Reidar Haugsrud

• Liu, Xin; Bjørheim, Tor Svendsen; Vines, Lasse; Fjellvåg, Øystein; Granerød, Cecilie Skjold; Prytz, Øystein; Yamamoto, Takafumi; Kageyama, Hiroshi; Norby, Truls Eivind & Haugsrud, Reidar (2019). Highly Correlated Hydride Ion Tracer Diffusion in SrTiO3–xHx Oxyhydrides. Journal of the American Chemical Society.  ISSN 0002-7863.  141(11), s 4653- 4659 . doi: 10.1021/jacs.8b12985
• Stange, Marit Synnøve Sæverud; Dayaghi, Amir Masoud; Denonville, Christelle; Larring, Yngve; Rørvik, Per Martin; Haugsrud, Reidar & Norby, Truls Eivind (2019). Fabrication of metal-supported proton-conducting electrolysers with thin film Sr- And Ce-doped BZY electrolyte. ECS Transactions.  ISSN 1938-5862.  91(1), s 941- 949 . doi: 10.1149/09101.0941ecst Show summary

  n this work, we present fabrication and initial testing of metal-supported proton ceramic electrolyser (MS-PCEC) single cells with a thin electrolyte. Plansee ITM porous metal is used as metal support. Spray-coating is used to deposit a conducting layer of La1-xSrxTi1-yNiyO3-δ (LSTN) which is used for low temperature (600-800 °C) deposition of a gas-tight, thin-film layer (~2 μm) of electrolyte by pulsed laser deposition (PLD). Post-annealing of the electrolyte is evaluated to improve its performance. In order to have a smaller thermal expansion coefficient (TEC) mismatch towards LSTN (~10-11 × 10-6 K-1), we developed a new Sr- and Ce-doped proton-conducting electrolyte, yielding a larger TEC (~10-11 × 10-6 K-1) compared to BZY (~8 × 10-6 K-1). The cell with Pt as air electrode shows acceptable open circuit voltage and low overpotentials at 600 °C, demonstrating the potential of developing the first working MS-PCEC.

• Stefan, Elena; Denonville, Christelle; Larring, Yngve; Stange, Marit Synnøve Sæverud & Haugsrud, Reidar (2019). Oxidation study of porous metal substrates for metal supported proton ceramic electrolyzer cells. Corrosion Science.  ISSN 0010-938X. . doi: 10.1016/j.corsci.2019.108335
• Desissa, Temesgen D.; Haugsrud, Reidar; Wiik, Kjell & Norby, Truls Eivind (2018). Inter-diffusion across a direct p-n heterojunction of Li-doped NiO and Al-doped ZnO. Solid State Ionics.  ISSN 0167-2738.  320, s 215- 220 . doi: 10.1016/j.ssi.2018.03.011 Show summary

  We herein report inter-diffusion across the interface between p-type Ni0.98Li0.02O and n-type Zn0.98Al0.02O for various applications including p-n-heterojunction diodes and oxide thermoelectrics. Diffusion couples were made of polished surfaces of ceramic samples pre-sintered at 1250 and 1350 °C for Ni0.98Li0.02O and Zn0.98Al0.02O, respectively. The inter-diffusion couples were annealed at 900–1200 °C for 160 h in ambient air. Electron Probe Micro Analysis (EPMA) was used to acquire diffusion profiles, followed by fitting to Fick's second law and Whipple–Le Claire's models for bulk and grain-boundary diffusion calculation, respectively. Zn2+ diffused into Ni0.98Li0.02O mainly by bulk diffusion with an activation energy of 250 ± 10 kJ/mol, whereas Ni2+ diffused into Zn0.98Al0.02O by both bulk and enhanced grain boundary diffusion with activation energies of 320 ± 120 kJ/mol and 245 ± 50 kJ/mol, respectively. The amount of Al3+ diffused from the Al-doped ZnO into the NiO phase was too small for a corresponding diffusion coefficient to be calculated. Li-ion distribution and diffusivity were not determined due to lack of analyzer sensitivity for Li. The bulk and effective diffusivities of Zn2+ and Ni2+ into NiO and ZnO enable prediction of inter-diffusion lengths as a function of time and temperature, allowing estimates of device performance, stability, and lifetimes at different operation temperatures.

