Microfluidic electrochemical cell for in situ structural characterization of amorphous thin-film catalysts using high-energy X-ray scattering

Kwon, Gihan; Cho, Yeong-Ho; Kim, Ki-Bum; Emery, Jonathan D.; Kim, In Soo; Zhang, Xiaoyi; Martinson, Alex B. F.; Tiede, David M.

doi:10.1107/S1600577519007240

Title: Microfluidic electrochemical cell for in situ structural characterization of amorphous thin-film catalysts using high-energy X-ray scattering

Journal Article · Fri Aug 09 00:00:00 EDT 2019 · Journal of Synchrotron Radiation (Online)

DOI:https://doi.org/10.1107/S1600577519007240· OSTI ID:1617944

; Cho, Yeong-Ho; Kim, Ki-Bum;

; Kim, In Soo; Zhang, Xiaoyi; Martinson, Alex B. F.;

Porous, high-surface-area electrode architectures are described that allow structural characterization of interfacial amorphous thin films with high spatial resolution under device-relevant functional electrochemical conditions using high-energy X-ray (>50 keV) scattering and pair distribution function (PDF) analysis. Porous electrodes were fabricated from glass-capillary array membranes coated with conformal transparent conductive oxide layers, consisting of either a 40 nm–50 nm crystalline indium tin oxide or a 100 nm–150 nm-thick amorphous indium zinc oxide deposited by atomic layer deposition. These porous electrodes solve the problem of insufficient interaction volumes for catalyst thin films in two-dimensional working electrode designs and provide sufficiently low scattering backgrounds to enable high-resolution signal collection from interfacial thin-film catalysts. For example, PDF measurements were readily obtained with 0.2 Å spatial resolution for amorphous cobalt oxide films with thicknesses down to 60 nm when deposited on a porous electrode with 40 µm-diameter pores. This level of resolution resolves the cobaltate domain size and structure, the presence of defect sites assigned to the domain edges, and the changes in fine structure upon redox state change that are relevant to quantitative structure–function modeling. The results suggest the opportunity to leverage the porous, electrode architectures for PDF analysis of nanometre-scale surface-supported molecular catalysts. In addition, a compact 3D-printed electrochemical cell in a three-electrode configuration is described which is designed to allow for simultaneous X-ray transmission and electrolyte flow through the porous working electrode.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Light Energy Activated Redox Processes (LEAP); Argonne National Laboratory (ANL), Argonne, IL (United States)

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

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1617944

Alternate ID(s):: OSTI ID: 1575070

Journal Information:: Journal of Synchrotron Radiation (Online), Journal Name: Journal of Synchrotron Radiation (Online) Vol. 26 Journal Issue: 5; ISSN 1600-5775

Publisher:: International Union of Crystallography (IUCr)Copyright Statement

Country of Publication:: Denmark

Language:: English

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Cited by: 9 works

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References (53)

