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Title: X-Ray Scattering and Imaging Studies of Electrode Structure and Dynamics

Abstract

We will review structures and dynamics of electrode interfaces studied in situ using x-ray scattering and imaging techniques. The examples cover single-crystal and nanocrystal structures relevant to electrocatalytic activities, anodic oxidation and corrosion, aqueous dissolution reactions, surface reconstructions, and surface modifications by under potential deposition. Here, the x-ray techniques include the widely used traditional surface x-ray scattering, such as crystal truncation rods and x-ray reflectivity, as well as recently developed resonance surface scattering, coherent surface x-ray photon correlation spectroscopy, coherent x-ray Bragg diffraction imaging, and surface ptychography. Results relevant to various electrochemical phenomena will be highlighted.

Authors:
 [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1559461
Alternate Identifier(s):
OSTI ID: 1473715
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Record
Additional Journal Information:
Journal Volume: 19; Journal Issue: 7; Journal ID: ISSN 1527-8999
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Coherent Diffraction Imaging; Electrochemical Interface; Nanofacet; Ptychography; Surface X-ray scattering

Citation Formats

You, Hoydoo. X-Ray Scattering and Imaging Studies of Electrode Structure and Dynamics. United States: N. p., 2018. Web. https://doi.org/10.1002/tcr.201800083.
You, Hoydoo. X-Ray Scattering and Imaging Studies of Electrode Structure and Dynamics. United States. https://doi.org/10.1002/tcr.201800083
You, Hoydoo. Mon . "X-Ray Scattering and Imaging Studies of Electrode Structure and Dynamics". United States. https://doi.org/10.1002/tcr.201800083. https://www.osti.gov/servlets/purl/1559461.
@article{osti_1559461,
title = {X-Ray Scattering and Imaging Studies of Electrode Structure and Dynamics},
author = {You, Hoydoo},
abstractNote = {We will review structures and dynamics of electrode interfaces studied in situ using x-ray scattering and imaging techniques. The examples cover single-crystal and nanocrystal structures relevant to electrocatalytic activities, anodic oxidation and corrosion, aqueous dissolution reactions, surface reconstructions, and surface modifications by under potential deposition. Here, the x-ray techniques include the widely used traditional surface x-ray scattering, such as crystal truncation rods and x-ray reflectivity, as well as recently developed resonance surface scattering, coherent surface x-ray photon correlation spectroscopy, coherent x-ray Bragg diffraction imaging, and surface ptychography. Results relevant to various electrochemical phenomena will be highlighted.},
doi = {10.1002/tcr.201800083},
journal = {Chemical Record},
number = 7,
volume = 19,
place = {United States},
year = {2018},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Figure 1 Figure 1: (a) A diffraction diagram for a momentum vector Q that has in-plane and normal components. The cylindrical object is an illustration of an electrochemical interface and ions in the double layer under the control of a potentiostat. $α$, and $β$ are the angles of incoming and exiting beamsmore » with respect to the electrode surface, and $φ$ is the in-plane angle of the exit beam. Vectors Ki and Ko indicate the directions of the incoming and existing x-ray beams. Vector Q is the momentum transfer, i.e., KoKi. Note that Q is decomposed to in-plane momentum transfer QII and normal momentum transfer Q. X-ray reflectivity is generally referred for the scans at QII≈0 ($φ$≈0) with typically small angles of $α$ and $β$. Specular CTR is along the direction of Q and off-specular CTRs are the direction of the vertical dashed arrows at the tip of Q. (b) An early electrochemical cell for x-ray diffraction studies in reflection mode. (c) An electrochemical cell in transmission mode used for xray reflectivity studies.« less

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Works referenced in this record:

The structure and phase behavior of electrodeposited halides on single-crystal metal surfaces
journal, April 1996


On the stability of unreconstructed Au(100)-(1×1) at negative potentials in aqueous sulfate solution
journal, September 1999


Extending the methodology of X-ray crystallography to allow imaging of micrometre-sized non-crystalline specimens
journal, July 1999

  • Miao, Jianwei; Charalambous, Pambos; Kirz, Janos
  • Nature, Vol. 400, Issue 6742
  • DOI: 10.1038/22498

The electrodeposition of Pb monolayers on low index Pt surfaces: an X-ray scattering and scanning tunneling microscopy study
journal, August 1993


Direct determination of one-dimensional interphase structures using normalized crystal truncation rod analysis
journal, April 2018

  • Kawaguchi, Tomoya; Liu, Yihua; Reiter, Anthony
  • Journal of Applied Crystallography, Vol. 51, Issue 3
  • DOI: 10.1107/S1600576718004326