• Liu, Xin; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2018). Formation of defects and their effects on hydride ion transport properties in a series of K2NiF4-type oxyhydrides. Journal of Materials Chemistry A.  ISSN 2050-7488.  6(4), s 1454- 1461 . doi: 10.1039/c7ta08435h
• Escolastico, S; Solis, C; Haugsrud, Reidar; Magraso, Anna & Serra, J. M. (2017). On the ionic character of H2 separation through mixed conducting Nd5.5W0.5Mo0.5O11.25−δ membrane. International journal of hydrogen energy.  ISSN 0360-3199.  42(16), s 11392- 11399 . doi: 10.1016/j.ijhydene.2017.02.087
• Hancke, Ragnhild & Haugsrud, Reidar (2017). The correlation between surface kinetic and bulk diffusion properties of proton conducting oxides. Solid State Ionics.  ISSN 0167-2738.  306, s 48- 54 . doi: 10.1016/j.ssi.2017.02.006
• Liu, Xin; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2017). Formation and migration of hydride ions in BaTiO3-xHx oxyhydride. Journal of Materials Chemistry A.  ISSN 2050-7488.  5(3), s 1050- 1056 . doi: 10.1039/c6ta06611a
• Malerød-Fjeld, Harald; Clark, Daniel Ryan; Yuste-Tirados, Irene; Zanón, Raquel; Catalán-Martinez, David; Beeaff, Dustin; Morejudo, Selene Hernandez; Vestre, Per K.; Norby, Truls Eivind; Haugsrud, Reidar; Serra, José M. & Kjølseth, Christian (2017). Thermo-electrochemical production of compressed hydrogen from methane with near-zero energy loss. Nature Energy.  ISSN 2058-7546.  2(12), s 923- 931 . doi: 10.1038/s41560-017-0029-4
• Sazinas, Rokas; Sakaguchi, Isao; Hasle, Ida Margrete; Polfus, Jonathan M.; Haugsrud, Reidar; Einarsrud, Mari-Ann & Grande, Tor (2017). Tracer diffusion of 96Zr and 134Ba in polycrystalline BaZrO3. Physical Chemistry, Chemical Physics - PCCP.  ISSN 1463-9076.  19(32), s 21878- 21886 . doi: 10.1039/C7CP04039C Full text in Research Archive.
• Stange, Marit Synnøve Sæverud; Stefan, Elena; Denonville, Christelle; Larring, Yngve; Rørvik, Per Martin & Haugsrud, Reidar (2017). Development of novel metal-supported proton ceramic electrolyser cell with thin film BZY15–Ni electrode and BZY15 electrolyte. International journal of hydrogen energy.  ISSN 0360-3199.  42(19), s 13454- 13462 . doi: 10.1016/j.ijhydene.2017.03.028
• Stefan, Elena; Stange, Marit Synnøve Sæverud; Denonville, Christelle; Larring, Yngve; Hildenbrand, Nicolas; Norby, Truls Eivind & Haugsrud, Reidar (2017). Layered microstructures based on BaZr0.85Y0.15O3−δ by pulsed laser deposition for metal-supported proton ceramic electrolyser cells. Journal of Materials Science.  ISSN 0022-2461.  52(11), s 6486- 6497 . doi: 10.1007/s10853-017-0884-1 Full text in Research Archive.
• Bjørheim, Tor Svendsen; Løken, Andreas & Haugsrud, Reidar (2016). On the relationship between chemical expansion and hydration thermodynamics of proton conducting perovskites. Journal of Materials Chemistry A.  ISSN 2050-7488.  4(16), s 5917- 5924 . doi: 10.1039/c5ta10090a Full text in Research Archive.
• Cao, Yong; Duan, Nanqi; Jian, Li; Evans, Anna & Haugsrud, Reidar (2016). Effect of Nb Doping on Hydration and Conductivity of La27W5O55.5. Journal of The American Ceramic Society.  ISSN 0002-7820.  99(10), s 3309- 3316 . doi: 10.1111/jace.14346
• Cao, Yong; Xiong, Chunyan; Jian, Li; Vøllestad, Einar; Evans, Anna & Haugsrud, Reidar (2016). Enhancement of the electron conductivity of La27(W0.85Nb0.15)5O55.5-δ by Mo doping for hydrogen permeation. Journal of the Electrochemical Society.  ISSN 0013-4651.  163(10), s F1151- F1156 . doi: 10.1149/2.1251609jes
• Liu, Xin; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2016). Thermochemical properties of rare-earth oxyhydrides from first principles phonon calculations. RSC Advances.  ISSN 2046-2069.  6(12), s 9822- 9826 . doi: 10.1039/c5ra26552e
• Løken, Andreas; Haugsrud, Reidar & Bjørheim, Tor Svendsen (2016). Unravelling the fundamentals of thermal and chemical expansion of BaCeO3 from first principles phonon calculations. Physical Chemistry, Chemical Physics - PCCP.  ISSN 1463-9076.  18, s 31296- 31303 . doi: 10.1039/C6CP05710A Full text in Research Archive.