The Artificial Leaf Nocera, Daniel G. Accounts of Chemical Research, Vol. 45, Issue 5 https://doi.org/10.1021/ar2003013	journal	January 2012
Solution Structures of Highly Active Molecular Ir Water-Oxidation Catalysts from Density Functional Theory Combined with High-Energy X-ray Scattering and EXAFS Spectroscopy Yang, Ke R.; Matula, Adam J.; Kwon, Gihan Journal of the American Chemical Society, Vol. 138, Issue 17 https://doi.org/10.1021/jacs.6b01750	journal	April 2016
Oxyanion induced variations in domain structure for amorphous cobalt oxide oxygen evolving catalysts, resolved by X-ray pair distribution function analysis Kwon, Gihan; Kokhan, Oleksandr; Han, Ali Acta Crystallographica Section B Structural Science, Crystal Engineering and Materials, Vol. 71, Issue 6 https://doi.org/10.1107/S2052520615022180	journal	December 2015
Electrochemical Oxidation of Size-Selected Pt Nanoparticles Studied Using in Situ High-Energy-Resolution X-ray Absorption Spectroscopy Merte, Lindsay R.; Behafarid, Farzad; Miller, Daniel J. ACS Catalysis, Vol. 2, Issue 11 https://doi.org/10.1021/cs300494f	journal	September 2012
A flow cell for transient voltammetry and in situ grazing incidence X-ray diffraction characterization of electrocrystallized cadmium(II) tetracyanoquinodimethane Veder, Jean-Pierre; Nafady, Ayman; Clarke, Graeme Electrochimica Acta, Vol. 56, Issue 3 https://doi.org/10.1016/j.electacta.2010.09.106	journal	January 2011
Design of an electrochemical cell for in situ XAS studies Watanabe, N.; Morais, J.; Alves, M. C. M. Journal of Electron Spectroscopy and Related Phenomena, Vol. 156-158 https://doi.org/10.1016/j.elspec.2006.12.021	journal	May 2007
The Problem with Determining Atomic Structure at the Nanoscale Billinge, S. J. L.; Levin, I. Science, Vol. 316, Issue 5824 https://doi.org/10.1126/science.1135080	journal	April 2007
Demonstration of thin film pair distribution function analysis (tfPDF) for the study of local structure in amorphous and crystalline thin films Jensen, Kirsten M. Ø.; Blichfeld, Anders B.; Bauers, Sage R. IUCrJ, Vol. 2, Issue 5 https://doi.org/10.1107/S2052252515012221	journal	July 2015
Water Oxidation by Electrodeposited Cobalt Oxides-Role of Anions and Redox-Inert Cations in Structure and Function of the Amorphous Catalyst Risch, Marcel; Klingan, Katharina; Ringleb, Franziska ChemSusChem, Vol. 5, Issue 3 https://doi.org/10.1002/cssc.201100574	journal	February 2012
Characterization of an Amorphous Iridium Water-Oxidation Catalyst Electrodeposited from Organometallic Precursors Blakemore, James D.; Mara, Michael W.; Kushner-Lenhoff, Maxwell N. Inorganic Chemistry, Vol. 52, Issue 4 https://doi.org/10.1021/ic301968j	journal	January 2013
A transmission geometry electrochemical cell for in situ x‐ray diffraction Robinson, K. M.; O’Grady, W. E. Review of Scientific Instruments, Vol. 64, Issue 4 https://doi.org/10.1063/1.1144178	journal	April 1993
Best Practices for Operando Battery Experiments: Influences of X-ray Experiment Design on Observed Electrochemical Reactivity Borkiewicz, Olaf J.; Wiaderek, Kamila M.; Chupas, Peter J. The Journal of Physical Chemistry Letters, Vol. 6, Issue 11 https://doi.org/10.1021/acs.jpclett.5b00891	journal	May 2015
Structure of Active Adlayers on Bimetallic Surfaces: Oxygen Reduction on Au(111) with Bi Adlayers Tamura, K.; Ocko, B. M.; Wang, J. X. The Journal of Physical Chemistry B, Vol. 106, Issue 15 https://doi.org/10.1021/jp012960t	journal	April 2002
