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EPR and speciation simulation study of Cu2+ complexes in an amine-based aqueous precursor system used for preparation of superconducting YBCO coatings

Petra Lommens (UGent) , Jonas Feys (UGent) , Henk Vrielinck (UGent) , Klaartje De Buysser (UGent) , Gerrit Herman (UGent) , Freddy Callens (UGent) and Isabel Van Driessche (UGent)
(2012) DALTON TRANSACTIONS. 41(12). p.3574-3582
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Abstract
In this work, we investigate the chemistry for an aqueous acetate-triethanolamine-ammonia based YBa2Cu3O7-d (YBCO) precursor system. These precursor solutions are suited for the chemical solution deposition of superconducting YBCO layers on top of single crystal SrTiO3 or buffered NiW tapes. The development of this kind of precursor inks often involves trial-and-error experimenting and thus is very time-consuming. To reduce labwork to the minimum, the theoretical prediction of pH stability limits and the complexation behaviour of the different metal ions and complexants in the inks are very important. For this purpose, we simulated, based on literature values, the complexation behaviour of Cu2+ in the aqueous precursor solutions as a function of pH. To validate the used model, we performed potentiometric pH titrations for solutions with similar composition and checked the correctness of fit between experiment and model. The generated complexometric results are coupled with X-band EPR spectra to further confirm the results. EPR spectra for fully prepared precursor solutions as well as for Cu2+ reference solutions containing only one type of ligand (acetate, triethanolamine or ammonia) were investigated as a function of pH. We find that, in line with speciation simulation, only acetates are actively complexing the Cu2+ ions at pH values below 7, while when reaching higher pH levels mainly triethanolamine complexes are formed. Over the entire pH range, no trace of free Cu2+ or Cu(OH)(2), possibly creating precipitation during gelation and thus complicating further processing, could be found.
Keywords
THIN-FILMS, ELECTRON-PARAMAGNETIC RESONANCE, SOLUTION DEPOSITION, COATED CONDUCTORS, BUFFER LAYERS, COPPER(II), YBA2CU3O7-DELTA, METAL, ION, SPECTRA

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Chicago
Lommens, Petra, Jonas Feys, Henk Vrielinck, Klaartje De Buysser, Gerrit Herman, Freddy Callens, and Isabel Van Driessche. 2012. “EPR and Speciation Simulation Study of Cu2+ Complexes in an Amine-based Aqueous Precursor System Used for Preparation of Superconducting YBCO Coatings.” Dalton Transactions 41 (12): 3574–3582.
APA
Lommens, P., Feys, J., Vrielinck, H., De Buysser, K., Herman, G., Callens, F., & Van Driessche, I. (2012). EPR and speciation simulation study of Cu2+ complexes in an amine-based aqueous precursor system used for preparation of superconducting YBCO coatings. DALTON TRANSACTIONS, 41(12), 3574–3582.
Vancouver
1.
Lommens P, Feys J, Vrielinck H, De Buysser K, Herman G, Callens F, et al. EPR and speciation simulation study of Cu2+ complexes in an amine-based aqueous precursor system used for preparation of superconducting YBCO coatings. DALTON TRANSACTIONS. 2012;41(12):3574–82.
MLA
Lommens, Petra, Jonas Feys, Henk Vrielinck, et al. “EPR and Speciation Simulation Study of Cu2+ Complexes in an Amine-based Aqueous Precursor System Used for Preparation of Superconducting YBCO Coatings.” DALTON TRANSACTIONS 41.12 (2012): 3574–3582. Print.
@article{2010209,
  abstract     = {In this work, we investigate the chemistry for an aqueous acetate-triethanolamine-ammonia based YBa2Cu3O7-d (YBCO) precursor system. These precursor solutions are suited for the chemical solution deposition of superconducting YBCO layers on top of single crystal SrTiO3 or buffered NiW tapes. The development of this kind of precursor inks often involves trial-and-error experimenting and thus is very time-consuming. To reduce labwork to the minimum, the theoretical prediction of pH stability limits and the complexation behaviour of the different metal ions and complexants in the inks are very important. For this purpose, we simulated, based on literature values, the complexation behaviour of Cu2+ in the aqueous precursor solutions as a function of pH. To validate the used model, we performed potentiometric pH titrations for solutions with similar composition and checked the correctness of fit between experiment and model. The generated complexometric results are coupled with X-band EPR spectra to further confirm the results. EPR spectra for fully prepared precursor solutions as well as for Cu2+ reference solutions containing only one type of ligand (acetate, triethanolamine or ammonia) were investigated as a function of pH. We find that, in line with speciation simulation, only acetates are actively complexing the Cu2+ ions at pH values below 7, while when reaching higher pH levels mainly triethanolamine complexes are formed. Over the entire pH range, no trace of free Cu2+ or Cu(OH)(2), possibly creating precipitation during gelation and thus complicating further processing, could be found.},
  author       = {Lommens, Petra and Feys, Jonas and Vrielinck, Henk and De Buysser, Klaartje and Herman, Gerrit and Callens, Freddy and Van Driessche, Isabel},
  issn         = {1477-9226},
  journal      = {DALTON TRANSACTIONS},
  keyword      = {THIN-FILMS,ELECTRON-PARAMAGNETIC RESONANCE,SOLUTION DEPOSITION,COATED CONDUCTORS,BUFFER LAYERS,COPPER(II),YBA2CU3O7-DELTA,METAL,ION,SPECTRA},
  language     = {eng},
  number       = {12},
  pages        = {3574--3582},
  title        = {EPR and speciation simulation study of Cu2+ complexes in an amine-based aqueous precursor system used for preparation of superconducting YBCO coatings},
  url          = {http://dx.doi.org/10.1039/C2DT11639A},
  volume       = {41},
  year         = {2012},
}

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