• Skomedal, Gunstein; Burkov, Alexander; Samunin, Alexander Yu; Haugsrud, Reidar & Middleton, Peter Hugh (2016). High temperature oxidation of Mg2(Si-Sn). Corrosion Science.  ISSN 0010-938X.  111(1), s 325- 333 . doi: 10.1016/j.corsci.2016.05.016
• Wachowski, Sebastian Lech; Mielewczyk-Gryn, Aleksandra; Zagorski, Krzysztof; Li, Cheng; Jasinski, Piotr; Skinner, Stephen J; Haugsrud, Reidar & Gazda, Maria (2016). Influence of Sb-substitution on ionic transport in lanthanum orthoniobates. Journal of Materials Chemistry A.  ISSN 2050-7488.  4(30), s 11696- 11707 . doi: 10.1039/c6ta03403a
• Ashok, Anuradha Machina; Haugsrud, Reidar; Norby, Truls & Olsen, Arne (2015). Structural study of the complex perovskite Ba4(Ba2Nb2)O11. Materials Characterization.  ISSN 1044-5803.  102, s 71- 78 . doi: 10.1016/j.matchar.2015.02.014
• Bjørheim, Tor Svendsen & Haugsrud, Reidar (2015). Proton transport properties of the RE3Ga5MO14 (RE = La, Nd and M = Si, Ti, Sn) langasite family of oxides. Solid State Ionics.  ISSN 0167-2738.  275, s 29- 34 . doi: 10.1016/j.ssi.2015.03.014
• Bjørheim, Tor Svendsen; Rahman, SMH; Eriksson, Sten G.; Knee, Christopher & Haugsrud, Reidar (2015). Hydration Thermodynamics of the Proton Conducting Oxygen-Deficient Perovskite Series BaTi1–xMxO3–x/2 with M = In or Sc. Inorganic Chemistry.  ISSN 0020-1669.  54(6), s 2858- 2865 . doi: 10.1021/ic503006u
• Bjørheim, Tor Svendsen; Shanmugappirabu, Vijay; Haugsrud, Reidar & Norby, Truls (2015). Protons in piezoelectric langatate; La3Ga5.5Ta0.5O14. Solid State Ionics.  ISSN 0167-2738.  278(1), s 275- 280 . doi: 10.1016/j.ssi.2015.06.024
• Hoque, Md Khairul; Haugsrud, Reidar & Knee, Christopher (2015). Structure and conductivity of acceptor doped La2BaZnO5 and Nd2BaZnO5. Solid State Ionics.  ISSN 0167-2738.  272, s 160- 165 . doi: 10.1016/j.ssi.2015.02.001
• Li, Zuoan; Kjølseth, Christian & Haugsrud, Reidar (2015). Hydrogen permeation, water splitting and hydration kinetics in Nd5.4Mo0.3W0.7O12−δ. Journal of Membrane Science.  ISSN 0376-7388.  476, s 105- 111 . doi: 10.1016/j.memsci.2014.11.013
• Løken, Andreas; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2015). The pivotal role of the dopant choice on the thermodynamics of hydration and associations in proton conducting BaCe0.9X0.1O3-δ (X = Sc, Ga, Y, In, Gd and Er). Journal of Materials Chemistry A.  ISSN 2050-7488.  3(46), s 23289- 23298 . doi: 10.1039/c5ta04932f Full text in Research Archive.
• Magraso, Anna; Falk-Windisch, Hannes; Froitzheim, Jan; Svensson, Jan-Erik & Haugsrud, Reidar (2015). Reduced long term electrical resistance in Ce/Co-coated ferritic stainless steel for solid oxide fuel cell metallic interconnects. International journal of hydrogen energy.  ISSN 0360-3199.  40(27), s 8579- 8585 . doi: 10.1016/j.ijhydene.2015.04.147
• Vøllestad, Einar; Teusner, Markus; De Souza, Roger A. & Haugsrud, Reidar (2015). Diffusion of Nd and Mo in lanthanum tungsten oxide. Solid State Ionics.  ISSN 0167-2738.  274, s 128- 133 . doi: 10.1016/j.ssi.2015.03.011
• Bjørheim, Tor Svendsen; Haugsrud, Reidar & Norby, Truls (2014). Protons in acceptor doped langasite, La3Ga5SiO14. Solid State Ionics.  ISSN 0167-2738.  264, s 76- 84 . doi: 10.1016/j.ssi.2014.05.017
• Cebasek, Nebojsa; Haugsrud, Reidar & Norby, Truls (2014). Cation transport in Sr and Cu substituted La2NiO4+δ studied by inter-diffusion. Solid State Ionics.  ISSN 0167-2738.  254, s 32- 39 . doi: 10.1016/j.ssi.2013.10.041
• Løken, Andreas; Kjølseth, Christian & Haugsrud, Reidar (2014). Electrical conductivity and TG-DSC study of hydration of Sc-doped CaSnO3 and CaZrO3. Solid State Ionics.  ISSN 0167-2738.  267, s 61- 67 . doi: 10.1016/j.ssi.2014.09.006
• Magraso, Anna; Fontaine, Marie-Laure; Bredesen, Rune; Haugsrud, Reidar & Norby, Truls (2014). Cathode compatibility, operation, and stability of LaNbO4-based proton conducting fuel cells. Solid State Ionics.  ISSN 0167-2738.  262, s 382- 387 . doi: 10.1016/j.ssi.2013.12.009 Show summary