Electrochemical cell for in situ x-ray diffraction under ultrapure conditions Koop, Th.; Schindler, W.; Kazimirov, A. Review of Scientific Instruments, Vol. 69, Issue 4 https://doi.org/10.1063/1.1148852	journal	April 1998
Structure–function analyses of solar fuelscatalysts using in situ X-ray scattering Mulfort, Karen L.; Mukherjee, Anusree; Kokhan, Oleksandr Chem. Soc. Rev., Vol. 42, Issue 6 https://doi.org/10.1039/C2CS35247H	journal	January 2013
Heterogeneous Water Oxidation: Surface Activity versus Amorphization Activation in Cobalt Phosphate Catalysts González-Flores, Diego; Sánchez, Irene; Zaharieva, Ivelina Angewandte Chemie International Edition, Vol. 54, Issue 8 https://doi.org/10.1002/anie.201409333	journal	January 2015
Water oxidation by amorphous cobalt-based oxides: in situ tracking of redox transitions and mode of catalysis Risch, Marcel; Ringleb, Franziska; Kohlhoff, Mike Energy & Environmental Science, Vol. 8, Issue 2 https://doi.org/10.1039/C4EE03004D	journal	January 2015
In Situ Formation of an Oxygen-Evolving Catalyst in Neutral Water Containing Phosphate and Co²⁺ Kanan, M. W.; Nocera, D. G. Science, Vol. 321, Issue 5892, p. 1072-1075 https://doi.org/10.1126/science.1162018	journal	August 2008
Conformal Coating on Ultrahigh-Aspect-Ratio Nanopores of Anodic Alumina by Atomic Layer Deposition Elam, J. W.; Routkevitch, D.; Mardilovich, P. P. Chemistry of Materials, Vol. 15, Issue 18, p. 3507-3517 https://doi.org/10.1021/cm0303080	journal	September 2003
PDFgetX2: a GUI-driven program to obtain the pair distribution function from X-ray powder diffraction data Qiu, Xiangyun; Thompson, Jeroen W.; Billinge, Simon J. L. Journal of Applied Crystallography, Vol. 37, Issue 4, p. 678-678 https://doi.org/10.1107/S0021889804011744	journal	July 2004
Atomic Layer Deposition of In ₂ O ₃ Using Cyclopentadienyl Indium: A New Synthetic Route to Transparent Conducting Oxide Films Elam, Jeffrey W.; Martinson, Alex B. F.; Pellin, Michael J. Chemistry of Materials, Vol. 18, Issue 15 https://doi.org/10.1021/cm060754y	journal	July 2006
In situ x-ray-scattering study of the Au(001) reconstruction in alkaline and acidic electrolytes Tidswell, I. M.; Marković, N. M.; Lucas, C. A. Physical Review B, Vol. 47, Issue 24 https://doi.org/10.1103/PhysRevB.47.16542	journal	June 1993
Applications of an amorphous silicon-based area detector for high-resolution, high-sensitivity and fast time-resolved pair distribution function measurements Chupas, Peter J.; Chapman, Karena W.; Lee, Peter L. Journal of Applied Crystallography, Vol. 40, Issue 3 https://doi.org/10.1107/S0021889807007856	journal	May 2007
Comprehensive Insights into the Structural and Chemical Changes in Mixed-Anion FeOF Electrodes by Using Operando PDF and NMR Spectroscopy Wiaderek, Kamila M.; Borkiewicz, Olaf J.; Castillo-Martínez, Elizabeth Journal of the American Chemical Society, Vol. 135, Issue 10 https://doi.org/10.1021/ja400229v	journal	March 2013
Portable chamber for the study of UHV prepared electrochemical interfaces by hard x-ray diffraction Renner, Frank Uwe; Gründer, Yvonne; Zegenhagen, Jörg Review of Scientific Instruments, Vol. 78, Issue 3 https://doi.org/10.1063/1.2714046	journal	March 2007
Ab initio determination of solid-state nanostructure Juhás, P.; Cherba, D. M.; Duxbury, P. M. Nature, Vol. 440, Issue 7084 https://doi.org/10.1038/nature04556	journal	March 2006
