Oxygen Mobility of Samarium Doped Neodymium Nickelates Sintered by E-Beams

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Abstract

Ruddlesden–Popper phases are known materials for electrochemical devices such as solid oxide fuel cells/electrolyzers, oxygen separation membranes. Doping A-site with lanthanides with less radii can allow to increase the oxygen mobility, however, this problem is still not studied well. This work aims at studying phase composition and transport properties of Sm doped Nd nickelates sintered by radiation-thermal technique using e-beams. Nd2–xSmxNiO4+δ (x = 0.2, 0.4) were synthesized by modified Pechini technique and sintered by e-beams at 1150–1250°C. The materials obtained were characterized by X-ray diffraction, X-ray photoelectron spectroscopy and temperature-programmed isotope exchange of oxygen with C18O2 in a flow reactor. The surface oxygen presents in two forms differing in binding energy. According to the temperature-programmed isotope exchange data, the samples possess nonuniformity in the oxygen mobility, and slow diffusion channel is present for the sample with x = 0.4. Such an oxygen diffusion features are probably related to the effect of doping with and radiation-thermal sintering on the structure with formation of admixed phases, hampering the cooperative migration due to emergence of local defects and variation of the surface and grain boundary composition.

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V. A. Sadykov

Boreskov Institute of Catalysis of the Siberian Branch of the Russian Academy of Sciences

Author for correspondence.
Email: sadykov@catalysis.ru
Russian Federation, Novosibirsk

E. M. Sadovskaya

Boreskov Institute of Catalysis of the Siberian Branch of the Russian Academy of Sciences

Email: sadykov@catalysis.ru
Russian Federation, Novosibirsk

Yu. N. Bespalko

Boreskov Institute of Catalysis of the Siberian Branch of the Russian Academy of Sciences

Email: sadykov@catalysis.ru
Russian Federation, Novosibirsk

E. A. Smal

Boreskov Institute of Catalysis of the Siberian Branch of the Russian Academy of Sciences

Email: sadykov@catalysis.ru
Russian Federation, Novosibirsk

O. A. Bulavchenko

Boreskov Institute of Catalysis of the Siberian Branch of the Russian Academy of Sciences

Email: sadykov@catalysis.ru
Russian Federation, Novosibirsk

N. F. Eremeev

Boreskov Institute of Catalysis of the Siberian Branch of the Russian Academy of Sciences

Email: yeremeev21@catalysis.ru
Russian Federation, Novosibirsk

I. P. Prosvirin

Boreskov Institute of Catalysis of the Siberian Branch of the Russian Academy of Sciences

Email: sadykov@catalysis.ru
Russian Federation, Novosibirsk

M. A. Mikhailenko

Institute of Solid State Chemistry and Mechanochemistry of the Siberian Branch of the Russian Academy of Sciences

Email: sadykov@catalysis.ru
Russian Federation, Novosibirsk

M. V. Korobeynikov

Budker Institute of Nuclear Physics of the Siberian Branch of the Russian Academy of Sciences

Email: sadykov@catalysis.ru
Russian Federation, Novosibirsk

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2. Fig. 1. Diffractograms of Nd1.8Sm0.2NiO4+δ samples sintered by RTS at 1150°C (1) and 1250°C (2). Phase designation: * - (Nd, Sm)2NiO4+δ (ICSD50440), ^ - (Nd, Sm)2O3 (ICSD60639), ↓ - NiO.

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3. Fig. 2. Diffractograms of Nd1.6Sm0.4NiO4+δ samples sintered by RTS at 1150°C (1) and 1250°C (2). Phase designation: * - (Nd, Sm)2NiO4+δ (ICSD50440), ♦ - (Nd, Sm)NiO3-δ (PDF 00-041-0344).

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4. Fig. 3. O1s XRD spectra of Nd1.8Sm0.2NiO4+δ samples sintered in the furnace at 1150°C (1), RTS at 1150°C (2), Nd1.6Sm0.4NiO4+δ sample sintered by RTS at 1150°C (3), and Nd1.8Sm0.2NiO4+δ sample sintered by RTS at 1250°C (4).

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5. Fig. 4. Temperature-programmed oxygen isotope exchange with C18O2 in the flow reactor for Nd2-xSmxNiO4+δ (x = 0.2 and 0.4) samples sintered by RTS at different temperatures. Dots - experiment, lines - model.

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6. Fig. 5. Dependence of the oxygen self-diffusion coefficient for Nd2-xSmxNiO4+δ samples sintered in the furnace and RTS according to the C18O2 TPIO data: (1) Nd2NiO4+δ sintered in the furnace at 1150°C [36], (2) Nd1.8Sm0. 2NiO4+δ sintered in the furnace at 1150°C [35], (3) Nd1.8Sm0.2NiO4+δ sintered RTS at 1150°C (this work), (4) Nd1.8Sm0.2NiO4+δ sintered RTS at 1250°C (this work), (5, 5ʹ) Nd1.6Sm0.4NiO4+δ sintered RTS at 1150°C (this work).

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