Cell design for in—situ X-ray scattering study of electrodes in transmission geometry
journal, January 1991


Potential dependence of the step line tension on surfaces in contact with an electrolyte
journal, March 2003


Advanced Photon Source
journal, March 2016


High-Resolution Scanning X-ray Diffraction Microscopy
journal, July 2008


Electrochemical Interfaces of Porous Silicon and Ruthenium Dioxide
journal, January 1999

  • You, Hoydoo; Chu, Yong S.; Lister, Tedd E.
  • Japanese Journal of Applied Physics, Vol. 38, Issue S1
  • DOI: 10.7567/JJAPS.38S1.239

X-ray Crystal Truncation Rod Studies of Surface Oxidation and Reduction on Pt(111)
journal, March 2016

  • Liu, Yihua; Barbour, Andi; Komanicky, Vladimir
  • The Journal of Physical Chemistry C, Vol. 120, Issue 29
  • DOI: 10.1021/acs.jpcc.6b00492

X-ray and electrochemical studies of Cu upd on single crystal electrodes in the presence of bromide: comparison between Au(111) and Pt(111) electrodes
journal, January 1999

  • Herrero, Enrique; Glazier, Samantha; Buller, Lisa J.
  • Journal of Electroanalytical Chemistry, Vol. 461, Issue 1-2
  • DOI: 10.1016/S0022-0728(98)00066-7

Synchrotron X-ray studies of model SOFC cathodes, part I: Thin film cathodes
journal, November 2017


Four-circle angle calculations for surface diffraction
journal, February 1988


Potential Dependence of Pt and Co Dissolution from Platinum-Cobalt Alloy PEFC Catalysts Using Time-Resolved Measurements
journal, January 2018

  • Ahluwalia, Rajesh K.; Papadias, Dionissios D.; Kariuki, Nancy N.
  • Journal of The Electrochemical Society, Vol. 165, Issue 6
  • DOI: 10.1149/2.0031806jes

High-density electrosorbed carbon monoxide monolayers on Pt(111) under atmospheric pressure
journal, January 2007


Improved Oxygen Reduction Activity on Pt3Ni(111) via Increased Surface Site Availability
journal, January 2007

  • Stamenkovic, V. R.; Fowler, B.; Mun, B. S.
  • Science, Vol. 315, Issue 5811, p. 493-497
  • DOI: 10.1126/science.1135941

Stability Limits and Defect Dynamics in Ag Nanoparticles Probed by Bragg Coherent Diffractive Imaging
journal, February 2017


Partial coherence effects on the imaging of small crystals using coherent x-ray diffraction
journal, November 2001


Ab Initio Calculations of Intermediates of Oxygen Reduction on Low-Index Platinum Surfaces
journal, January 2004

  • Panchenko, A.; Koper, M. T. M.; Shubina, T. E.
  • Journal of The Electrochemical Society, Vol. 151, Issue 12
  • DOI: 10.1149/1.1809586

Stability and Dissolution of Platinum Surfaces in Perchloric Acid
journal, January 2006

  • Komanicky, V.; Chang, K. C.; Menzel, A.
  • Journal of The Electrochemical Society, Vol. 153, Issue 10
  • DOI: 10.1149/1.2229284

Surface structure and relaxation during the oxidation of carbon monoxide on Pt–Pd bimetallic surfaces
journal, May 2001


The kinetics of the (5 × 20) → (1 × 1) structural transition for Au(100)
journal, January 1992


X-Ray Intensity Fluctuation Spectroscopy Observations of Critical Dynamics in Fe3Al
journal, March 1995


Specular X-ray reflection for the “in situ” study of electrode surfaces
journal, January 1991

  • Melendres, C. A.; You, H.; Maroni, V. A.
  • Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 297, Issue 2
  • DOI: 10.1016/0022-0728(91)80051-Q

Analysis of irreversible oxidation wave of adsorbed CO at Pt(1 1 1), Pt(1 0 0) and Pt(1 1 0) electrodes
journal, June 1993

  • Kita, H.; Narumi, H.; Ye, S.
  • Journal of Applied Electrochemistry, Vol. 23, Issue 6
  • DOI: 10.1007/BF00721950

Oxidation-reduction-induced roughening of platinum (1 1 1) surface
journal, April 1994


The structural and luminescence properties of porous silicon
journal, August 1997

  • Cullis, A. G.; Canham, L. T.; Calcott, P. D. J.
  • Journal of Applied Physics, Vol. 82, Issue 3
  • DOI: 10.1063/1.366536