  Cathodes compatible with Ca-doped LaNbO4 (LCNO) and the operation of a complete proton conducting fuel cell based on this electrolyte are presented. The best performing cathode was a 50 vol.% La0.8Sr0.2MnO3 (LSM)–50 vol.% LCNO composite, with an overall area specific resistance (ASR) of ~ 10 Ω cm2 at 800 °C in wet air. Pt and La0.8Sr0.2(Cr0.5Mn0.5)O3-based cathodes exhibit higher ASRs. The performance of a complete Ni–LCNO//LCNO//LSM–LCNO fuel cell shows a high open circuit voltage but with relatively low performance, in agreement with the modest proton conductivity of LaNbO4-based materials and cathode performances. The cell exhibits stable operation with CO2 containing atmosphere on the cathode side, confirming the chemical robustness of LaNbO4-based electrolytes.

• Magraso, Anna; Fontaine, Marie-Laure; Haugsrud, Reidar & Norby, Truls (2014). Hydrogen oxidation kinetics and performance of Ni-LaNbO4 cermet anodes for proton conducting SOFCs. Journal of the Electrochemical Society.  ISSN 0013-4651.  161(4), s F373- F379 . doi: 10.1149/2.002404jes Show summary

  Ni composite anodes for Ca-doped LaNbO4 (LCNO) based proton conducting solid oxide fuel cells were fabricated as screen-printed Ni-LCNO cermets on a dense self-supported LCNO electrolyte and as a semi-symmetrical cell consisting of a ∼ 15 μm thick LCNO electrolyte deposited on a tape-cast Ni-LCNO anode support. The influence of Ni content and sintering temperature on the polarization resistance of the Ni-LCNO interface was investigated. The interface was characterized by electrochemical impedance spectroscopy, and the effects of temperature, pO2 and pH2O on the area specific resistance (ASR) at open circuit were used to determine the rate limiting steps of the hydrogen kinetics of these anodes. The total electrode response is 1.1 Ωcm2 for 40/60 (vol) Ni/LCNO cermet support, at 800°C in wet H2, and the activation energy ∼ 0.5 eV. Three processes were suggested to contribute to the polarization resistance of Ni-LCNO cermet anodes, the most resistive believed to correspond to a charge transfer process at the interface between hydrogen atoms on or in Ni and protons in the electrolyte.

• Magraso, Anna & Haugsrud, Reidar (2014). Effects of the La/W ratio and doping on the structure, defect structure, stability and functional properties of proton-conducting lanthanum tungstate La28-xW4+x/O54+δ. A review. Journal of Materials Chemistry A.  ISSN 2050-7488.  2(32), s 12630- 12641 . doi: 10.1039/c4ta00546e
• Rahman, Seikh, R. H; Ahmed, Istaq; Haugsrud, Reidar; Eriksson, S.G. & Knee, Christopher (2014). Characterisation of structure and conductivity of BaTi<sub>0.5</sub>Sc <sub>0.5</sub>O<sub>3 - δ</sub>. Solid State Ionics.  ISSN 0167-2738.  255, s 140- 146 . doi: 10.1016/j.ssi.2013.12.010
• Vigen, Camilla Kaori & Haugsrud, Reidar (2014). Hydrogen flux in La0.87Sr0.13CrO3–δ. Journal of Membrane Science.  ISSN 0376-7388.  468, s 317- 323 . doi: 10.1016/j.memsci.2014.06.012

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• Dayaghi, Amir Masoud; Stange, Marit Synnøve Sæverud; Denonville, Christelle; Larring, Yngve; Rørvik, Per Martin; Haugsrud, Reidar & Norby, Truls Eivind (2019). Thin-film electrolyte with TEC optimized for metal-supported proton ceramic electrochemical cell.
• Emhjellen, Linn Katinka; Xing, Wen; Li, Zuoan & Haugsrud, Reidar (2019). Electrochemical Transport in Molten/Solid Composite V2O5-ZrV2O7.
• Li, Zuoan; Liu, Xin & Haugsrud, Reidar (2019). Dissociation of oxygen on oxides determined by a modified gas phase analysis (GPA).
• Norby, Truls Eivind; Kalland, Liv-Elisif Queseth; Løken, Andreas; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2019). Hydration of fluorite-related rare-earth cerates.
• Norby, Truls Eivind; Liu, Xin; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2019). Hydride ion conduction.
• Stange, Marit Synnøve Sæverud; Dayaghi, Amir Masoud; Denonville, Christelle; Larring, Yngve; Rørvik, Per Martin; Haugsrud, Reidar & Norby, Truls Eivind (2019). Fabrication of Metal-Supported Proton-Conducting Electrolysers with Thin Film Sr- and Ce-Doped BZY Electrolyte.
• Stange, Marit Synnøve Sæverud; Dayaghi, Amir Masoud; Denonville, Christelle; Larring, Yngve; Rørvik, Per Martin; Haugsrud, Reidar & Norby, Truls Eivind (2019). Key challenges in fabrication of metal-supported thin film proton conducting electrolyser cells.
• Thoréton, Vincent; Bjørheim, Tor Svendsen; Liu, Xin; Li, Zuoan & Haugsrud, Reidar (2019). Influence of water vapour on the surface exchange kinetics of functional oxides.
• Clark, Daniel Ryan; Malerød-Fjeld, Harald; Budd, Michael; Catalán-Martinez, David; Beeaff, Dustin; Norby, Truls Eivind & Haugsrud, Reidar (2018). Design and development of next-generation protonic reactors.
• Desissa, Temesgen D.; Norby, Truls Eivind & Haugsrud, Reidar (2018). Stability and properties of materials and interfaces for oxide thermoelectrics. Series of dissertations submitted to the Faculty of Mathematics and Natural Sciences, University of Oslo.. 1969.
• Liu, Xin; Haugsrud, Reidar; Bjørheim, Tor Svendsen & Fjellvåg, Helmer (2018). Defect, Stability and Transport in Oxyhydrides. Series of dissertations submitted to the Faculty of Mathematics and Natural Sciences, University of Oslo.. 1980.
• Clark, Daniel Ryan; Kjølseth, Christian; Malerød-Fjeld, Harald; Hernandez Morejudo, Selene; Zanon, R.; Serra, J; Beeaff, Dustin; Vigen, Camilla Kaori; Tirados, Irene Yuste; Vestre, Per Kristian & Haugsrud, Reidar (2017). Intensified Conversion of Natural Gas Using Proton-Conducting Ceramics.
• Emhjellen, Linn Katinka; Haugsrud, Reidar; Bjørheim, Tor Svendsen & Strandbakke, Ragnar (2017). Defects and Transport in SrFe1-xMoxO3-δ.
• Haugsrud, Reidar; Chen, Min & Bjørheim, Tor Svendsen (2017). SSPC-18 Conference Special Issue. Solid State Ionics.  ISSN 0167-2738.  306, s 1 . doi: 10.1016/j.ssi.2017.04.012
• Li, Zuoan & Haugsrud, Reidar (2017). Oxygen dissociation rate of oxide ion conductors determined by a novel gas phase analysis technique.
• Løken, Andreas; Haugsrud, Reidar; Norby, Truls Eivind & Bjørheim, Tor Svendsen (2017). Hydration thermodynamics of oxides.
• Stange, Marit Synnøve Sæverud; Denonville, Christelle; Larring, Yngve; Stefan, Elena; Rørvik, Per Martin; Haugsrud, Reidar & Norby, Truls Eivind (2017). Manufacturing of Metal Supported Protonic Ceramic Electrolyser Cells (PCEC).
• Stub, Sindre Østby; Haugsrud, Reidar & Norby, Truls Eivind (2017). Protonic Conduction in Porous Oxides.
• Gutterød, Emil Sebastian; Haugsrud, Reidar & Polfus, Jonathan M. (2016). An Experimental and Computational Study of Nitrogen Activation on Promoted Ruthenium Catalysts. Show summary

