skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Enabling liquid solvent structure analysis using hard x-ray absorption spectroscopy with a transferrable microfluidic reactor

Abstract

In this study, a vacuum compatible microfluidic device, system for analysis at the liquid vacuum interface, is integrated to hard x-ray absorption spectroscopy to obtain the local structure of K3[Fe(CN)6] in aqueous solutions with three concentrations of 0.5 M, 0.05 M, and 0.005 M. The solutions were sealed in a microchannel 500 µm wide and 300 µm deep in a portable microfluidic device. The Fe K-edge x-ray absorption spectra indicate a presence of Fe(III) in the complex in water, with an octahedral geometry coordinated with 6 C atoms in the first shell with a distance of ~1.92 Å and 6 N atoms in the second shell with a distance of ~3.10 Å. Varying the concentration has no observable influence on the structure of K3[Fe(CN)6]. Our results demonstrate the feasibility of using microfluidic based liquid cells in large synchrotron facilities. Using portable microfludic reactors provides a viable approach to enable multifaceted measurements of liquids in the future.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [2]; ORCiD logo [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1439303
Report Number(s):
BNL-205713-2018-JAAM
Journal ID: ISSN 0953-8984; TRN: US1900599
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physics. Condensed Matter
Additional Journal Information:
Journal Volume: 30; Journal Issue: 18; Journal ID: ISSN 0953-8984
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; x-ray absorption spectroscopy; SALVI; aqueous solution; solvation structure

Citation Formats

Zheng, Jian, Zhang, Wei, Wang, Feng, and Yu, Xiao -Ying. Enabling liquid solvent structure analysis using hard x-ray absorption spectroscopy with a transferrable microfluidic reactor. United States: N. p., 2018. Web. https://doi.org/10.1088/1361-648X/aab87f.
Zheng, Jian, Zhang, Wei, Wang, Feng, & Yu, Xiao -Ying. Enabling liquid solvent structure analysis using hard x-ray absorption spectroscopy with a transferrable microfluidic reactor. United States. https://doi.org/10.1088/1361-648X/aab87f
Zheng, Jian, Zhang, Wei, Wang, Feng, and Yu, Xiao -Ying. Wed . "Enabling liquid solvent structure analysis using hard x-ray absorption spectroscopy with a transferrable microfluidic reactor". United States. https://doi.org/10.1088/1361-648X/aab87f. https://www.osti.gov/servlets/purl/1439303.
@article{osti_1439303,
title = {Enabling liquid solvent structure analysis using hard x-ray absorption spectroscopy with a transferrable microfluidic reactor},
author = {Zheng, Jian and Zhang, Wei and Wang, Feng and Yu, Xiao -Ying},
abstractNote = {In this study, a vacuum compatible microfluidic device, system for analysis at the liquid vacuum interface, is integrated to hard x-ray absorption spectroscopy to obtain the local structure of K3[Fe(CN)6] in aqueous solutions with three concentrations of 0.5 M, 0.05 M, and 0.005 M. The solutions were sealed in a microchannel 500 µm wide and 300 µm deep in a portable microfluidic device. The Fe K-edge x-ray absorption spectra indicate a presence of Fe(III) in the complex in water, with an octahedral geometry coordinated with 6 C atoms in the first shell with a distance of ~1.92 Å and 6 N atoms in the second shell with a distance of ~3.10 Å. Varying the concentration has no observable influence on the structure of K3[Fe(CN)6]. Our results demonstrate the feasibility of using microfluidic based liquid cells in large synchrotron facilities. Using portable microfludic reactors provides a viable approach to enable multifaceted measurements of liquids in the future.},
doi = {10.1088/1361-648X/aab87f},
journal = {Journal of Physics. Condensed Matter},
number = 18,
volume = 30,
place = {United States},
year = {2018},
month = {4}
}

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

Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Prediction of Iron K-Edge Absorption Spectra Using Time-Dependent Density Functional Theory
journal, December 2008

  • DeBeer George, Serena; Petrenko, Taras; Neese, Frank
  • The Journal of Physical Chemistry A, Vol. 112, Issue 50
  • DOI: 10.1021/jp803174m

High‐pressure, capillary x‐ray absorption fine structure cell for studies of liquid and supercritical fluid solutions
journal, August 1996

  • Wallen, Scott L.; Pfund, David M.; Fulton, John L.
  • Review of Scientific Instruments, Vol. 67, Issue 8
  • DOI: 10.1063/1.1147115

Full Quantitative Multiple-Scattering Analysis of X-ray Absorption Spectra:  Application to Potassium Hexacyanoferrat(II) and -(III) Complexes
journal, December 2004

  • Hayakawa, Kuniko; Hatada, Keisuke; D'Angelo, Paola
  • Journal of the American Chemical Society, Vol. 126, Issue 47
  • DOI: 10.1021/ja045561v

Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal–Organic Framework
journal, July 2017

  • Ikuno, Takaaki; Zheng, Jian; Vjunov, Aleksei
  • Journal of the American Chemical Society, Vol. 139, Issue 30
  • DOI: 10.1021/jacs.7b02936

XAFS in dilute magnetic semiconductors
journal, January 2013

  • Sun, Zhihu; Yan, Wensheng; Yao, Tao
  • Dalton Transactions, Vol. 42, Issue 38
  • DOI: 10.1039/c3dt50888a

Resonant soft X-ray emission of solids and liquids
journal, January 2004


Performance of a microfluidic device for in situ ToF-SIMS analysis of selected organic molecules at aqueous surfaces
journal, January 2013

  • Yang, Li; Zhu, Zihua; Yu, Xiao-Ying
  • Analytical Methods, Vol. 5, Issue 10
  • DOI: 10.1039/c3ay26513g

Two coexisting liquid phases in switchable ionic liquids
journal, January 2017

  • Yao, Juan; Lao, David B.; Sui, Xiao
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 34
  • DOI: 10.1039/c7cp03754f

Photoelectron Spectroscopy at the Graphene-Liquid Interface Reveals the Electronic Structure of an Electrodeposited Cobalt/Graphene Electrocatalyst
journal, October 2015

  • Velasco-Velez, Juan J.; Pfeifer, Verena; Hävecker, Michael
  • Angewandte Chemie International Edition, Vol. 54, Issue 48
  • DOI: 10.1002/anie.201506044

Light at the interface: the potential of attenuated total reflection infrared spectroscopy for understanding heterogeneous catalysis in water
journal, January 2010

  • Mojet, Barbara Louise; Ebbesen, Sune Dalgaard; Lefferts, Leon
  • Chemical Society Reviews, Vol. 39, Issue 12
  • DOI: 10.1039/c0cs00014k

X-Ray Absorption Spectroscopy of TiO 2 Nanoparticles in Water Using a Holey Membrane-Based Flow Cell
journal, October 2017

  • Petit, Tristan; Ren, Jian; Choudhury, Sneha
  • Advanced Materials Interfaces, Vol. 4, Issue 23
  • DOI: 10.1002/admi.201700755

Photoinduced Ferrimagnetic Systems in Prussian Blue Analogues C I x Co 4 [Fe(CN) 6 ] y (C I = Alkali Cation). 1. Conditions to Observe the Phenomenon
journal, July 2000

  • Bleuzen, Anne; Lomenech, Claire; Escax, Virginie
  • Journal of the American Chemical Society, Vol. 122, Issue 28
  • DOI: 10.1021/ja000348u

Making a hybrid microfluidic platform compatible for in situ imaging by vacuum-based techniques
journal, November 2011

  • Yang, Li; Yu, Xiao-Ying; Zhu, Zihua
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 29, Issue 6
  • DOI: 10.1116/1.3654147

Imaging liquids using microfluidic cells
journal, May 2013


GNXAS, A Multiple-Scattering Approach to EXAFS Analysis: Methodology and Applications to Iron Complexes
journal, February 1995

  • Westre, Tami E.; Di Cicco, Andrea; Filipponi, Adriano
  • Journal of the American Chemical Society, Vol. 117, Issue 5
  • DOI: 10.1021/ja00110a012

Solid and liquid spectroscopic analysis (SALSA)–a soft x-ray spectroscopy endstation with a novel flow-through liquid cell
journal, December 2009

  • Blum, M.; Weinhardt, L.; Fuchs, O.
  • Review of Scientific Instruments, Vol. 80, Issue 12
  • DOI: 10.1063/1.3257926

In situ chemical probing of the electrode–electrolyte interface by ToF-SIMS
journal, January 2014

  • Liu, Bingwen; Yu, Xiao-Ying; Zhu, Zihua
  • Lab Chip, Vol. 14, Issue 5
  • DOI: 10.1039/c3lc50971k

Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes
journal, June 2015

  • Li, Y.; Zakharov, D.; Zhao, S.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8583

X-Ray Emission Spectroscopy of Hydrogen Bonding and Electronic Structure of Liquid Water
journal, September 2002


In Situ Molecular Imaging of the Biofilm and Its Matrix
journal, October 2016


Probing liquid surfaces under vacuum using SEM and ToF-SIMS
journal, January 2011

  • Yang, Li; Yu, Xiao-Ying; Zhu, Zihua
  • Lab on a Chip, Vol. 11, Issue 15
  • DOI: 10.1039/c0lc00676a

Understanding the Effects of Concentration on the Solvation Structure of Ca 2+ in Aqueous Solution. I:  The Perspective on Local Structure from EXAFS and XANES
journal, June 2003

