between Ag and Mn ₃ O ₄ in Alkaline Media Park, Shin-Ae; Lim, Hankwon; Kim, Yong-Tae ACS Catalysis, Vol. 5, Issue 7 https://doi.org/10.1021/acscatal.5b00495	journal	June 2015
Electrooxidation of Methanol at SnO _x –Pt Interface: A Tunable Activity of Tin Oxide Nanoparticles Zhou, Wei-Ping; An, Wei; Su, Dong The Journal of Physical Chemistry Letters, Vol. 3, Issue 22 https://doi.org/10.1021/jz3015925	journal	October 2012
Nanostructured electrocatalysts with tunable activity and selectivity Mistry, Hemma; Varela, Ana Sofia; Kühl, Stefanie Nature Reviews Materials, Vol. 1, Issue 4 https://doi.org/10.1038/natrevmats.2016.9	journal	March 2016
Electron Transfer Facilitated by Dendrimer-Encapsulated Pt Nanoparticles Across Ultrathin, Insulating Oxide Films Ostojic, Nevena; Thorpe, James H.; Crooks, Richard M. Journal of the American Chemical Society, Vol. 138, Issue 21 https://doi.org/10.1021/jacs.6b03149	journal	May 2016
Microelectrochemical Flow Cell for Studying Electrocatalytic Reactions on Oxide-Coated Electrodes Anderson, Morgan J.; Ostojic, Nevena; Crooks, Richard M. Analytical Chemistry, Vol. 89, Issue 20 https://doi.org/10.1021/acs.analchem.7b03016	journal	October 2017
On the Origin of the Efficient Nanoparticle Mediated Electron Transfer across a Self-Assembled Monolayer Chazalviel, Jean-Noël; Allongue, Philippe Journal of the American Chemical Society, Vol. 133, Issue 4 https://doi.org/10.1021/ja109295x	journal	February 2011
Electrochemical charge transfer mediated by metal nanoparticles and quantum dots Kissling, Gabriela P.; Miles, David O.; Fermín, David J. Physical Chemistry Chemical Physics, Vol. 13, Issue 48 https://doi.org/10.1039/c1cp21996k	journal	January 2011
Nanoparticle Mediated Electron Transfer Across Organic Layers: From Current Understanding to Applications Gooding, J. Justin; Alam, Muhammad Tanzirul; Barfidokht, Abbas Journal of the Brazilian Chemical Society https://doi.org/10.5935/0103-5053.20130306	journal	January 2013
Electrochemistry at a Metal Nanoparticle on a Tunneling Film: A Steady-State Model of Current Densities at a Tunneling Ultramicroelectrode Hill, Caleb M.; Kim, Jiyeon; Bard, Allen J. Journal of the American Chemical Society, Vol. 137, Issue 35 https://doi.org/10.1021/jacs.5b04519	journal	August 2015
Preparation of Cu Nanoclusters within Dendrimer Templates Zhao, Mingqi; Sun, Li; Crooks, Richard M. Journal of the American Chemical Society, Vol. 120, Issue 19 https://doi.org/10.1021/ja980438n	journal	May 1998
Tunneling Dendrimers. Enhancing Charge Transport through Insulating Layer Using Redox Molecular Objects Lhenry, Sébastien; Jalkh, Joanna; Leroux, Yann R. Journal of the American Chemical Society, Vol. 136, Issue 52 https://doi.org/10.1021/ja5110359	journal	December 2014
Dendrimer-encapsulated nanoparticles: New synthetic and characterization methods and catalytic applications Myers, V. Sue; Weir, Michael G.; Carino, Emily V. Chemical Science, Vol. 2, Issue 9 https://doi.org/10.1039/c1sc00256b	journal	January 2011
Dendrimers as Encapsulating, Stabilizing, or Directing Agents for Inorganic Nanoparticles Bronstein, Lyudmila M.; Shifrina, Zinaida B. Chemical Reviews, Vol. 111, Issue 9 https://doi.org/10.1021/cr2000724	journal	September 2011
State of the art in gold nanoparticle synthesis Zhao, Pengxiang; Li, Na; Astruc, Didier Coordination Chemistry Reviews, Vol. 257, Issue 3-4 https://doi.org/10.1016/j.ccr.2012.09.002	journal	February 2013
Size-Selective Catalytic Activity of Pd Nanoparticles Encapsulated within End-Group Functionalized Dendrimers Oh, Sang-Keun; Niu, Yanhui; Crooks, Richard M. Langmuir, Vol. 21, Issue 22 https://doi.org/10.1021/la050524i	journal	April 2005
Atomic Layer Deposition: An Overview George, Steven M. Chemical Reviews, Vol. 110, Issue 1, p. 111-131 https://doi.org/10.1021/cr900056b	journal	January 2010
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y. Physical Review B, Vol. 57, Issue 3, p. 1505-1509 https://doi.org/10.1103/PhysRevB.57.1505	journal	January 1998
Sources of Electrical Conductivity in ${SnO}_{2}$ Singh, Abhishek Kumar; Janotti, Anderson; Scheffler, Matthias Physical Review Letters, Vol. 101, Issue 5 https://doi.org/10.1103/PhysRevLett.101.055502	journal	July 2008
A fast and robust algorithm for Bader decomposition of charge density Henkelman, Graeme; Arnaldsson, Andri; Jónsson, Hannes Computational Materials Science, Vol. 36, Issue 3 https://doi.org/10.1016/j.commatsci.2005.04.010	journal	June 2006
A grid-based Bader analysis algorithm without lattice bias Tang, W.; Sanville, E.; Henkelman, G. Journal of Physics: Condensed Matter, Vol. 21, Issue 8 https://doi.org/10.1088/0953-8984/21/8/084204	journal	January 2009
The stability of SnO ₂ surfaces Mulheran, P. A.; Harding, J. H. Modelling and Simulation in Materials Science and Engineering, Vol. 1, Issue 1 https://doi.org/10.1088/0965-0393/1/1/004	journal	October 1992
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode Nørskov, J. K.; Rossmeisl, J.; Logadottir, A. The Journal of Physical Chemistry B, Vol. 108, Issue 46 https://doi.org/10.1021/jp047349j	journal	November 2004
Identifying active surface phases for metal oxide electrocatalysts: a study of manganese oxide bi-functional catalysts for oxygen reduction and water oxidation catalysis Su, Hai-Yan; Gorlin, Yelena; Man, Isabela C. Physical Chemistry Chemical Physics, Vol. 14, Issue 40 https://doi.org/10.1039/c2cp40841d	journal	January 2012
Surface Pourbaix diagrams and oxygen reduction activity of Pt, Ag and Ni(111) surfaces studied by DFT Hansen, Heine A.; Rossmeisl, Jan; Nørskov, Jens K. Physical Chemistry Chemical Physics, Vol. 10, Issue 25 https://doi.org/10.1039/b803956a	journal	January 2008
Electrochemical Properties of Metal-Oxide-Coated Carbon Electrodes Prepared by Atomic Layer Deposition Loussaert, James A.; Fosdick, Stephen E.; Crooks, Richard M. Langmuir, Vol. 30, Issue 45 https://doi.org/10.1021/la503232m	journal	November 2014
Preparation and Characterization of 1−2 nm Dendrimer-Encapsulated Gold Nanoparticles Having Very Narrow Size Distributions Kim, Yong-Gu; Oh, Sang-Keun; Crooks, Richard M. Chemistry of Materials, Vol. 16, Issue 1 https://doi.org/10.1021/cm034932o	journal	January 2004
Size Stability and H ₂ /CO Selectivity for Au Nanoparticles during Electrocatalytic CO ₂ Reduction Trindell, Jamie A.; Clausmeyer, Jan; Crooks, Richard M. Journal of the American Chemical Society, Vol. 139, Issue 45 https://doi.org/10.1021/jacs.7b06775	journal	November 2017
Au@Pt dendrimer encapsulated nanoparticles as model electrocatalysts for comparison of experiment and theory Yancey, David F.; Zhang, Liang; Crooks, Richard M. Chemical Science, Vol. 3, Issue 4 https://doi.org/10.1039/c2sc00971d	journal	January 2012
A Theoretical and Experimental Approach for Correlating Nanoparticle Structure and Electrocatalytic Activity Anderson, Rachel M.; Yancey, David F.; Zhang, Liang Accounts of Chemical Research, Vol. 48, Issue 5 https://doi.org/10.1021/acs.accounts.5b00125	journal	May 2015
Calculations of CO Oxidation over a Au/TiO ₂ Catalyst: A Study of Active Sites, Catalyst Deactivation, and Moisture Effects Duan, Zhiyao; Henkelman, Graeme ACS Catalysis, Vol. 8, Issue 2 https://doi.org/10.1021/acscatal.7b03993	journal	January 2018
Origins of Coexistence of Conductivity and Transparency in ${SnO}_{2}$ Kılıç, Çetin; Zunger, Alex Physical Review Letters, Vol. 88, Issue 9 https://doi.org/10.1103/PhysRevLett.88.095501	journal	February 2002
Electrocatalytic Reduction of Oxygen on Platinum Nanoparticles in the Presence and Absence of Interactions with the Electrode Surface Ostojic, Nevena; Crooks, Richard M. Langmuir, Vol. 32, Issue 38 https://doi.org/10.1021/acs.langmuir.6b02578	journal	September 2016