  Ruthenium based catalysts for ammonia synthesis have been studied extensively following the industrial adoption of a promoted carbon supported ruthenium catalyst in the Kellogg Advanced Ammonia Process (KAAP). Nevertheless, there are still fundamental aspects such as the dissociative adsorption of nitrogen—generally regarded as the rate determining step of NH3 synthesis—and the influence of the barium promoter, not fully explored. In the present work, the activation of nitrogen on barium promoted ruthenium is elucidated through a combined experimental and computational approach. Nitrogen dissociation and association on a clean and barium promoted Ru(0001) step were investigated through DFT based calculations using VASP. Unpromoted dissociation was found to proceed with an energy barrier of 51 kJmol−1, with a N-N distance of the transition state (TS) of 1.864 Å. The calculated activation barrier for association was 135 kJmol−1, which increased to 161 kJmol−1 when diffusion of atomic nitrogen along the terrace was considered. Upon promotion by a unit of atomic Ba, BaOH and BaO at the step, the dissociation barrier decreased rather similarly by 21, 18 and 18 kJmol−1, respectively. The chemical state of the promoting unit was determined to have a larger effect on the association barrier, which decreases by 19, 10 and 5 kJmol−1, respectively. A previously not reported local energy minimum state with one nitrogen atom adsorbed on the b5-hcp site and the other at a step-bridge site was identified. A significant stabilization of the local minimum state is observed upon promotion: the N-N distance of the initial and final state of dissociation increased (which can be associated with a weakening of the N-N bond), while it decreased for the TS and the local minimum state. The promoting effect decreases rapidly with increasing distance to the dissociating nitrogen, indicating that the interactions were of electronic nature. Powdered catalyst samples of Ru-Ba/AC were prepared by Ba(NO3)2 wet-impregnation of 5 wt% Ru on activated carbon. The nitrogen isotope exchange (IE) reaction 14,14N2 + 15,15N2 = 214,15N2 on Ru-Ba/AC was investigated in the temperature range 320– 750°C at N2 pressures of 20–230mbar, by means of gas-phase analysis with mass spectrometry (GPA-MS). Apparent isotope exchange activation energies in range 162– 178 kJmol−1 were obtained below 425°C. This is in good agreement with the literature and the present computational results. At higher temperatures the apparent activaiii Abstract tion energy abruptly decreases to 64–88 kJmol−1. It is suggested that the change in temperature dependence is due to limitations by pore diffusion at higher temperatures. In the presence of 1mbar water vapor in the temperature range 575–625°C, the isotope exchange rate was significantly reduced compared to under dry conditions, and the apparent activation energy increased from 88 ± 2 kJmol−1 to 126 ± 12 kJmol−1. When water vapor was introduced, evolution of H2 was observed, indicating that oxidation of partially reduced Ba occurred in the presence of H2O. Isotherms of the isotope exchange rate showed reaction orders with respect to nitrogen partial pressure of 0.83 ± 0.05 and 0.88 ± 0.03 at 625°C and 700°C, respectively, and 1.1 at 450°C. All of which are in good agreement with values reported in literature for NH3 synthesis. Deactivation of the catalyst was observed at temperatures above 500°C, resulting in a significantly decreasing IE rate with time. In accordance with reports from literature, and the computational and experimental results, it is proposed the isotope exchange rate and activation energy are highly dependent on the chemical state of the barium promoter, which is further dependent on the environmental conditions, such as temperature and the presence of water vapor. iv

