scholarly journals Full Energy Range Resonant Inelastic X-Ray Scattering of O2 and CO2: Direct Comparison with Oxygen Redox State in Batteries

2019 ◽  
Author(s):  
Zengqing Zhuo ◽  
Yi-Sheng Liu ◽  
Jinghua Guo ◽  
Yi-de Chuang ◽  
Feng Pan ◽  
...  
Keyword(s):  
Energy Range ◽  
High Efficiency ◽  
Full Range ◽  
Molecular Configuration ◽  
X Ray ◽  
Full Energy ◽  
Oxide Electrodes ◽  
X Ray Scattering ◽  
Oxygen State ◽  
Ray Scattering

The varying oxygen state plays key roles in the performance and stability of various electrochemical systems. However, the nature of the non-divalent state remains elusive with speculations under active debates. A direct comparison between these unconventional states on their full oxygen spectroscopic profile is critical but remains missing. Here, high-efficiency full energy range O-K mapping of resonant inelastic x-ray scattering (mRIXS) was collected from O<sub>2</sub> (O<sup>0</sup>) and CO<sub>2</sub> (O<sup>2-</sup>) gas molecules. The results are compared directly with Li<sub>2</sub>O<sub>2</sub> (O<sup>1-</sup>) and more importantly, the oxidized oxygen (O<sup>n-</sup>, 0-n-2) state in representative Na-ion and Li-ion battery electrodes. All the mRIXS features of O<sub>2</sub> and CO<sub>2</sub> are interpreted, and we focus on the contrasts of two characteristic features among all oxidized oxygen species, especially on the striking 523.7 eV emission feature. The full mRIXS profile reveals that oxygen redox states in batteries have distinct distributions along the excitation energy compared with Li<sub>2</sub>O<sub>2</sub> and O<sub>2</sub>. This work provides not only the first full range mRIXS results of O<sub>2</sub> and CO<sub>2</sub>, but also the direct comparison of four different oxygen states, i.e., O<sup>2-</sup>, O<sup>1-</sup>, O<sup>n-</sup>(0-n-2), and O<sup>0</sup>. Our results indicate that the nature of the oxidized oxygen state in oxide electrodes is beyond a simple molecular configuration of either peroxide or O<sub>2</sub>.

scholarly journals Full Energy Range Resonant Inelastic X-Ray Scattering of O2 and CO2: Direct Comparison with Oxygen Redox State in Batteries

2019 ◽  
Author(s):  
Zengqing Zhuo ◽  
Yi-Sheng Liu ◽  
Jinghua Guo ◽  
Yi-de Chuang ◽  
Feng Pan ◽  
...  
Keyword(s):  
Energy Range ◽  
High Efficiency ◽  
Full Range ◽  
Molecular Configuration ◽  
X Ray ◽  
Full Energy ◽  
Oxide Electrodes ◽  
X Ray Scattering ◽  
Oxygen State ◽  
Ray Scattering

The varying oxygen state plays key roles in the performance and stability of various electrochemical systems. However, the nature of the non-divalent state remains elusive with speculations under active debates. A direct comparison between these unconventional states on their full oxygen spectroscopic profile is critical but remains missing. Here, high-efficiency full energy range O-K mapping of resonant inelastic x-ray scattering (mRIXS) was collected from O<sub>2</sub> (O<sup>0</sup>) and CO<sub>2</sub> (O<sup>2-</sup>) gas molecules. The results are compared directly with Li<sub>2</sub>O<sub>2</sub> (O<sup>1-</sup>) and more importantly, the oxidized oxygen (O<sup>n-</sup>, 0-n-2) state in representative Na-ion and Li-ion battery electrodes. All the mRIXS features of O<sub>2</sub> and CO<sub>2</sub> are interpreted, and we focus on the contrasts of two characteristic features among all oxidized oxygen species, especially on the striking 523.7 eV emission feature. The full mRIXS profile reveals that oxygen redox states in batteries have distinct distributions along the excitation energy compared with Li<sub>2</sub>O<sub>2</sub> and O<sub>2</sub>. This work provides not only the first full range mRIXS results of O<sub>2</sub> and CO<sub>2</sub>, but also the direct comparison of four different oxygen states, i.e., O<sup>2-</sup>, O<sup>1-</sup>, O<sup>n-</sup>(0-n-2), and O<sup>0</sup>. Our results indicate that the nature of the oxidized oxygen state in oxide electrodes is beyond a simple molecular configuration of either peroxide or O<sub>2</sub>.

