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- Strømsheim, Marie D., et al.
(author)
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Segregation dynamics of a Pd-Ag surface during CO oxidation investigated by NAP-XPS
- 2022
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In: Catalysis Today. - : Elsevier BV. - 0920-5861. ; 384-386, s. 265-273
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Journal article (peer-reviewed)abstract
- The dynamic changes in composition in the near-surface region of a Pd75%Ag25%(100) single crystal were monitored using near-ambient pressure x-ray photoelectron spectroscopy (NAP-XPS) during CO oxidation under oxygen rich conditions at a total pressure of 1.1 mbar. Six CO oxidation temperature cycles were investigated at different heating rates and maximum temperatures of 450 °C or 600 °C. It was found that the history of the bimetallic sample plays an important role, as the CO2 formation profile varies depending on initial conditions, and previous heating rates and maximum temperatures. In terms of CO coverage effects, normal, reversed and no hysteresis behaviour were all observed. In agreement with previous modelling predictions, the NAP-XPS data confirm a dynamic segregation behaviour upon heating/cooling where the amount of Pd in the surface region decreases with increasing temperature. Nevertheless, the Pd 3d5/2 core level relative area assessment is not fully capable of capturing all the surface dynamics inferred from the temperature dependent CO2 formation profiles, due to the probing depth. While residing at ambient temperature in the reaction mixture, however, there is a build-up of adsorbed CO at the surface showing that CO induces segregation of Pd to the topmost surface layer under these conditions. In total, this suggests that the segregation is kinetically relatively facile during temperature cycling, and that adsorbate coverage is the main controlling factor for the surface termination.
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2. |
- Østli, Elise R., et al.
(author)
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On the Durability of Protective Titania Coatings on High‐Voltage Spinel Cathodes
- 2022
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In: ChemSusChem. - : John Wiley & Sons. - 1864-5631 .- 1864-564X. ; 15:12
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Journal article (peer-reviewed)abstract
- TiO2-coating of LiNi0.5-xMn1.5+xO4 (LNMO) by atomic layer deposition (ALD) has been studied as a strategy to stabilize the cathode/electrolyte interface and mitigate transition metal (TM) ion dissolution. The TiO2 coatings were found to be uniform, with thicknesses estimated to 0.2, 0.3, and 0.6 nm for the LNMO powders exposed to 5, 10, and 20 ALD cycles, respectively. While electrochemical characterization in half-cells revealed little to no improvement in the capacity retention neither at 20 nor at 50 °C, improved capacity retention and coulombic efficiencies were demonstrated for the TiO2-coated LNMO in LNMO||graphite full-cells at 20 °C. This improvement in cycling stability could partly be attributed to thinner cathode electrolyte interphase on the TiO2-coated samples. Additionally, energy-dispersive X-ray spectroscopy revealed a thinner solid electrolyte interphase on the graphite electrode cycled against TiO2-coated LNMO, indicating retardation of TM dissolution by the TiO2-coating.
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