• Hasle, Ida Margrete; Haugsrud, Reidar & Polfus, Jonathan M. (2016). Computational Studies of Cation Transport in Barium Zirconate.
• Hasle, Ida Margrete; Vøllestad, Einar; Haugsrud, Reidar; De Souza, Roger; Gries, Ute & Waldow, Stephan (2016). B-site Cation (Zr4+) Diffusion in Yttrium doped Barium Zirconate.
• Lervik, Adrian; Bjørheim, Tor Svendsen; Nguyen, Phuong Dan; Diplas, Spyridon; Haugsrud, Reidar & Gunnæs, Anette Eleonora (2016). Chemical and Structural Investigations of Grain Boundaries in Y-Doped BaZrO3.
• Lervik, Adrian; Haugsrud, Reidar; Diplas, Spyridon & Gunnæs, Anette Eleonora (2016). Structural- and Compositional Investigations of Grain Boundaries in Y-Doped BaZrO3.
• Liu, Xin; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2016). Hydride migration and electron localization in BaTiO3-xHx oxyhydride.
• Løken, Andreas; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2016). The detrimental role of acceptor and oxygen vacancy clustering on the hydration and transport properties of proton conducting oxides.
• Løken, Andreas; Haugsrud, Reidar & Bjørheim, Tor Svendsen (2016). Unravelling the Fundamentals of Thermal and Chemical Expansion of Proton Conducting Oxides.
• Løken, Andreas; Olsen, Malin Solheim; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2016). The Effect of Clustering of Acceptors and Oxygen Vacancies on the Hydration and Transport of Proton Conducting Oxides.
• Prato Modestino, Rafael Albert; Haugsrud, Reidar; Strandbakke, Ragnar & Vøllestad, Einar (2016). TRANSPORT PROPERTIES AND SURFACE KINETICS OF Ba0.8+xGd0.8La0.2+xCo2O6-d. Show summary

  The main topics of this thesis are the surface kinetics and bulk diffusion of oxygen in Ba(1-x)Gd0.8La(0.2+x)Co2O(6-d) (BGLC). Previous work has identified BGLC as very promising electrode material for SOFC’s and electrolyzers. With conductivities in the range of ~1000 S/cm and polarization resistances in the order of 10^-2 Ocm2 around operating temperatures (i.e. 500-700 ºC). BGLC is in line to surpass current state of the art materials. Yet in order to introduce a new electrode, thorough characterization needs to be performed on its physicochemical properties. BGLC has been identified as double perovkite (double on the c-axis) by x-ray diffractometry (XRD), and synchotron measurements, in the form of AA'B2O(6-d). Cobalt occupies the B sites at the cell’s corners, with octahedral coordination of oxygen atoms, while barium and the lanthanides occupy the center of each square cell. Such a structure is highly defective; the heterovalency between barium and the lanthanides introduces oxygen vacancies in the material. The perfect structure is defined at BaGd0.8La0.2Co2O6 in order to establish a defect model. It is suggested that cobalt ions of differing valence (+2, +3 and +4) are evenly distributed through the material, and that the oxygen sites are ordered in layers surrounding the different cations. From this starting point, effects of temperature and atmosphere on the structure and properties of BGLC is studied. High temperature in-situ XRD in the temperature range from 25 to 800 ºC shows little change in the structure. As opposed to other perovskites (ex.: GdBaCo2O6-d), BGLC remains stable through operating temperatures. Lanthanum can be used to dope the barium sites without compromising stability, leading to more compositions. Synchotron data shows the majority of oxygen vacancies aggregated in the lanthanide layer (O1 site), a reduced amount in the cobalt layer (O2 site), and no vacancies present in the barium layer (O3 site). Such a flexible structure can be reduced or oxidized easily. Changes in temperature using a thermal balance revealed the oxygen non-stoichiometry as function of temperature down to [O] ~4.9. The same experiments were performed isothermally with changing pO2. The defect model proposed is able to model the data closely for BGLC and related double perovskites. These oxygen vacancies allow for ionic diffusion through the material. The transport regimes were divided in two: surface exchange of oxigen, and bulk diffusion (self-, chemical, and tracer). Thermogravimetry (TG), isotope exchange gas phase analysis (GPA) and time-of-flight secondary ion mass spectroscopy (ToF-SIMS) were employed to measure the diffusion coefficients (D) and surface coefficient (k) of BGLC at various temperatures between 350 to 800 ºC. Dchem was measured to 10^-6 to 10^-7 cm2/s at relatively low temperatures of 600 – 500 ºC with an equally low activation energy of ~0.74 eV. This leads to an oxide ion conductivity of 10^-2 to 10^-3 S/cm at operating conditions. The values were found to be competitive with state-of-the-art materials in literature. The pre-exponential values and activation energies are in close agreement to related double perovskites such as GdBaCo2O6-d and PrBaCo2O6-d. The oxygen surface exchange was studied using GPA, where a mass spectrometer tracks the concentration of species in the gas phase of a reaction chamber. Various reaction sequences are proposed for the oxygen exchange process of adsorption-dissociation-association-desorption. The desorption/adsorption steps were found to be rate limiting for this material. The surface exchange coefficient, k, is characterized by 6.0*10^-2 Exp(-66570/RT), a high value for k0 and low Ea for perovskites, but on par with novel double-perovskites. An imporant of feature of BGLC is the relatively high proton content (~1 mol%) under wet atmosphere. The hydration properties are included and modeled in the defect structure.

• Stange, Marit Synnøve Sæverud; Stefan, Elena; Denonville, Christelle; Fontaine, Marie-Laure; Larring, Yngve & Haugsrud, Reidar (2016). Development of metal supported proton ceramic electrolyser cells (PCEC) for renewable hydrogen production.
• Stange, Marit Synnøve Sæverud; Stefan, Elena; Denonville, Christelle; Larring, Yngve & Haugsrud, Reidar (2016). DEVELOPMENT OF MS-PCEC.
• Stange, Marit Synnøve Sæverud; Stefan, Elena; Denonville, Christelle; Larring, Yngve; Rørvik, Per Martin; Fontaine, Marie-Laure & Haugsrud, Reidar (2016). Development of metal supported proton ceramic electrolyser cells (PCEC) for renewable hydrogen production.
• Stange, Marit Synnøve Sæverud; Stefan, Elena; Denonville, Christelle; Larring, Yngve; Rørvik, Per Martin & Haugsrud, Reidar (2016). Progress on development of metal-supported proton conducting electrolysis cells (PCEC).
• Stefan, Elena; Stange, Marit Synnøve Sæverud; Denonville, Christelle; Larring, Yngve; Norby, Truls & Haugsrud, Reidar (2016). Fabrication of Multi-layered Microstructures based on BaZr0.85Y0.15O3-δ for Metal Supported Proton Ceramic Electrolyzer Cells by Pulsed Laser Deposition.
• Desissa, Temesgen D.; Haugsrud, Reidar & Norby, Truls (2015). Interface properties of p-n junction of oxide thermoelectric materials. Show summary