  • Fulton, John L.; Heald, Steve M.; Badyal, Yaspal S.
  • The Journal of Physical Chemistry A, Vol. 107, Issue 23
  • DOI: 10.1021/jp0272264

Chemical imaging of molecular changes in a hydrated single cell by dynamic secondary ion mass spectrometry and super-resolution microscopy
journal, April 2016

  • Hua, Xin; Szymanski, Craig; Wang, Zhaoying
  • Integrative Biology, Vol. 8, Issue 5
  • DOI: 10.1039/c5ib00308c

Hard X-rays QEXAFS instrumentation with scan range 20 to 4000eV
journal, September 2011

  • Khalid, S.; Ehrlich, S. N.; Lenhard, A.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 649, Issue 1
  • DOI: 10.1016/j.nima.2010.11.074

Concentration dependence of EXAFS and XANES of copper(II) perchlorate aqueous solution: comparison of solute structure in liquid and glassy states
journal, October 1988

  • Nomura, Masaharu; Yamaguchi, Toshio
  • The Journal of Physical Chemistry, Vol. 92, Issue 21
  • DOI: 10.1021/j100332a061

Graphene oxide windows for in situ environmental cell photoelectron spectroscopy
journal, August 2011

  • Kolmakov, Andrei; Dikin, Dmitriy A.; Cote, Laura J.
  • Nature Nanotechnology, Vol. 6, Issue 10
  • DOI: 10.1038/nnano.2011.130

In situ nuclear magnetic resonance microimaging of live biofilms in a microchannel
journal, January 2017

  • Renslow, R. S.; Marshall, M. J.; Tucker, A. E.
  • The Analyst, Vol. 142, Issue 13
  • DOI: 10.1039/c7an00078b

Deciphering the aqueous chemistry of glyoxal oxidation with hydrogen peroxide using molecular imaging
journal, January 2017

  • Sui, Xiao; Zhou, Yufan; Zhang, Fei
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 31
  • DOI: 10.1039/c7cp02071f

X-ray Spectroscopic Study of Solvent Effects on the Ferrous and Ferric Hexacyanide Anions
journal, September 2014

  • Penfold, T. J.; Reinhard, M.; Rittmann-Frank, M. H.
  • The Journal of Physical Chemistry A, Vol. 118, Issue 40
  • DOI: 10.1021/jp5055588

Liquid EXAFS cells for measurements in transmission and fluorescence mode of corrosive samples
journal, June 1994

  • Marcos, Enrique Sánchez; Gil, Manuel; Martínez, José M.
  • Review of Scientific Instruments, Vol. 65, Issue 6
  • DOI: 10.1063/1.1144718

Sailing into uncharted waters: recent advances in the in situ monitoring of catalytic processes in aqueous environments
journal, January 2015

  • Shi, Hui; Lercher, Johannes A.; Yu, Xiao-Ying
  • Catalysis Science & Technology, Vol. 5, Issue 6
  • DOI: 10.1039/c4cy01720j

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005


Sailing into uncharted waters: recent advances in the in situ monitoring of catalytic processes in aqueous environments
journal, January 2015

  • Shi, Hui; Lercher, Johannes A.; Yu, Xiao-Ying
  • Catalysis Science & Technology, Vol. 5, Issue 6
  • DOI: 10.1039/C4CY01720J

Chemical imaging of molecular changes in a hydrated single cell by dynamic secondary ion mass spectrometry and super-resolution microscopy
journal, April 2016

  • Hua, Xin; Szymanski, Craig; Wang, Zhaoying
  • Integrative Biology, Vol. 8, Issue 5
  • DOI: 10.1039/C5IB00308C

In situ nuclear magnetic resonance microimaging of live biofilms in a microchannel
journal, January 2017

  • Renslow, R. S.; Marshall, M. J.; Tucker, A. E.
  • The Analyst, Vol. 142, Issue 13
  • DOI: 10.1039/C7AN00078B

In situ chemical probing of the electrode–electrolyte interface by ToF-SIMS
journal, January 2014

  • Liu, Bingwen; Yu, Xiao-Ying; Zhu, Zihua
  • Lab Chip, Vol. 14, Issue 5
  • DOI: 10.1039/C3LC50971K

Two coexisting liquid phases in switchable ionic liquids
journal, January 2017

  • Yao, Juan; Lao, David B.; Sui, Xiao
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 34
  • DOI: 10.1039/C7CP03754F

Deciphering the aqueous chemistry of glyoxal oxidation with hydrogen peroxide using molecular imaging
journal, January 2017

  • Sui, Xiao; Zhou, Yufan; Zhang, Fei
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 31
  • DOI: 10.1039/C7CP02071F

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005


X-Ray Emission Spectroscopy of Hydrogen Bonding and Electronic Structure of Liquid Water
journal, September 2002


Resonant soft X-ray emission of solids and liquids
journal, January 2004