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

Title: Soft x-ray spectroscopy of high pressure liquid

Abstract

Here, we describe a new experimental technique that allows for soft x-ray spectroscopy studies (~100-1000 eV) of high pressure liquid (~100 bars). We achieve this through a liquid cell with a 100 nm-thick Si 3N 4 membrane window, which is sandwiched by two identical O-rings for vacuum sealing. The thin Si 3N 4 membrane allows soft x-rays to penetrate, while separating the high-pressure liquid under investigation from the vacuum required for soft x-ray transmission and detection. The burst pressure of the Si 3N 4 membrane increases with decreasing size and more specifically is inversely proportional to the side length of the square window. It also increases proportionally with the membrane thickness. Pressures > 60 bars could be achieved for 100 nm-thick square Si 3N 4 windows that are smaller than 65 μm. However, above a certain pressure, the failure of the Si wafer becomes the limiting factor. The failure pressure of the Si wafer is sensitive to the wafer thickness. Moreover, the deformation of the Si 3N 4 membrane is quantified using vertical scanning interferometry. As an example of the performance of the high-pressure liquid cell optimized for total-fluorescence detected soft x-ray absorption spectroscopy (sXAS), the sXAS spectra at themore » Ca L edge (~350 eV) of a CaCl 2 aqueous solution are collected under different pressures up to 41 bars.« less

Authors:
 [1];  [2];  [1];  [3];  [1];  [1];  [1]; ORCiD logo [4];  [4];  [5];  [4];  [1]; ORCiD logo [1];  [1];  [6];  [3]; ORCiD logo [1]
  1. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Soochow Univ., Jiangsu (China). Jiangsu Key Lab. for Carbon-Based Functional Materials and Devices, Inst. of Functional Nano and Soft Materials (FUNSOM) and Joint International Research Lab. of Carbon-Based Functional Materials and Devices
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Center for X-Ray Optic
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Geoscience Division
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Engineering Division
  6. Jiangsu Key Laboratory for Carbon-Based Functional Materials &, Devices, Institute of Functional Nano &, Soft Materials (FUNSOM), Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou 215123, Jiangsu, China
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1436167
Alternate Identifier(s):
OSTI ID: 1418709
Grant/Contract Number:
AC02-05CH11231; U1432249
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Review of Scientific Instruments
Additional Journal Information:
Journal Volume: 89; Journal Issue: 1; Journal ID: ISSN 0034-6748
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; materials properties; x-ray spectroscopy; semiconductors; etching; interferometry; light sensitive materials; chemical compounds; absorption spectra

Citation Formats

Qiao, Ruimin, Xia, Yujian, Feng, Xuefei, Macdougall, James, Pepper, John, Armitage, Kevin, Borsos, Jason, Knauss, Kevin G., Lee, Namhey, Allezy, Arnaud, Gilbert, Benjamin, MacDowell, Alastair A., Liu, Yi-Sheng, Glans, Per-Anders, Sun, Xuhui, Chao, Weilun, and Guo, Jinghua. Soft x-ray spectroscopy of high pressure liquid. United States: N. p., 2018. Web. doi:10.1063/1.5008444.
Qiao, Ruimin, Xia, Yujian, Feng, Xuefei, Macdougall, James, Pepper, John, Armitage, Kevin, Borsos, Jason, Knauss, Kevin G., Lee, Namhey, Allezy, Arnaud, Gilbert, Benjamin, MacDowell, Alastair A., Liu, Yi-Sheng, Glans, Per-Anders, Sun, Xuhui, Chao, Weilun, & Guo, Jinghua. Soft x-ray spectroscopy of high pressure liquid. United States. doi:10.1063/1.5008444.
Qiao, Ruimin, Xia, Yujian, Feng, Xuefei, Macdougall, James, Pepper, John, Armitage, Kevin, Borsos, Jason, Knauss, Kevin G., Lee, Namhey, Allezy, Arnaud, Gilbert, Benjamin, MacDowell, Alastair A., Liu, Yi-Sheng, Glans, Per-Anders, Sun, Xuhui, Chao, Weilun, and Guo, Jinghua. Mon . "Soft x-ray spectroscopy of high pressure liquid". United States. doi:10.1063/1.5008444.
@article{osti_1436167,
title = {Soft x-ray spectroscopy of high pressure liquid},
author = {Qiao, Ruimin and Xia, Yujian and Feng, Xuefei and Macdougall, James and Pepper, John and Armitage, Kevin and Borsos, Jason and Knauss, Kevin G. and Lee, Namhey and Allezy, Arnaud and Gilbert, Benjamin and MacDowell, Alastair A. and Liu, Yi-Sheng and Glans, Per-Anders and Sun, Xuhui and Chao, Weilun and Guo, Jinghua},
abstractNote = {Here, we describe a new experimental technique that allows for soft x-ray spectroscopy studies (~100-1000 eV) of high pressure liquid (~100 bars). We achieve this through a liquid cell with a 100 nm-thick Si3N4 membrane window, which is sandwiched by two identical O-rings for vacuum sealing. The thin Si3N4 membrane allows soft x-rays to penetrate, while separating the high-pressure liquid under investigation from the vacuum required for soft x-ray transmission and detection. The burst pressure of the Si3N4 membrane increases with decreasing size and more specifically is inversely proportional to the side length of the square window. It also increases proportionally with the membrane thickness. Pressures > 60 bars could be achieved for 100 nm-thick square Si3N4 windows that are smaller than 65 μm. However, above a certain pressure, the failure of the Si wafer becomes the limiting factor. The failure pressure of the Si wafer is sensitive to the wafer thickness. Moreover, the deformation of the Si3N4 membrane is quantified using vertical scanning interferometry. As an example of the performance of the high-pressure liquid cell optimized for total-fluorescence detected soft x-ray absorption spectroscopy (sXAS), the sXAS spectra at the Ca L edge (~350 eV) of a CaCl2 aqueous solution are collected under different pressures up to 41 bars.},
doi = {10.1063/1.5008444},
journal = {Review of Scientific Instruments},
number = 1,
volume = 89,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2018},
month = {Mon Jan 01 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on January 1, 2019
Publisher's Version of Record