  Thermoelectric materials are used to convert waste heat to consumable power. Among these materials, oxide thermoelectric materials are emerging as promising candidate materials as they are stable at high temperature and non-toxic as well as environment friendly. In the present work, we are investigating the stability and thermodynamic co-existence at the interface of a newly proposed thermoelectric generator. In this type of module configuration, the p and n legs will be put in direct contact without metallic interconnect. The barrier layer that could be formed at high temperature side could be surmounted by operating at high temperature to increase the generation rate of minority charge carriers. At low temperature side, there will be a recombination of majority charge carriers. This implies that the Ohmic behavior of the materials at p-n junction increases with increasing temperature. Powders such as “Ca3Co4O9” (CCO) and Sr0.9La0.1TiO3 (SLTO) as p-type and n-type, respectively, were used via standard solid state reaction methods of powder synthesis. Then the samples were subjected to characterization and measurements.

• Fjellvåg, Øystein Slagtern; Fjellvåg, Helmer; Liu, Xin; Haugsrud, Reidar & Sjåstad, Anja Olafsen (2015). Hydride oxides with perovskite related structure: Case study of La2LiHO3.
• Fjellvåg, Øystein Slagtern; Sjåstad, Anja Olafsen; Haugsrud, Reidar & Gunnæs, Anette Eleonora (2015). Investigation of Novel Hydride Oxides for Holistic Understanding of Functional Materials.
• Hasle, Ida Margrete & Haugsrud, Reidar (2015). Metal Cation Inter-diffusion in BaZr0.9Y0.1O3-δ(BZY).
• Hasle, Ida Margrete & Haugsrud, Reidar (2015). Metal Cation Inter-diffusion in BaZr0.9Y0.1O3-δ(BZY).
• Lervik, Adrian; Haugsrud, Reidar; Diplas, Spyridon & Gunnæs, Anette Eleonora (2015). A TEM approach to BZY.
• Løken, Andreas; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2015). Defect Associations as a Potential Cause for Limiting Proton Concentrations in Acceptor Doped Oxides.
• Løken, Andreas; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2015). Origins of limiting proton concentrations in acceptor doped oxides.
• Morland, Bjørn Helge; Dugstad, Arne & Haugsrud, Reidar (2015). Corrosion in CO2 transport pipeline The effect of dissolved and free water in dense phase CO2. Show summary

  The carbon dioxide (CO2) concentration in the atmosphere has increased dramatically over the last century, and much of this increase is a direct consequence of human activities. Being a greenhouse gas, CO2 significantly contributes to global warming, and there is an international agreement to reduce emission of CO2. One method to reduce CO2 release is carbon dioxide capture and storage (CCS). CCS entails to capture waste CO2 from large point sources, and transport it to a permanently deposit, usually in geological formations. The transported CO2 is likely to contain impurities like water, oxygen, nitrogen dioxide, sulfur dioxide and hydrogen sulfide. These impurities are known to cause corrosion, dust and/or solid formations, and may lead to operational difficulties. The present study examined how water as an impurity, both as a free water phase and water dissolved in dense phase CO2, affects the corrosion of carbon steel. There are few experimental studies that have examined corrosion in CO2 transport pipelines, and these few studies have shown different corrosion rates in experiments where the reported amount of dissolved water in the CO2 was the same. These discrepancies may reflect short-comings in methodology in some of these studies, where formation of free water may have contributed to high corrosion rates. The present study was undertaken to resolve some of the controversy related to corrosion in pure CO2/water systems. For this study we designed experimental equipment that allowed complete control of the water concentration in CO2, without the risk of droplet formation. This provides realistic results that mimic the situation in the operating pipelines. Three corrosion experiments were conducted with water dissolved in CO2 at 25 °C and 95 bar of pressure. Even with water concentrations close to the solubility limit, the general corrosion rates were below 1.5 µm/y and no localized attacks were found. A fourth experiment was conducted at and above the solubility limit of water in CO2. Even though we could confirm at the end of the experiment that water had accumulated in the loop, the corrosion rate was still at 1.0 µm/y, with no localized attacks. A final experiment was performed at 35 °C and 95 bar of pressure, in which no corrosion was detected. Corrosion products were found on the surface in all experiments, but at low quantities, most likely less than of practical significance. However, with water levels above the solubility limits, i.e. in the present of free water phase, the corrosion rate increased by 3 to 4 orders of magnitude (2 mm/y to 16 mm/y, pressure depended). For a CO2 transport pipeline these results suggest that the corrosion will not be a problem as long as the water is kept below the solubility limit. However, it is extremely important to avoid liquid water ingress as this would dramatically reduce the lifetime of the pipeline.

