Title: Tuning the Electronic Structure of LaNiO ₃ through Alloying with Strontium to Enhance Oxygen Evolution Activity

Abstract

The perovskite oxide LaNiO3 is a promising oxygen electrocatalyst for renewable energy storage and conversion technologies. Here, it is shown that strontium substitution for lanthanum in coherently strained, epitaxial LaNiO3 films (La1-xSrxNiO3) significantly enhances the oxygen evolution reaction (OER) activity, resulting in performance at x = 0.5 comparable to the state-of-the-art catalyst Ba0.5Sr0.5Co0.8Fe0.2O3-delta. By combining X-ray photoemission and X-ray absorption spectroscopies with density functional theory, it is shown that an upward energy shift of the O 2p band relative to the Fermi level occurs with increasing x in La1-xSrxNiO3. This alloying step strengthens Ni 3d-O 2p hybridization and decreases the charge transfer energy, which in turn accounts for the enhanced OER activity.

Authors:

Liu, Jishan ^[1]; Jia, Endong ^[2]; Wang, Le  ^[3];

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Stoerzinger, Kelsey A. ^[4]; Zhou, Hua ^[5]; Tang, Chi Sin ^[6]; Yin, Xinmao ^[7]; He, Xu ^[8]; Bousquet, Eric ^[8]; Bowden, Mark E. ^[9]; Wee, Andrew T. S. ^[7]; Chambers, Scott A. ^[3]; Du, Yingge ^[3]

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1. State Key Laboratory of Functional Materials for InformaticsShanghai Institute of Microsystem and Information TechnologyChinese Academy of Sciences Shanghai 200050 China, Center for Excellence in Superconducting ElectronicsChinese Academy of Sciences Shanghai 200050 China, Physical and Computational Sciences DirectoratePacific Northwest National Laboratory Richland WA 99354 USA
2. Physical and Computational Sciences DirectoratePacific Northwest National Laboratory Richland WA 99354 USA, The Key Laboratory of Solar Thermal Energy and Photovoltaic SystemInstitute of Electrical EngineeringChinese Academy of Sciences Beijing 100190 China, Department of PhysicsUniversity of Chinese Academy of Sciences Beijing 100190 China
3. Physical and Computational Sciences DirectoratePacific Northwest National Laboratory Richland WA 99354 USA
4. Physical and Computational Sciences DirectoratePacific Northwest National Laboratory Richland WA 99354 USA, School of ChemicalBiological and Environmental EngineeringOregon State University Corvallis OR 97331 USA
5. X‐Ray Science DivisionAdvanced Photon SourceArgonne National Laboratory Lemont IL 60439 USA
6. Department of PhysicsFaculty of ScienceNational University of Singapore Singapore 117542 Singapore, NUS Graduate School for Integrative Sciences and EngineeringNational University of Singapore Singapore 117456 Singapore
7. Department of PhysicsFaculty of ScienceNational University of Singapore Singapore 117542 Singapore
8. Theoretical Materials PhysicsQ‐MATCesamUniversity of Liège B‐4000 Liège Belgium
9. Environmental Molecular Sciences LaboratoryPacific Northwest National Laboratory Richland WA 99354 USA

Publication Date:

Wed Aug 07 00:00:00 EDT 2019

Research Org.:

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1568921

Alternate Identifier(s):

OSTI ID: 1568923; OSTI ID: 1571524; OSTI ID: 1574233

Report Number(s):

PNNL-SA-141734
Journal ID: ISSN 2198-3844; 1901073

Grant/Contract Number:  

AC05-76RL01830; AC02-06CH11357

Resource Type:

Published Article

Journal Name:

Advanced Science

Additional Journal Information:

Journal Name: Advanced Science Journal Volume: 6 Journal Issue: 19; Journal ID: ISSN 2198-3844

Publisher:

Wiley

Country of Publication:

Germany

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nickelates; LaNiO3; oxygen evolution reaction; hole doping; hybridization