Save / Share:
  • A high pressure in situ x-ray absorption spectroscopy cell with two different path lengths and path positions is presented for studying element-specifically both the liquid phase and the solid-liquid interface at pressures up to 250 bar and temperatures up to 220 deg. C. For this purpose, one x-ray path probes the bottom, while the other x-ray path penetrates through the middle of the in situ cell. The basic design of the cell resembles a 10 ml volume batch reactor, which is equipped with in- and outlet lines to dose compressed gases and liquids as well as a stirrer for goodmore » mixing. Due to the use of a polyetheretherketone inset it is also suitable for measurements under corrosive conditions. The characteristic features of the cell are illustrated using case studies from catalysis and solid state chemistry: (a) the ruthenium-catalyzed formylation of an amine in 'supercritical' carbon dioxide in the presence of hydrogen; (b) the cycloaddition of carbon dioxide to propylene oxide in the presence of a solid Zn-based catalyst, and (c) the solvothermal synthesis of MoO{sub 3} nanorods from MoO{sub 3}-2H{sub 2}O.« less
  • We report a methodology for a direct investigation of the solid/liquid interface using high pressure x-ray photoelectron spectroscopy (HPXPS). The technique was demonstrated with an electrochemical system represented by a Li-ion battery using a silicon electrode and a liquid electrolyte of LiClO{sub 4} in propylene carbonate (PC) cycled versus metallic lithium. For the first time the presence of a liquid electrolyte was realized using a transfer procedure where the sample was introduced into a 2 mbar N{sub 2} environment in the analysis chamber without an intermediate ultrahigh vacuum (UHV) step in the load lock. The procedure was characterized in detailmore » concerning lateral drop gradients as well as stability of measurement conditions over time. The X-ray photoelectron spectroscopy (XPS) measurements demonstrate that the solid substrate and the liquid electrolyte can be observed simultaneously. The results show that the solid electrolyte interphase (SEI) composition for the wet electrode is stable within the probing time and generally agrees well with traditional UHV studies. Since the methodology can easily be adjusted to various high pressure photoelectron spectroscopy systems, extending the approach towards operando solid/liquid interface studies using liquid electrolytes seems now feasible.« less
  • The authors present a table-top soft x-ray absorption spectrometer, accomplishing investigations of the near-edge x-ray absorption fine structure (NEXAFS) in a laboratory environment. The system is based on a low debris plasma ignited by a picosecond laser in a pulsed krypton gas jet, emitting soft x-ray radiation in the range from 1 to 5 nm. For absorption spectroscopy in and around the “water window” (2.3–4.4 nm), a compact helium purged sample compartment for experiments at atmospheric pressure has been constructed and tested. NEXAFS measurements on CaCl{sub 2} and KMnO{sub 4} samples were conducted at the calcium and manganese L-edges, as well asmore » at the oxygen K-edge in air, atmospheric helium, and under vacuum, respectively. The results indicate the importance of atmospheric conditions for an investigation of sample hydration processes.« less
  • We present a novel synchrotron endstation with a flow-through liquid cell designed to study the electronic structure of liquids using soft x-ray spectroscopies. In this cell, the liquid under study is separated from the vacuum by a thin window membrane, such that the sample liquid can be investigated at ambient pressure. The temperature of the probing volume can be varied in a broad range and with a fast temperature response. The optimized design of the cell significantly reduces the amount of required sample liquid and allows the use of different window membrane types necessary to cover a broad energy range.more » The liquid cell is integrated into the solid and liquid spectroscopic analysis SALSA endstation that includes a high-resolution, high-transmission x-ray spectrometer and a state-of-the-art electron analyzer. The modular design of SALSA also allows the measurement of solid-state samples. The capabilities of the liquid cell and the x-ray spectrometer are demonstrated using a resonant inelastic x-ray scattering map of a 25 wt percent NaOD solution.« less