• Norby, Truls; Haugsrud, Reidar & Polfus, Jonathan M. (2015). Defects and transport in proton conducting BZY.
• Stange, Marit Synnøve Sæverud; Denonville, Christelle; Stefan, Elena; Haugsrud, Reidar; Rørvik, Per Martin & Larring, Yngve (2015). Development of thin film based metal supported PCEC.
• Stange, Marit Synnøve Sæverud; Stefan, Elena; Denonville, Christelle; Larring, Yngve; Dahl-Hansen, Runar; Rørvik, Per Martin & Haugsrud, Reidar (2015). Development of metal supported protonic electrolyzer cells (MSD-PCEC).
• Stefan, Elena; Stange, Marit Synnøve Sæverud; Denonville, Christelle; Dahl-Hansen, Runar; Larring, Yngve; Rørvik, Per Martin; Fontaine, Marie-Laure; Norby, Truls & Haugsrud, Reidar (2015). Fabrication and Characterization of Metal Supported Proton Ceramic Electrolyzer Cells (PCEC).
• Stefan, Elena; Stange, Marit Synnøve Sæverud; Denonville, Christelle; Dahl-Hansen, Runar; Larring, Yngve; Rørvik, Per Martin; Norby, Truls & Haugsrud, Reidar (2015). Layered Microstructures based on BaZr0.85Y0.15O3-δ for Proton Ceramic Electrolyser Cells by Pulsed Laser Deposition.
• Stefan, Elena; Stange, Marit Synnøve Sæverud; Denonville, Christelle; Larring, Yngve; Dahl-Hansen, Runar; Rørvik, Per Martin; Haugsrud, Reidar & Norby, Truls (2015). Electrode and Electrolyte Microstructures based on BaZr0.85Y0.15O3-δ for Proton Ceramic Electrolyzer Cells by Pulsed Laser Deposition.
• Stefan, Elena; Stange, Marit Synnøve Sæverud; Denonville, Christelle; Larring, Yngve; Dahl-Hansen, Runar; Rørvik, Per Martin; Norby, Truls & Haugsrud, Reidar (2015). Characterization of BaZr0.85Y0.15O3-δ Thin Films for Proton Ceramic Electrolyzer Cells by Pulsed Laser Deposition.
• Bjørheim, Tor Svendsen; Haugsrud, Reidar; Knee, Christopher & Rahman, Seikh, R. H (2014). Hydration thermodynamics of the oxygen deficient perovskite series BaTi1-xMxO3-d (M=In, Sc).
• Bjørheim, Tor Svendsen; Kotomin, Eugene; Haugsrud, Reidar & Maier, Joachim (2014). Defect thermodynamics of BaZrO3 from first principles phonon calculations.
• Bjørheim, Tor Svendsen; Kotomin, Eugene; Haugsrud, Reidar & maier, joachim (2014). Defect thermodynamics of BaZrO3 from first principles phonon calculations.
• Bjørheim, Tor Svendsen; Toyoura, Kazuaki; Norby, Truls & Haugsrud, Reidar (2014). Proton transport in the langasite family of oxides.
• Hancke, Ragnhild; Li, Zuoan & Haugsrud, Reidar (2014). Correlation between bulk and surface kinetics of YBC and LWO.
• Kalland, Liv-Elisif Queseth; Haugsrud, Reidar; Knee, Christopher & Norby, Truls (2014). Protons in rare earth fluorites.
• Li, Zuoan; Vigen, Camilla Kaori; Saeed, Sarmad Waheed; Evans, Anna; Hancke, Ragnhild; Vøllestad, Einar; Haugsrud, Reidar & Norby, Truls (2014). Research on Dense Ceramic Gas Separation Membranes at UiO.
• Løken, Andreas; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2014). Hydration thermodynamics of BaCe0.9M0.1O3-δ (M = Sc, Ga, Y, In, Gd and Er): Elucidating effects of dopant choice.
• Løken, Andreas; Bjørheim, Tor Svendsen & Haugsrud, Reidar (2014). Proton Mobility in BaCe0.9M0.1O3-δ (M = In, Sc, Y and Gd): Addressing the effects of dopant trapping.
• Stefan, Elena; Stange, Marit Synnøve Sæverud; Denonville, Christelle; Dahl-Hansen, Runar; Larring, Yngve; Rørvik, Per Martin; Fontaine, Marie-Laure; Haugsrud, Reidar & Norby, Truls (2014). Metal Supported Proton Ceramic Electrolyser Cells (PCEC) for Renewable Hydrogen Production.
• Strandbakke, Ragnar; Norby, Truls Eivind & Haugsrud, Reidar (2014). Oxygen electrodes for ceramic fuel cells with proton and oxide ion conducting electrolytes.
• Stub, Sindre Østby; Rørvik, Per Martin; Haugsrud, Reidar & Norby, Truls (2014). MODELLING OF PROTONIC SURFACE TRANSPORT OF POROUS OXIDES.
• Stub, Sindre Østby; Rørvik, Per Martin; Haugsrud, Reidar & Norby, Truls (2014). Modelling of surface conduction of porous oxides.
• Vigen, Camilla Kaori; Haugsrud, Reidar & Norby, Truls Eivind (2014). Mixed conductivity in novel oxides for dense ceramic hydrogen gas separation membranes.
• Vøllestad, Einar & Haugsrud, Reidar (2014). Cation diffusion related degradation in proton conducting oxides.

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