Breaking OER and CER scaling relations via strain and its relaxation in RuO2 (101)

Prajwal Adiga; William Nunn; Cindy Wong; Anusha K. Manjeshwar; Sreejith Nair; Bharat Jalan; Kelsey A. Stoerzinger

doi:10.1016/j.mtener.2022.101087

Breaking OER and CER scaling relations via strain and its relaxation in RuO₂ (101)

Prajwal Adiga, William Nunn, Cindy Wong, Anusha K. Manjeshwar, Sreejith Nair, Bharat Jalan, Kelsey A. Stoerzinger

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

Green hydrogen production from abundant water sources is an important component of renewable energy storage. Water oxidation catalysts are typically considered bound by adsorbate scaling relations, limiting their activity for the oxygen evolution reaction (OER) as well as selectivity between OER and the chlorine evolution reaction (CER) that compete in saline water streams. RuO₂ is highly active for both reactions, and recent measurements have shown that the OER activity is greater on undercoordinated, high index facets compared to the lowest energy (110) facet often studied. The growth of such orientations as epitaxial films, however, can result in appreciable strain and potential surface faceting via its relaxation. We find the activity and selectivity toward OER and CER vary with thickness in epitaxial (101) RuO₂ thin films: OER activity decreases four times as film thickness increases from 8 nm to 48 nm, while CER activity is comparable. Thus, strain and its relaxation can be used to break scaling relationships between OER and CER, highlighting the important role that defects play in selective oxidation processes on RuO₂ in chloride-containing media.

Original language	English (US)
Article number	101087
Pages (from-to)	101087
Journal	Materials Today Energy
Volume	28
DOIs	https://doi.org/10.1016/j.mtener.2022.101087 https://doi.org/10.1016/j.mtener.2022.101087
State	Published - Aug 2022

Bibliographical note

Funding Information:
This material is based upon work supported by the National Science Foundation under Grant No. 2041153 . P.A. acknowledges support from the Link Foundation Energy Fellowship. K.A.S. acknowledges support from Oregon State University as a Callahan Faculty Scholar. The work at the UMN was supported primarily by the National Science Foundation through the University of Minnesota MRSEC under Award Number DMR-2011401 . A.K.M and W.N. acknowledge support from the U.S. DOE through DE-SC002021 and Air Force Office of Scientific Research ( AFOSR ) through Grants FA9550-21-1-0025 , respectively. Part of this work was also carried out in the College of Science and Engineering Characterization Facility, University of Minnesota , which has received capital equipment funding from the NSF through the UMN MRSEC program. W. N. also acknowledges support from the Vannevar Bush Faculty Fellowship.

Publisher Copyright:
© 2022 Elsevier Ltd

Keywords

Chlorine evolution reaction
Defects
Epitaxial thin films
Oxygen evolution reaction
Rutile

MRSEC Support

Partial

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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https://linkinghub.elsevier.com/retrieve/pii/S2468606922001459

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Cite this

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title = "Breaking OER and CER scaling relations via strain and its relaxation in RuO2 (101)",

abstract = "Green hydrogen production from abundant water sources is an important component of renewable energy storage. Water oxidation catalysts are typically considered bound by adsorbate scaling relations, limiting their activity for the oxygen evolution reaction (OER) as well as selectivity between OER and the chlorine evolution reaction (CER) that compete in saline water streams. RuO2 is highly active for both reactions, and recent measurements have shown that the OER activity is greater on undercoordinated, high index facets compared to the lowest energy (110) facet often studied. The growth of such orientations as epitaxial films, however, can result in appreciable strain and potential surface faceting via its relaxation. We find the activity and selectivity toward OER and CER vary with thickness in epitaxial (101) RuO2 thin films: OER activity decreases four times as film thickness increases from 8 nm to 48 nm, while CER activity is comparable. Thus, strain and its relaxation can be used to break scaling relationships between OER and CER, highlighting the important role that defects play in selective oxidation processes on RuO2 in chloride-containing media.",

keywords = "Chlorine evolution reaction, Defects, Epitaxial thin films, Oxygen evolution reaction, Rutile",

author = "Prajwal Adiga and William Nunn and Cindy Wong and Manjeshwar, {Anusha K.} and Sreejith Nair and Bharat Jalan and Stoerzinger, {Kelsey A.}",

note = "Funding Information: This material is based upon work supported by the National Science Foundation under Grant No. 2041153 . P.A. acknowledges support from the Link Foundation Energy Fellowship. K.A.S. acknowledges support from Oregon State University as a Callahan Faculty Scholar. The work at the UMN was supported primarily by the National Science Foundation through the University of Minnesota MRSEC under Award Number DMR-2011401 . A.K.M and W.N. acknowledge support from the U.S. DOE through DE-SC002021 and Air Force Office of Scientific Research ( AFOSR ) through Grants FA9550-21-1-0025 , respectively. Part of this work was also carried out in the College of Science and Engineering Characterization Facility, University of Minnesota , which has received capital equipment funding from the NSF through the UMN MRSEC program. W. N. also acknowledges support from the Vannevar Bush Faculty Fellowship. Publisher Copyright: {\textcopyright} 2022 Elsevier Ltd",

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month = aug,

doi = "10.1016/j.mtener.2022.101087",

language = "English (US)",

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AU - Adiga, Prajwal

AU - Nunn, William

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AU - Manjeshwar, Anusha K.

