Thickness dependent OER electrocatalysis of epitaxial thin film of high entropy oxide

Patel, Ranjan Kumar; Jenjeti, Ramesh Naidu; Kumar, Rajat; Bhattacharya, Nandana; Kumar, Siddharth; Ojha, Shashank Kumar; Zhang, Zhan; Zhou, Hua; Qu, Ke; Wang, Zhen; Yang, Zhenzhong; Klewe, Christoph; Shafer, Padraic; Sampath, S.; Middey, Srimanta

doi:10.1063/5.0146005

Thickness dependent OER electrocatalysis of epitaxial thin film of high entropy oxide

Journal Article · Tue Aug 01 00:00:00 EDT 2023 · Applied Physics Reviews

DOI:https://doi.org/10.1063/5.0146005· OSTI ID:2294104

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Department of Physics, Indian Institute of Science 1 , Bengaluru 560012, India
Department of Inorganic and Physical Chemistry, Indian Institute of Science 2 , Bengaluru 560012, India
Advanced Photon Source, Argonne National Laboratory 3 , Lemont, Illinois 60439, USA
Key Laboratory of Polar Materials and Devices, East China Normal University Shanghai 4 , Shanghai 200241, China
Advanced Light Source, Lawrence Berkeley National Laboratory 5 , Berkeley, California 94720, USA

High entropy oxides (HEOs), which contain multiple elements in the same crystallographic site, are a promising platform for electrocatalysis in oxygen evolution reaction (OER). Investigating these materials in epitaxial thin film form expands the possibility of tuning OER activity by several means, which are not realizable in polycrystalline samples. To date, very few such studies have been reported. In this work, the OER activity of single-crystalline thin films of (La_0.2Pr_0.2Nd_0.2Sm_0.2Eu_0.2)NiO₃, grown on NdGaO₃ substrates have been investigated in 0.1 M KOH electrolyte as a function of film thickness. The OER activity increases with the thickness of the film. X-ray absorption spectroscopy measurements find an increase in Ni $$d$$-O $$p$$ covalency and a decrease in charge transfer energy with the increase in film thickness. These facilitate higher charge transfer between Ni and surface adsorbates, increasing OER activity. However, the OER process leads to excessive leaching of thicker films and the OER activity of a 75 unit cell thick film is found to be optimal in the present study. In conclusion, this work demonstrates that the thickness of perovskite oxides can be used as a parameter to enhance OER activity.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Natural Science Foundation of China (NSFC); Science and Engineering Research Board (SERB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 2294104

Alternate ID(s):: OSTI ID: 2342143
OSTI ID: 2294105

Journal Information:: Applied Physics Reviews, Journal Name: Applied Physics Reviews Journal Issue: 3 Vol. 10; ISSN 1931-9401

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Epitaxial stabilization of ultra thin films of high entropy perovskite

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