Rapid-acquisition pair distribution function (RA-PDF) analysis Chupas, Peter J.; Qiu, Xiangyun; Hanson, Jonathan C. Journal of Applied Crystallography, Vol. 36, Issue 6, p. 1342-1347 https://doi.org/10.1107/S0021889803017564	journal	November 2003
Structure and Valency of a Cobalt−Phosphate Water Oxidation Catalyst Determined by in Situ X-ray Spectroscopy Kanan, Matthew W.; Yano, Junko; Surendranath, Yogesh Journal of the American Chemical Society, Vol. 132, Issue 39 https://doi.org/10.1021/ja1023767	journal	October 2010
Wireless Solar Water Splitting Using Silicon-Based Semiconductors and Earth-Abundant Catalysts Reece, S. Y.; Hamel, J. A.; Sung, K. Science, Vol. 334, Issue 6056 https://doi.org/10.1126/science.1209816	journal	September 2011
Water Oxidation by Amorphous Cobalt-Based Oxides: Volume Activity and Proton Transfer to Electrolyte Bases Klingan, Katharina; Ringleb, Franziska; Zaharieva, Ivelina ChemSusChem, Vol. 7, Issue 5 https://doi.org/10.1002/cssc.201301019	journal	January 2014
Mechanistic Studies of the Oxygen Evolution Reaction by a Cobalt-Phosphate Catalyst at Neutral pH Surendranath, Yogesh; Kanan, Matthew W.; Nocera, Daniel G. Journal of the American Chemical Society, Vol. 132, Issue 46 https://doi.org/10.1021/ja106102b	journal	November 2010
In situ X-ray absorption near edge structure studies of mechanisms of passivity Virtanen, S. Electrochimica Acta, Vol. 47, Issue 19 https://doi.org/10.1016/S0013-4686(02)00230-X	journal	July 2002
Intermediate-Range Structure of Self-Assembled Cobalt-Based Oxygen-Evolving Catalyst Farrow, Christopher L.; Bediako, D. Kwabena; Surendranath, Yogesh Journal of the American Chemical Society, Vol. 135, Issue 17 https://doi.org/10.1021/ja401276f	journal	April 2013
Atomic Layer Deposition of Indium Tin Oxide Thin Films Using Nonhalogenated Precursors Elam, Jeffrey W.; Baker, David A.; Martinson, Alex B. F. The Journal of Physical Chemistry C, Vol. 112, Issue 6 https://doi.org/10.1021/jp7097312	journal	February 2008
Time-resolved grazing-incidence pair distribution functions during deposition by radio-frequency magnetron sputtering Roelsgaard, Martin; Dippel, Ann-Christin; Borup, Kasper Andersen IUCrJ, Vol. 6, Issue 2 https://doi.org/10.1107/S2052252519001192	journal	February 2019
Electrolyte-Dependent Electrosynthesis and Activity of Cobalt-Based Water Oxidation Catalysts Surendranath, Yogesh; Dincǎ, Mircea; Nocera, Daniel G. Journal of the American Chemical Society, Vol. 131, Issue 7 https://doi.org/10.1021/ja807769r	journal	February 2009
In situ x-ray-diffraction and -reflectivity studies of the Au(111)/electrolyte interface: Reconstruction and anion adsorption Wang, Jia; Ocko, B. M.; Davenport, Alison J. Physical Review B, Vol. 46, Issue 16 https://doi.org/10.1103/PhysRevB.46.10321	journal	October 1992
Atomic layer deposition of tin oxide films using tetrakis(dimethylamino) tin Elam, Jeffrey W.; Baker, David A.; Hryn, Alexander J. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 26, Issue 2 https://doi.org/10.1116/1.2835087	journal	March 2008
In Situ Synchrotron X-ray Diffraction Experiments on Electrochemically Deposited ZnO Nanostructures Ingham, Bridget; Illy, Benoit N.; Toney, Michael F. The Journal of Physical Chemistry C, Vol. 112, Issue 38 https://doi.org/10.1021/jp806184z	journal	August 2008
Conduction and Reactivity in Heterogeneous-Molecular Catalysis: New Insights in Water Oxidation Catalysis by Phosphate Cobalt Oxide Films Costentin, Cyrille; Porter, Thomas R.; Savéant, Jean-Michel Journal of the American Chemical Society, Vol. 138, Issue 17 https://doi.org/10.1021/jacs.6b00737	journal	April 2016