AU - Nair, Sreejith

AU - Jalan, Bharat

AU - Stoerzinger, Kelsey A.

N1 - Funding Information: This material is based upon work supported by the National Science Foundation under Grant No. 2041153 . P.A. acknowledges support from the Link Foundation Energy Fellowship. K.A.S. acknowledges support from Oregon State University as a Callahan Faculty Scholar. The work at the UMN was supported primarily by the National Science Foundation through the University of Minnesota MRSEC under Award Number DMR-2011401 . A.K.M and W.N. acknowledge support from the U.S. DOE through DE-SC002021 and Air Force Office of Scientific Research ( AFOSR ) through Grants FA9550-21-1-0025 , respectively. Part of this work was also carried out in the College of Science and Engineering Characterization Facility, University of Minnesota , which has received capital equipment funding from the NSF through the UMN MRSEC program. W. N. also acknowledges support from the Vannevar Bush Faculty Fellowship. Publisher Copyright: © 2022 Elsevier Ltd

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N2 - Green hydrogen production from abundant water sources is an important component of renewable energy storage. Water oxidation catalysts are typically considered bound by adsorbate scaling relations, limiting their activity for the oxygen evolution reaction (OER) as well as selectivity between OER and the chlorine evolution reaction (CER) that compete in saline water streams. RuO2 is highly active for both reactions, and recent measurements have shown that the OER activity is greater on undercoordinated, high index facets compared to the lowest energy (110) facet often studied. The growth of such orientations as epitaxial films, however, can result in appreciable strain and potential surface faceting via its relaxation. We find the activity and selectivity toward OER and CER vary with thickness in epitaxial (101) RuO2 thin films: OER activity decreases four times as film thickness increases from 8 nm to 48 nm, while CER activity is comparable. Thus, strain and its relaxation can be used to break scaling relationships between OER and CER, highlighting the important role that defects play in selective oxidation processes on RuO2 in chloride-containing media.

AB - Green hydrogen production from abundant water sources is an important component of renewable energy storage. Water oxidation catalysts are typically considered bound by adsorbate scaling relations, limiting their activity for the oxygen evolution reaction (OER) as well as selectivity between OER and the chlorine evolution reaction (CER) that compete in saline water streams. RuO2 is highly active for both reactions, and recent measurements have shown that the OER activity is greater on undercoordinated, high index facets compared to the lowest energy (110) facet often studied. The growth of such orientations as epitaxial films, however, can result in appreciable strain and potential surface faceting via its relaxation. We find the activity and selectivity toward OER and CER vary with thickness in epitaxial (101) RuO2 thin films: OER activity decreases four times as film thickness increases from 8 nm to 48 nm, while CER activity is comparable. Thus, strain and its relaxation can be used to break scaling relationships between OER and CER, highlighting the important role that defects play in selective oxidation processes on RuO2 in chloride-containing media.

KW - Chlorine evolution reaction

KW - Defects

KW - Epitaxial thin films

KW - Oxygen evolution reaction

KW - Rutile

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JO - Materials Today Energy

JF - Materials Today Energy

M1 - 101087

ER -

Breaking OER and CER scaling relations via strain and its relaxation in RuO₂ (101)

Abstract

Bibliographical note

Keywords

MRSEC Support

UN SDGs

Publisher link

Find It

Other files and links

Fingerprint

University of Minnesota Materials Research Science and Engineering Center (DMR-2011401)

IRG-1: Ionic Control of Materials

X-ray Diffraction and Atomic Force Microscopy of RuO2 thin films

Cite this

Breaking OER and CER scaling relations via strain and its relaxation in RuO2 (101)

Abstract

Bibliographical note

Keywords

MRSEC Support

UN SDGs

Publisher link

Find It

Other files and links

Fingerprint

Projects

University of Minnesota Materials Research Science and Engineering Center (DMR-2011401)

IRG-1: Ionic Control of Materials

Datasets

X-ray Diffraction and Atomic Force Microscopy of RuO2 thin films

Cite this

Breaking OER and CER scaling relations via strain and its relaxation in RuO₂ (101)