scholarly journals Fingerprint Oxygen Redox Reactions in Batteries through High-Efficiency Mapping of Resonant Inelastic X-ray Scattering

2019 ◽  
Vol 4 (1) ◽  
pp. 5 ◽  
Author(s):  
Jinpeng Wu ◽  
Qinghao Li ◽  
Shawn Sallis ◽  
Zengqing Zhuo ◽  
William E. Gent ◽  
...  
Keyword(s):  
Redox Reactions ◽  
High Efficiency ◽  
Full Range ◽  
Oxygen Absorption ◽  
Battery Materials ◽  
X Ray ◽  
X Ray Scattering ◽  
Electrochemical Cycling ◽  
Energy And Power Density ◽  
Ray Scattering

Realizing reversible reduction-oxidation (redox) reactions of lattice oxygen in batteries is a promising way to improve the energy and power density. However, conventional oxygen absorption spectroscopy fails to distinguish the critical oxygen chemistry in oxide-based battery electrodes. Therefore, high-efficiency full-range mapping of resonant inelastic X-ray scattering (mRIXS) has been developed as a reliable probe of oxygen redox reactions. Here, based on mRIXS results collected from a series of Li1.17Ni0.21Co0.08Mn0.54O2 electrodes at different electrochemical states and its comparison with peroxides, we provide a comprehensive analysis of five components observed in the mRIXS results. While all the five components evolve upon electrochemical cycling, only two of them correspond to the critical states associated with oxygen redox reactions. One is a specific feature at 531.0 eV excitation and 523.7 eV emission energy, the other is a low-energy loss feature. We show that both features evolve with electrochemical cycling of Li1.17Ni0.21Co0.08Mn0.54O2 electrodes, and could be used for characterizing oxidized oxygen states in the lattice of battery electrodes. This work provides an important benchmark for a complete assignment of all mRIXS features collected from battery materials, which sets a general foundation for future studies in characterization, analysis, and theoretical calculation for probing and understanding oxygen redox reactions.

scholarly journals Full Energy Range Resonant Inelastic X-ray Scattering of O2 and CO2: Direct Comparison with Oxygen Redox State in Batteries

2020 ◽  
Vol 11 (7) ◽  
pp. 2618-2623 ◽  
Author(s):  
Zengqing Zhuo ◽  
Yi-sheng Liu ◽  
Jinghua Guo ◽  
Yi-de Chuang ◽  
Feng Pan ◽  
...  
Keyword(s):  
Energy Range ◽  
Redox State ◽  
X Ray ◽  
Full Energy ◽  
X Ray Scattering ◽  
Ray Scattering

scholarly journals Supramolecular Dimerization in a Polymer Melt from Small-Angle X-ray Scattering and Rheology: A Miscible Model System

Polymers ◽  
2020 ◽  
Vol 12 (4) ◽  
pp. 880
Author(s):  
Mariapaola Staropoli ◽  
Margarita Kruteva ◽  
Jürgen Allgaier ◽  
Andreas Wischnewski ◽  
Wim Pyckhout-Hintzen
Keyword(s):  
Hydrogen Bonding ◽  
Small Angle ◽  
Full Range ◽  
Polymer Melt ◽  
Self Healing ◽  
Temperature Dependent ◽  
Base Pairs ◽  
X Ray ◽  
X Ray Scattering ◽  
Ray Scattering

We present a structural and dynamic study on the simplest supramolecular hetero-association, recently investigated by the authors to prepare architectural homogeneous structures in the melt state, based on the bio-inspired hydrogen-bonding of thymine/diaminotriazine (thy–DAT) base-pairs. In the combination with an amorphous low Tg poly(butylene oxide) (PBO), no micellar structures are formed, which is expected for nonpolar polymers because of noncompatibility with the highly polar supramolecular groups. Instead, a clear polymer-like transient architecture is retrieved. This makes the heterocomplementary thy–DAT association an ideal candidate for further exploitation of the hydrogen-bonding ability in the bulk for self-healing purposes, damage management in rubbers or even the development of easily processable branched polymers with built-in plasticizer. In the present work, we investigate the temperature range from Tg + 20 °C to Tg + 150 °C of an oligomeric PBO using small-angle X-ray scattering (SAXS) and linear rheology on the pure thy and pure DAT monofunctionals and on an equimolar mixture of thy/DAT oligomers. The linear rheology performed at low temperature is found to correspond to fully closed-state dimeric configurations. At intermediate temperatures, SAXS probes the equilibrium between open and closed states of the thy–DAT mixtures. The temperature-dependent association constant in the full range between open and closed H-bonds and an enhancement of the monomeric friction coefficient due to the groups is obtained. The thy–DAT association in the melt is more stable than the DAT–DAT, whereas the thy–thy association seems to involve additional long-lived interactions.

