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@PHDTHESIS{Duznovic:238311,
      author       = {Duznovic, Ivana},
      title        = {{I}on-conducting {N}anopores in {P}olymer {M}embranes for
                      ({B}io){M}olecular {S}ensory {A}pplications},
      school       = {Technische Universität Darmstadt},
      type         = {Dissertation},
      address      = {Darmstadt},
      publisher    = {Technische Universität Darmstadt},
      reportid     = {GSI-2021-00800},
      pages        = {XVIII, 179 Seiten},
      year         = {2021},
      note         = {Dissertation, Technische Universität Darmstadt, 2020},
      abstract     = {In the recent years, track-etched nanopores became the
                      major impulse in the development of nanofluidic biosensing
                      devices. The fabrication is processed first by bombarding
                      polymeric films with swift heavy ions. Subsequently, damaged
                      zones within the polymer membrane are created, which are
                      transformed into nanopores via chemical etching technique.
                      Here, pore geometry and diameter are controlled by selecting
                      a suitable chemical etchant and track-etching conditions.
                      As-prepared nanopores are cation selective due to the
                      presence of the ionized carboxylic acid moieties under
                      physiological conditions, which are generated as a
                      consequence of the ion-track etching process. The fixed
                      surface charge polarity and concomitant ion-selectivity of
                      nanopores is tuneable by the modification of native
                      carboxylic acid groups. Moreover, these groups are used to
                      attach desired receptors for biorecognition purpose through
                      specific ligand-receptor interactions. Surface modification
                      and biorecognition processes are monitored by measuring the
                      changes in the electric response of the nanopore via
                      current-voltage (IV) experiments. Regarding the design and
                      miniaturization of nanopore-based biosensing devices, this
                      thesis focusses on the three major challenges, which must be
                      taken into account to enable applications in real systems:
                      i) investigating the application of commercially available
                      nanopore membranes and biodegradable membranes as
                      alternative substrates for nanofluidic sensors. ii)
                      Examining innovative receptor-analyte moieties towards their
                      sensitive, selective and reproducible sensing performance.
                      Here, a variety of receptors and analytes are investigated
                      regarding the detection of metal cations, small molecules
                      (histamine) and biomacromolecules (proteins) as well as
                      polyelectrolytes. In case of metal cations, the selective
                      recognition of potassium ion is achieved by immobilizing
                      pseudo-crown ether-moieties on the pore surface. Moreover,
                      ultrasensitive subnanomolar Cu(II)-detection is obtained by
                      decorating nanopores with an amino-terminated copper and
                      nickel (ATCUN) motif. Both metal cations play crucial roles
                      within neuronal systems of living organisms. Hence,
                      monitoring of ion level is beneficial regarding diagnostic
                      applications. Further inflammatory indicators like histamine
                      are also successfully detected by the use of nanopore
                      membranes functionalized with Ni(II)-nitrilotriacetic acid
                      (NTA)-complexes. In Addition, LBL-deposition is achieved
                      inside nanopores through the electrostatic attraction
                      between poly(allylamine hydrochloride) and poly(acrylic
                      acid) with poly(4-vinylpyridine) (PVP) as a hydrogen-bond
                      compound. After the cross-linking of stacked
                      polyelectrolytes, the exposure to basic pH-conditions
                      triggered the PVP-release, leading to the formation of
                      porous networks in the nanopores as observed by changes in
                      the electrical readout and an increased mass transport
                      across the membrane. This represents the proof of concept
                      for the stimulated release of drugs. Moreover, the highly
                      selective and sensitive performance of pore-bounded camellia
                      nanobody-protein is successfully investigated, which are
                      single domain antibodies and, therefore, considered as
                      highly efficient detectors within immune systems. The used
                      nanobodies exhibit high affinity towards fluorescent
                      proteins (GFP and mCherry) as evidenced by IV-changes of
                      modified pore membranes and by CLSM-imaging methods. This
                      study demonstrates novel analyte detection using nanobody as
                      receptors on nanopore surfaces and to date receptor-analyte
                      interactions were performed in macro-sized setup, whose
                      implantation in real system is quite challenging due to
                      their sampling volumes of about 7 mL. Therefore, nanoporous
                      membranes were integrated in miniaturized Lab-on-Chips to
                      investigate the modification and sensing performance.
                      Further, the standard aqueous electrolyte used for
                      IV-measurements is exchanged by human serum to investigate
                      the IV-impact of a more complex medium on receptor-analyte
                      interactions across nanopore membranes.},
      cin          = {MAT},
      cid          = {I:(DE-Ds200)MAT-20051214OR025},
      pnm          = {6G15 - GSI-MML Ion Facilities (POF4-6G15) / FAIR Phase-0 -
                      FAIR Phase-0 Research Program (GSI-FAIR-Phase-0) / HGS-HIRe
                      - HGS-HIRe for FAIR (HGS-HIRe)},
      pid          = {G:(DE-HGF)POF4-6G15 / G:(Ds200)GSI-FAIR-Phase-0 /
                      G:(DE-Ds200)HGS-HIRe},
      experiment   = {$EXP:(DE-Ds200)UMat_M1;M2;M3-20200803$},
      typ          = {PUB:(DE-HGF)11},
      urn          = { 	urn:nbn:de:tuda-tuprints-140701},
      doi          = {10.26083/TUPRINTS-00014070},
      url          = {https://repository.gsi.de/record/238311},
}