Fast <i>operando</i> X-ray pair distribution function using the DRIX electrochemical cell

Diaz‐Lopez, Maria; Cutts, Geoffrey L.; Allan, Phoebe K.; Keeble, Dean S.; Ross, Allan M.; Raveau, B.; Spiekermann, Georg; Chater, Philip A.

doi:10.1107/s160057752000747x

Cited by 25 publications

(23 citation statements)

References 42 publications

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“…The angular aperture of transmission cells may however need to be extended when full patterns are required, such as for Pair Distribution Function (PDF) analysis but, as discussed in the next section, attenuation and shadowing by a flat window would be limiting the available angular range. For this reason, cells developed specifically for PDF usually use a different geometry with the incident beam normal to the cell axis, [42] rendering them no longer suitable for Bragg‐Brentano geometry.…”

Section: Resultsmentioning

confidence: 99%

Experimental Considerations for Operando Metal‐Ion Battery Monitoring using X‐ray Techniques

et al. 2021

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Operando experiments represent a powerful tool for the monitoring of internal processes upon battery cycling that provide valuable insights regarding the fundamental electrochemical redox mechanisms and ageing phenomena in battery materials. However, obtaining high-quality, representative and exploitable data from operando measurements requires careful control of many experimental parameters such as the cell configuration, the nature of the cell components, the electrode preparation approach, the optical/goniometer geometry, data acquisition protocols and data interpretation methodology. In this work we discuss the impact of all these factors in X-ray scattering and spectroscopic techniques based on experimental results obtained from different electrode materials using a multifunctional electrochemical in situ cell developed at our laboratory.

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Section: Resultsmentioning

confidence: 99%

Experimental Considerations for Operando Metal‐Ion Battery Monitoring using X‐ray Techniques

et al. 2021

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“…As mentioned above, the AMPIX cells are adopted widely for the in situ PDF of X‐ray total scatterings, and novel battery design includes diamond radial in situ X‐ray (DRIX) cell for fast operando data collection. [ 325 ] For the PDF of neutron scattering, the realization of in situ condition has rarely been reported. Since knowledge of light‐element dynamics (e.g., Li‐ion transportation, oxygen sublattice distortion, and so on) has not been clearly clarified for many battery materials, it is of great significance to develop an in situ neutron PDF technique for battery material investigations.…”

Section: Summary and Perspectivesmentioning

confidence: 99%

Bridging Structural Inhomogeneity to Functionality: Pair Distribution Function Methods for Functional Materials Development

et al. 2021

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The correlation between structure and function lies at the heart of materials science and engineering. Especially, modern functional materials usually contain inhomogeneities at an atomic level, endowing them with interesting properties regarding electrons, phonons, and magnetic moments. Over the past few decades, many of the key developments in functional materials have been driven by the rapid advances in short‐range crystallographic techniques. Among them, pair distribution function (PDF) technique, capable of utilizing the entire Bragg and diffuse scattering signals, stands out as a powerful tool for detecting local structure away from average. With the advent of synchrotron X‐rays, spallation neutrons, and advanced computing power, the PDF can quantitatively encode a local structure and in turn guide atomic‐scale engineering in the functional materials. Here, the PDF investigations in a range of functional materials are reviewed, including ferroelectrics/thermoelectrics, colossal magnetoresistance (CMR) magnets, high‐temperature superconductors (HTSC), quantum dots (QDs), nano‐catalysts, and energy storage materials, where the links between functions and structural inhomogeneities are prominent. For each application, a brief description of the structure‐function coupling will be given, followed by selected cases of PDF investigations. Before that, an overview of the theory, methodology, and unique power of the PDF method will be also presented.

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“…Local structure analysis has previously proven crucial in properly identifying structural features/distortions that underpin material behaviour in a wide variety of systems, be it determining local structure mechanisms of battery materials (Malavasi, 2011;Diaz-Lopez et al, 2020), defects in metalorganic frameworks (Cliffe et al, 2014;Coudert, 2015) or the nature of phase transitions in multiferroic materials (Gilioli & Ehm, 2014). Thus far, analogous experiments have not been possible for hydrostatic high-pressure neutron experiments, restricting exploration of local structure in crystalline materials to near-ambient pressure.…”

Section: Discussionmentioning

confidence: 99%

“…are designed such that non-sample scattering is reduced as much as possible. The only caveat is that, for generated PDFs to be physically meaningful, parasitic scattering arising from the sample environments must be accounted for by subtracting the scattering signature of the empty equipment (Saha et al, 2015;Sławin ´ski et al, 2019;Diaz-Lopez et al, 2020).…”

Section: Introductionmentioning

confidence: 99%

Recovering local structure information from high-pressure total scattering experiments

et al. 2021

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High pressure is a powerful thermodynamic tool for exploring the structure and the phase behaviour of the crystalline state, and is now widely used in conventional crystallographic measurements. High-pressure local structure measurements using neutron diffraction have, thus far, been limited by the presence of a strongly scattering, perdeuterated, pressure-transmitting medium (PTM), the signal from which contaminates the resulting pair distribution functions (PDFs). Here, a method is reported for subtracting the pairwise correlations of the commonly used 4:1 methanol:ethanol PTM from neutron PDFs obtained under hydrostatic compression. The method applies a molecular-dynamics-informed empirical correction and a non-negative matrix factorization algorithm to recover the PDF of the pure sample. Proof of principle is demonstrated, producing corrected high-pressure PDFs of simple crystalline materials, Ni and MgO, and benchmarking these against simulated data from the average structure. Finally, the first local structure determination of α-quartz under hydrostatic pressure is presented, extracting compression behaviour of the real-space structure.

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Fast operando X-ray pair distribution function using the DRIX electrochemical cell

Cited by 25 publications

References 42 publications

Experimental Considerations for Operando Metal‐Ion Battery Monitoring using X‐ray Techniques

Experimental Considerations for Operando Metal‐Ion Battery Monitoring using X‐ray Techniques

Bridging Structural Inhomogeneity to Functionality: Pair Distribution Function Methods for Functional Materials Development

Recovering local structure information from high-pressure total scattering experiments

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