Structural evolution during electrocrystallization: deposition of Tl on Ag(100) from monolayer to bilayer and to bulk crystallites
journal, December 1995


Trends in electrocatalysis on extended and nanoscale Pt-bimetallic alloy surfaces
journal, February 2007

  • Stamenkovic, Vojislav R.; Mun, Bongjin Simon; Arenz, Matthias
  • Nature Materials, Vol. 6, Issue 3, p. 241-247
  • DOI: 10.1038/nmat1840

Nanofaceted Platinum Surfaces:  A New Model System for Nanoparticle Catalysts
journal, December 2005

  • Komanicky, Vladimir; Menzel, Andreas; Chang, Kee-Chul
  • The Journal of Physical Chemistry B, Vol. 109, Issue 49
  • DOI: 10.1021/jp0541516

One-dimensional commensurate-incommensurate transition: Bromide on the Au(100) electrode
journal, March 1996


The limits of macropore array fabrication
journal, April 1997


Coherent x-ray scattering experiments of Pt(001) surface dynamics near a roughening transition
journal, November 2012


Carbon monoxide adlayer structures on platinum (111) electrodes: A synergy between in‐situ scanning tunneling microscopy and infrared spectroscopy
journal, July 1994

  • Villegas, Ignacio; Weaver, Michael J.
  • The Journal of Chemical Physics, Vol. 101, Issue 2
  • DOI: 10.1063/1.467786

Ptychographic x-ray imaging of surfaces on crystal truncation rod
journal, March 2015

  • Zhu, Chenhui; Harder, Ross; Diaz, Ana
  • Applied Physics Letters, Vol. 106, Issue 10
  • DOI: 10.1063/1.4914927

Investigation of Oxygen Reduction Reaction Kinetics at (111)−(100) Nanofaceted Platinum Surfaces in Acidic Media
journal, December 2005

  • Komanicky, Vladimir; Menzel, Andreas; You, Hoydoo
  • The Journal of Physical Chemistry B, Vol. 109, Issue 49
  • DOI: 10.1021/jp054155a

Dealloying in Individual Nanoparticles and Thin Film Grains: A Bragg Coherent Diffractive Imaging Study
journal, May 2017

  • Cha, Wonsuk; Liu, Yihua; You, Hoydoo
  • Advanced Functional Materials, Vol. 27, Issue 25
  • DOI: 10.1002/adfm.201700331

Coherent X-ray diffraction imaging of strain at the nanoscale
journal, April 2009

  • Robinson, Ian; Harder, Ross
  • Nature Materials, Vol. 8, Issue 4
  • DOI: 10.1038/nmat2400

Epitaxial oxide bilayer on Pt (001) nanofacets
journal, January 2012

  • Hennessy, Daniel; Komanicky, Vladimir; Iddir, Hakim
  • The Journal of Chemical Physics, Vol. 136, Issue 4
  • DOI: 10.1063/1.3678858

Charge induced (1×3) reconstruction of the Au(110) surface: An x-ray scattering study
journal, December 1992


Angle calculations for a six-circle surface X-ray diffractometer
journal, October 1993


Surface X-Ray Speckles: Coherent Surface Diffraction from Au(001)
journal, October 2009


The in-situ preparation of well-defined, single crystal electrodes
journal, August 1987

  • Zurawski, D.; Rice, L.; Hourani, M.
  • Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 230, Issue 1-2
  • DOI: 10.1016/0022-0728(87)80144-4

Adsorbate-Geometry Specific Subsurface Relaxation in the CO/Pt(111) System
journal, January 2005

  • Wang, J. X.; Robinson, I. K.; Ocko, B. M.
  • The Journal of Physical Chemistry B, Vol. 109, Issue 1
  • DOI: 10.1021/jp045082i

Surface x-ray-scattering measurements of the substrate-induced spatial modulation of an incommensurate adsorbed monolayer
journal, September 1990

  • Toney, Michael F.; Gordon, Joseph G.; Samant, Mahesh G.
  • Physical Review B, Vol. 42, Issue 9
  • DOI: 10.1103/PhysRevB.42.5594

Applications of surface X-ray scattering to electrochemistry problems
journal, July 2002


Electrochemical Deposition of Copper on a Gold Electrode in Sulfuric Acid: Resolution of the Interfacial Structure
journal, December 1995


Structure-Activity-Stability Relationships of Pt−Co Alloy Electrocatalysts in Gas-Diffusion Electrode Layers
journal, February 2007

  • Koh, Shirlaine; Leisch, Jennifer; Toney, Michael F.
  • The Journal of Physical Chemistry C, Vol. 111, Issue 9
  • DOI: 10.1021/jp067269a

