Understanding the Electronic Structure Evolution of Epitaxial LaNi 1- x Fe x O 3 Thin Films for Water Oxidation.

Autor: Wang L; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Adiga P; School of Chemical, Biological and Environmental Engineering, Oregon State University, Corvallis, Oregon 97331, United States., Zhao J; Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100039, China.; Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China., Samarakoon WS; School of Chemical, Biological and Environmental Engineering, Oregon State University, Corvallis, Oregon 97331, United States., Stoerzinger KA; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.; School of Chemical, Biological and Environmental Engineering, Oregon State University, Corvallis, Oregon 97331, United States., Spurgeon SR, Matthews BE, Bowden ME, Sushko PV; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Kaspar TC; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Sterbinsky GE; Advanced Photon Source, Argonne National Laboratory, Lemont, Illinois 60439, United States., Heald SM; Advanced Photon Source, Argonne National Laboratory, Lemont, Illinois 60439, United States., Wang H; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Wangoh LW; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Wu J; Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States., Guo EJ; Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China., Qian H; Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100039, China., Wang J; Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100039, China., Varga T, Thevuthasan S, Feng Z; School of Chemical, Biological and Environmental Engineering, Oregon State University, Corvallis, Oregon 97331, United States., Yang W; Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States., Du Y; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States., Chambers SA; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.
Jazyk: angličtina
Zdroj: Nano letters [Nano Lett] 2021 Oct 13; Vol. 21 (19), pp. 8324-8331. Date of Electronic Publication: 2021 Sep 21.
DOI: 10.1021/acs.nanolett.1c02901
Abstrakt: Rare earth nickelates including LaNiO 3 are promising catalysts for water electrolysis to produce oxygen gas. Recent studies report that Fe substitution for Ni can significantly enhance the oxygen evolution reaction (OER) activity of LaNiO 3 . However, the role of Fe in increasing the activity remains ambiguous, with potential origins that are both structural and electronic in nature. On the basis of a series of epitaxial LaNi 1- x Fe x O 3 thin films synthesized by molecular beam epitaxy, we report that Fe substitution tunes the Ni oxidation state in LaNi 1- x Fe x O 3 and a volcano-like OER trend is observed, with x = 0.375 being the most active. Spectroscopy and ab initio modeling reveal that high-valent Fe 3+δ cationic species strongly increase the transition-metal (TM) 3d bandwidth via Ni-O-Fe bridges and enhance TM 3d-O 2p hybridization, boosting the OER activity. These studies deepen our understanding of structural and electronic contributions that give rise to enhanced OER activity in perovskite oxides.
Databáze: MEDLINE