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@PHDTHESIS{Seyffertitz:630678,
author = {Seyffertitz, Malina},
title = {{S}upercapacitors with {A}queous {E}lectrolytes: {W}hat
{C}an {W}e {L}earn from {I}n-{S}itu and {O}perando
{S}ynchrotron and {N}eutron {T}echniques?},
school = {Montanuniversität Leoben},
type = {Dissertation},
reportid = {PUBDB-2025-01898},
pages = {217},
year = {2025},
note = {Dissertation, Montanuniversität Leoben, 2025},
abstract = {This thesis investigates the fundamental processes
governing supercapacitors with aqueous electrolytes through
the development and application of in-situ and operando
synchrotronand neutron techniques. Using a suite of
complementary methods, including X-ray Transmission (XRT),
X-ray Fluorescence (XRF), (Anomalous) Small-Angle X-ray
Scattering ((A)SAXS), Small-Angle Neutron Scattering (SANS),
X-ray Diffraction (XRD), and Neutron Diffraction (ND), a
detailed experimental framework is established to probe
supercapacitor behaviour under working conditions. The work
focuses on experimentally accessing and interpreting the
following aspects of supercapacitor operation: (1) ion and
solvent concentration changes and charge-balancing
mechanisms, (2) structural changes in the electrode during
operation, (3) wetting effects, (4) local ion and solvent
(re-)arrangement, (5) charging dynamics, (6) atomic-scale
interactions via pair distribution functions, and (7) the
influence of electrode geometry and cell design. These
phenomena are explored in detail for two electrochemical
systems: MSP-20X activated carbon electrodes with 1 M RbBr
(aq.) electrolyte, and Ni3(HITP)2 conductive metal-organic
framework electrodes with 1 M NaTFSI (aq.) electrolyte. For
both, tailored experimentalapproaches are developed and
critically assessed. While this thesis provides a practical
framework for applying in-situ and operando synchrotron and
neutron techniques to electrochemical systems, its central
contribution lies in the insights it offers into electric
double-layer formation and ion and solvent behavior in
supercapacitors under operating conditions. By revealing how
a range of interconnected processes unfold during charging
and discharging, these findings offer a comprehensive and
nuanced understanding of how supercapacitors function and
how their performance might be more effectively tailored in
the future.},
cin = {FS DOOR-User},
cid = {$I:(DE-H253)FS_DOOR-User-20241023$},
pnm = {6G3 - PETRA III (DESY) (POF4-6G3) / FS-Proposal: I-20220173
EC (I-20220173-EC) / FS-Proposal: I-20230206 EC
(I-20230206-EC)},
pid = {G:(DE-HGF)POF4-6G3 / G:(DE-H253)I-20220173-EC /
G:(DE-H253)I-20230206-EC},
experiment = {EXP:(DE-H253)P-P62-20221101},
typ = {PUB:(DE-HGF)11},
url = {https://bib-pubdb1.desy.de/record/630678},
}