Angle calculations using two detector circles and wavelength
journal, July 2018


Charge-induced equilibrium dynamics and structure at the Ag(001)–electrolyte interface
journal, January 2015

  • Karl Jr., Robert M.; Barbour, Andi; Komanicky, Vladimir
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 26
  • DOI: 10.1039/C5CP02138C

X-ray and neutron scattering from rough surfaces
journal, August 1988


Double layer on silver single crystal electrodes in contact with electrolytes having anions which are slightly specifically adsorbed
journal, September 1989

  • Valette, Georges
  • Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 269, Issue 1
  • DOI: 10.1016/0022-0728(89)80112-3

Surface X-ray diffraction
journal, May 1992


Layering and Ordering in Electrochemical Double Layers
journal, February 2018

  • Liu, Yihua; Kawaguchi, Tomoya; Pierce, Michael S.
  • The Journal of Physical Chemistry Letters, Vol. 9, Issue 6
  • DOI: 10.1021/acs.jpclett.8b00123

X-ray-reflectivity study of the copper-water interface in a transmission geometry under in situ electrochemical control
journal, May 1992


Electrocatalytic activity of surface oxides on platinum nanofacets and surfaces
journal, October 2013


Kinetics of Oxygen Reduction on Pt(hkl) Electrodes: Implications for the Crystallite Size Effect with Supported Pt Electrocatalysts
journal, January 1997

  • Markovic, Nenad
  • Journal of The Electrochemical Society, Vol. 144, Issue 5
  • DOI: 10.1149/1.1837646

Angle calculations for a `4S+2D' six-circle diffractometer
journal, August 1999


Titanium oxide nanotube arrays prepared by anodic oxidation
journal, December 2001

  • Gong, Dawei; Grimes, Craig A.; Varghese, Oomman K.
  • Journal of Materials Research, Vol. 16, Issue 12
  • DOI: 10.1557/JMR.2001.0457

In Situ Surface X-Ray Scattering Observation of Long-Range Ordered ( 19 × 19 )R23.4°-13CO Structure on Pt(111) in Aqueous Electrolytes
journal, January 2004

  • Tolmachev, Yuriy V.; Menzel, Andreas; Tkachuk, Andrei V.
  • Electrochemical and Solid-State Letters, Vol. 7, Issue 3
  • DOI: 10.1149/1.1645354

Angle calculations for a five-circle diffractometer used for surface X-ray diffraction
journal, October 1987

  • Vlieg, E.; Van der Veen, J. F.; Macdonald, J. E.
  • Journal of Applied Crystallography, Vol. 20, Issue 5
  • DOI: 10.1107/S0021889887086527

Electrochemical, in-situ surface EXAFS and CTR studies of Co monolayers irreversibly adsorbed onto Pt(111)
journal, March 1999


A Study of the Hydration of the Alkali Metal Ions in Aqueous Solution
journal, December 2011

  • Mähler, Johan; Persson, Ingmar
  • Inorganic Chemistry, Vol. 51, Issue 1
  • DOI: 10.1021/ic2018693

High-Speed in situ Surface X-ray Diffraction Studies of the Electrochemical Dissolution of Au(001)
journal, March 2011

  • Golks, Frederik; Krug, Klaus; Gründer, Yvonne
  • Journal of the American Chemical Society, Vol. 133, Issue 11
  • DOI: 10.1021/ja1115748

The adsorption and oxidation of carbon monoxide at the Pt(111)/electrolyte interface: atomic structure and surface relaxation
journal, April 1999


Durability of De-Alloyed Platinum-Nickel Cathode Catalyst in Low Platinum Loading Membrane-Electrode Assemblies Subjected to Accelerated Stress Tests
journal, January 2018

  • Ahluwalia, R. K.; Wang, X.; Peng, J-K
  • Journal of The Electrochemical Society, Vol. 165, Issue 6
  • DOI: 10.1149/2.0341806jes

Lattice-strain control of the activity in dealloyed core–shell fuel cell catalysts
journal, April 2010

  • Strasser, Peter; Koh, Shirlaine; Anniyev, Toyli
  • Nature Chemistry, Vol. 2, Issue 6
  • DOI: 10.1038/nchem.623

Persistent oscillations of x-ray speckles: Pt (001) step flow
journal, September 2011

  • Pierce, M. S.; Hennessy, D. C.; Chang, K. C.
  • Applied Physics Letters, Vol. 99, Issue 12
  • DOI: 10.1063/1.3640227

Ex situ scanning tunneling microscopy study of under-potential oxidation of a Ag(111) electrode in an alkaline electrolyte
journal, March 2001