scholarly journals Advances in soft X-ray RIXS for studying redox reaction states in batteries

2020 ◽  
Vol 49 (39) ◽  
pp. 13519-13527
Author(s):  
Jue Wu ◽  
Yong Yang ◽  
Wanli Yang
Keyword(s):  
Redox Reaction ◽  
High Efficiency ◽  
X Ray ◽  
Redox States ◽  
X Ray Scattering ◽  
Ray Scattering

High-efficiency mapping of resonant inelastic X-ray scattering (mRIXS) for detecting and quantifying both cationic and anionic redox states in batteries.

An endstation for resonant inelastic X-ray scattering studies of solid and liquid samples

2017 ◽  
Vol 24 (1) ◽  
pp. 302-306 ◽  
Author(s):  
Zhong Yin ◽  
Hans-Bernhard Peters ◽  
Ulrich Hahn ◽  
Josef Gonschior ◽  
Daniel Mierwaldt ◽  
...  
Keyword(s):  
Energy Range ◽  
Electronic Configuration ◽  
Resolving Power ◽  
Liquid Jet ◽  
X Ray ◽  
X Ray Scattering ◽  
Liquid Samples ◽  
Sample Chamber ◽  
High Flexibility ◽  
Ray Scattering

A novel experimental setup is presented for resonant inelastic X-ray scattering investigations of solid and liquid samples in the soft X-ray region for studying the complex electronic configuration of (bio)chemical systems. The uniqueness of the apparatus is its high flexibility combined with optimal energy resolution and energy range ratio. The apparatus enables investigation of chemical analyses, which reflects the chemical imprints. The endstation is composed of a main sample chamber, a sample holder for either solid or liquid jet delivery system, and a soft X-ray grating spectrometer for 210–1250 eV with a resolving power of ∼1000. It combines for the first time liquid jet technology with a soft X-ray spectrometer based on the variable line spacing principle. This setup was commissioned at the soft X-ray beamline P04 at PETRA III of the Deutsches Elektronen-Synchrotron in Hamburg which is currently the most brilliant storage-ring-based X-ray radiation source in the world. The first results of liquid and solid samples show that this setup allows the detection of photons across an energy range of ∼300 eV. This covers simultaneously the emission lines of life-important elements like carbon, nitrogen and oxygen in a shot-based procedure.

Pore Morphology Study of Silica Aerogels

1994 ◽  
Vol 346 ◽  
Author(s):  
D.W. Hua ◽  
J. Anderson ◽  
S. Hæreid ◽  
D.M. Smith ◽  
G. Beaucage
Keyword(s):  
Light Scattering ◽  
Pore Size ◽  
Small Angle ◽  
High Efficiency ◽  
Silica Aerogels ◽  
X Ray ◽  
X Ray Scattering ◽  
Small Angle Light Scattering ◽  
Matching Criteria ◽  
Ray Scattering

ABSTRACTSilica aerogels have numerous properties which suggest applications such as ultra high efficiency thermal insulation. These properties relate directly to the aerogel's pore size distribution. The micro and meso pore size ranges can be investigated by normal small angle x-ray scattering and possibly, nitrogen adsorption. However, the measurement of larger pores (> 250 Å) is more difficult. Due to their limited mechanical strength, mercury porosimetry and nitrogen condensation can disrupt the gel structure and electron microscopy provides only limited large scale structure information. The use of small angle light scattering techniques seems to have promise, the only hurdle is that aerogels exhibit significant multiple scattering. This can be avoided if one observes the gels in the wet stage since the structure of the aerogel should be very similar to the wet gel (as the result of supercritical drying). Thus, if one can match the refractive index, the morphology can be probed. The combination of certain alcoholic solvents fit this index matching criteria. Preliminary results for the gel network (micron range) and primary particle structure (nanometer) are reported by using small angle light scattering and ultra-small angle x-ray scattering. The effects on structure over the length scale range of <1 nm to >5 μπι under different conditions (precursors, pH, etc.) are presented. The change in structure of an aerogel during isostatic compaction to 228 MPa (to simulate drying from wetting solvents) are also discussed.

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