Elucidating the Domain Structure of the Cobalt Oxide Water Splitting Catalyst by X-ray Pair Distribution Function Analysis Du, Pingwu; Kokhan, Oleksandr; Chapman, Karena W. Journal of the American Chemical Society, Vol. 134, Issue 27 https://doi.org/10.1021/ja303826a	journal	June 2012
The Structure of Ferrihydrite, a Nanocrystalline Material Michel, F. M.; Ehm, L.; Antao, S. M. Science, Vol. 316, Issue 5832 https://doi.org/10.1126/science.1142525	journal	June 2007
In situ x-ray reflectivity and diffraction studies of the Au(001) reconstruction in an electrochemical cell Ocko, B. M.; Wang, Jia; Davenport, Alison Physical Review Letters, Vol. 65, Issue 12 https://doi.org/10.1103/PhysRevLett.65.1466	journal	September 1990
Water splitting–biosynthetic system with CO ₂ reduction efficiencies exceeding photosynthesis Liu, Chong; Colón, Brendan C.; Ziesack, Marika Science, Vol. 352, Issue 6290 https://doi.org/10.1126/science.aaf5039	journal	June 2016
The AMPIX electrochemical cell: a versatile apparatus for in situ X-ray scattering and spectroscopic measurements Borkiewicz, Olaf J.; Shyam, Badri; Wiaderek, Kamila M. Journal of Applied Crystallography, Vol. 45, Issue 6 https://doi.org/10.1107/S0021889812042720	journal	November 2012
Electrochemical cells for in situ EXAFS Kordesch, M. E.; Hoffman, R. W. Nuclear Instruments and Methods in Physics Research, Vol. 222, Issue 1-2 https://doi.org/10.1016/0167-5087(84)90556-8	journal	May 1984
Ultrasmooth, High Electron Mobility Amorphous In–Zn–O Films Grown by Atomic Layer Deposition Lee, Do-Joong; Kwon, Jang-Yeon; Kim, Jiyeon The Journal of Physical Chemistry C, Vol. 118, Issue 1 https://doi.org/10.1021/jp409738f	journal	December 2013
Activity–Stability Trends for the Oxygen Evolution Reaction on Monometallic Oxides in Acidic Environments Danilovic, Nemanja; Subbaraman, Ramachandran; Chang, Kee-Chul The Journal of Physical Chemistry Letters, Vol. 5, Issue 14 https://doi.org/10.1021/jz501061n	journal	July 2014
In situ X-ray diffraction techniques as a powerful tool to study battery electrode materials Morcrette, M.; Chabre, Y.; Vaughan, G. Electrochimica Acta, Vol. 47, Issue 19 https://doi.org/10.1016/S0013-4686(02)00233-5	journal	July 2002
Efficient simultaneous reverse Monte Carlo modeling of pair-distribution functions and extended x-ray-absorption fine structure spectra of crystalline disordered materials Németh, Károly; Chapman, Karena W.; Balasubramanian, Mahalingam The Journal of Chemical Physics, Vol. 136, Issue 7 https://doi.org/10.1063/1.3684547	journal	February 2012
Elucidation of the Local and Long-Range Structural Changes that Occur in Germanium Anodes in Lithium-Ion Batteries Jung, Hyeyoung; Allan, Phoebe K.; Hu, Yan-Yan Chemistry of Materials, Vol. 27, Issue 3 https://doi.org/10.1021/cm504312x	journal	January 2015
Two-dimensional detector software: From real detector to idealised image or two-theta scan Hammersley, A. P.; Svensson, S. O.; Hanfland, M. High Pressure Research, Vol. 14, Issue 4-6, p. 235-248 https://doi.org/10.1080/08957959608201408	journal	January 1996
Application of high-energy X-rays and Pair-Distribution-Function analysis to nano-scale structural studies in catalysis Chupas, Peter J.; Chapman, Karena W.; Chen, Hailong Catalysis Today, Vol. 145, Issue 3-4 https://doi.org/10.1016/j.cattod.2009.03.026	journal	July 2009

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