  • Shaikhutdinov, Sh. K.; Savinova, E. R.; Scheybal, A.
  • Journal of Electroanalytical Chemistry, Vol. 500, Issue 1-2
  • DOI: 10.1016/S0022-0728(00)00346-6

Study of electrode surface dynamics using coherent surface X-ray scattering
journal, November 2012


Bioceramics
journal, July 1998


LEED and voltammetry of carbon monoxide electrosorbed on platinum(111)
journal, March 1990

  • Zurawski, D.; Wasberg, M.; Wieckowski, Andrzej.
  • The Journal of Physical Chemistry, Vol. 94, Issue 5
  • DOI: 10.1021/j100368a064

Polarization-dependent resonant anomalous surface X-ray scattering of CO/Pt(111)
journal, June 2006


Pt Catalyst Degradation in Aqueous and Fuel Cell Environments studied via In-Operando Anomalous Small-Angle X-ray Scattering
journal, August 2015


The effects of anions on the underpotential deposition of Hg on Au(111) An electrochemical and in situ surface X-ray diffraction study
journal, March 1998

  • Li, Jun; Herrero, Enrique; Abruña, Héctor D.
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 134, Issue 1-2
  • DOI: 10.1016/S0927-7757(97)00341-5

Two-dimensional infrared photonic crystal based on macroporous silicon
journal, April 1996


In-Operando Anomalous Small-Angle X-Ray Scattering Investigation of Pt 3 Co Catalyst Degradation in Aqueous and Fuel Cell Environments
journal, January 2015

  • Gilbert, James A.; Kropf, A. Jeremy; Kariuki, Nancy N.
  • Journal of The Electrochemical Society, Vol. 162, Issue 14
  • DOI: 10.1149/2.0531514jes

Dealloying of Cu 3 Pt (111) Studied by Surface X-ray Scattering
journal, April 2011

  • Yang, Ruizhi; Strasser, Peter; Toney, Michael F.
  • The Journal of Physical Chemistry C, Vol. 115, Issue 18
  • DOI: 10.1021/jp111978m

Phase retrieval algorithms: a comparison
journal, January 1982


Activity–stability relationships of ordered and disordered alloy phases of Pt3Co electrocatalysts for the oxygen reduction reaction (ORR)
journal, February 2007


Resonance anomalous surface X-ray scattering
journal, November 2006


X-ray Scattering Study of Tl Adlayers on the Au(111) Electrode in Alkaline Solutions: Metal Monolayer, OH- Coadsorption, and Oxide Formation
journal, July 1994

  • Wang, Jia X.; Adzic, R. R.; Ocko, B. M.
  • The Journal of Physical Chemistry, Vol. 98, Issue 29
  • DOI: 10.1021/j100080a014

Shape-Dependent Activity of Platinum Array Catalyst
journal, April 2009

  • Komanicky, Vladimir; Iddir, Hakim; Chang, Kee-Chul
  • Journal of the American Chemical Society, Vol. 131, Issue 16
  • DOI: 10.1021/ja900459w

Structure of Tl Adlayers on the Pt(111) Electrode Surface:  Effects of Solution pH and Bisulfate Coadsorption
journal, January 1996

  • Adžić, R. R.; Wang, J. X.; Magnussen, O. M.
  • The Journal of Physical Chemistry, Vol. 100, Issue 35
  • DOI: 10.1021/jp960030h

Surface X-ray diffraction studies of single crystal electrocatalysts
journal, November 2016


In situ x-ray reflectivity and diffraction studies of the Au(001) reconstruction in an electrochemical cell
journal, September 1990


Diffraction anomalous fine structure: A new x-ray structural technique
journal, November 1992


In‐situ x‐ray reflectivity study of incipient oxidation of Pt(111) surface in electrolyte solutions
journal, March 1994

  • You, H.; Zurawski, D. J.; Nagy, Z.
  • The Journal of Chemical Physics, Vol. 100, Issue 6
  • DOI: 10.1063/1.466254

Voltage-dependent ordering of water molecules at an electrode–electrolyte interface
journal, March 1994

  • Toney, Michael F.; Howard, Jason N.; Richer, Jocelyn
  • Nature, Vol. 368, Issue 6470
  • DOI: 10.1038/368444a0

X-ray and Electrochemical Studies of Cu UPD on Au(111) Single-Crystal Electrodes in the Presence of Bromide
journal, December 1998

  • Herrero, Enrique; Glazier, Samantha; Abruña, Héctor D.
  • The Journal of Physical Chemistry B, Vol. 102, Issue 49
  • DOI: 10.1021/jp982192e