Cited By (2)

Interfacial effects in supported catalysts for electrocatalysis Li, Hao; Chen, Chen; Yan, Dafeng Journal of Materials Chemistry A, Vol. 7, Issue 41 https://doi.org/10.1039/c9ta04888j	journal	January 2019
Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study Li, Qiaoling; Zhang, Tianran; Yu, Xiaofei Frontiers in Chemistry, Vol. 7 https://doi.org/10.3389/fchem.2019.00674	journal	October 2019

Similar Records

Effect of TiO_x Substrate Interactions on the Electrocatalytic Oxygen Reduction Reaction at Au Nanoparticles

Journal Article · Tue Apr 28 00:00:00 EDT 2020 · Journal of Physical Chemistry. C · OSTI ID:1617148

Galyamova, Aigerim; Shin, Kihyun; Henkelman, Graeme; +1 more

Electrooxidation of CO on Platinum Nanoparticles Supported on NiO Thin Films

Journal Article · Tue Apr 11 00:00:00 EDT 2023 · Journal of Physical Chemistry. C · OSTI ID:1617148

Galyamova, Aigerim; Ha, Hyunwoo; Henkelman, Graeme; +1 more

Electrochemical Cleaning Stability and Oxygen Reduction Reaction Activity of 1-2 nm Dendrimer-Encapsulated Au Nanoparticles

Journal Article · Tue Jul 06 00:00:00 EDT 2021 · ChemElectroChem · OSTI ID:1617148

Strasser, Juliette W.; Hersbach, Thomas P.; Liu, Jing; +3 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
redox reactions
metal nanoparticles
gold
electrodes
dendrons

Title: Electrocatalytic Study of the Oxygen Reduction Reaction at Gold Nanoparticles in the Absence and Presence of Interactions with SnOx Supports

Citation Formats

References (60)

Cited By (2)

Similar Records

Related Subjects

Title: Electrocatalytic Study of the Oxygen Reduction Reaction at Gold Nanoparticles in the Absence and Presence of Interactions with SnO_x Supports