Water flipping and the oxygen evolution reaction on Fe2O3 nanolayers
Hematite photoanodes are promising for the oxygen evolution reaction, however, their high overpotential (0.5-0.6 V) for water oxidation and limited photocurrent make them economically unviable at present. The work needed to orient dipoles at an electrode surface may be an overlooked contribution to...
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| Published in | Nature communications Vol. 16; no. 1; pp. 3585 - 9 |
|---|---|
| Main Authors | , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
15.04.2025
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
| ISSN | 2041-1723 2041-1723 |
| DOI | 10.1038/s41467-025-58842-y |
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| Abstract | Hematite photoanodes are promising for the oxygen evolution reaction, however, their high overpotential (0.5-0.6 V) for water oxidation and limited photocurrent make them economically unviable at present. The work needed to orient dipoles at an electrode surface may be an overlooked contribution to the overpotential, especially regarding dipoles of water, the electron source in the oxygen evolution reaction (OER). Here, we employ second harmonic amplitude and phase measurements to quantify the number of net-aligned Stern layer water molecules and the work associated with water flipping, on hematite, an earth abundant OER semiconductor associated with a high overpotential. At zero applied bias, the pH-dependent potentials for Stern layer water molecule flipping exhibit Nernstian behavior. At positive applied potentials and pH 13, approximately one to two monolayers of water molecules points the oxygen atoms towards the electrode, favorable for the OER. The work associated with water flipping matches the cohesive energy of liquid water (44 kJ mol
-1
) and the OER current density is highest. This current is negligible at pH 5, where the work approaches 100 kJ mol
-1
. Our findings suggest a causal relationship between the need for Stern layer water flipping and the OER overpotential, which may lead to developing strategies for decreasing the latter.
Using second harmonic amplitude and phase measurements the authors characterize the alignment of water molecules in the Stern-layer and the work associated with water flipping on hematite electrodes, suggesting a causal relationship between water flipping and the oxygen evolution reaction overpotential. |
|---|---|
| AbstractList | Hematite photoanodes are promising for the oxygen evolution reaction, however, their high overpotential (0.5-0.6 V) for water oxidation and limited photocurrent make them economically unviable at present. The work needed to orient dipoles at an electrode surface may be an overlooked contribution to the overpotential, especially regarding dipoles of water, the electron source in the oxygen evolution reaction (OER). Here, we employ second harmonic amplitude and phase measurements to quantify the number of net-aligned Stern layer water molecules and the work associated with water flipping, on hematite, an earth abundant OER semiconductor associated with a high overpotential. At zero applied bias, the pH-dependent potentials for Stern layer water molecule flipping exhibit Nernstian behavior. At positive applied potentials and pH 13, approximately one to two monolayers of water molecules points the oxygen atoms towards the electrode, favorable for the OER. The work associated with water flipping matches the cohesive energy of liquid water (44 kJ mol-1) and the OER current density is highest. This current is negligible at pH 5, where the work approaches 100 kJ mol-1. Our findings suggest a causal relationship between the need for Stern layer water flipping and the OER overpotential, which may lead to developing strategies for decreasing the latter. Hematite photoanodes are promising for the oxygen evolution reaction, however, their high overpotential (0.5-0.6 V) for water oxidation and limited photocurrent make them economically unviable at present. The work needed to orient dipoles at an electrode surface may be an overlooked contribution to the overpotential, especially regarding dipoles of water, the electron source in the oxygen evolution reaction (OER). Here, we employ second harmonic amplitude and phase measurements to quantify the number of net-aligned Stern layer water molecules and the work associated with water flipping, on hematite, an earth abundant OER semiconductor associated with a high overpotential. At zero applied bias, the pH-dependent potentials for Stern layer water molecule flipping exhibit Nernstian behavior. At positive applied potentials and pH 13, approximately one to two monolayers of water molecules points the oxygen atoms towards the electrode, favorable for the OER. The work associated with water flipping matches the cohesive energy of liquid water (44 kJ mol -1 ) and the OER current density is highest. This current is negligible at pH 5, where the work approaches 100 kJ mol -1 . Our findings suggest a causal relationship between the need for Stern layer water flipping and the OER overpotential, which may lead to developing strategies for decreasing the latter. Using second harmonic amplitude and phase measurements the authors characterize the alignment of water molecules in the Stern-layer and the work associated with water flipping on hematite electrodes, suggesting a causal relationship between water flipping and the oxygen evolution reaction overpotential. Hematite photoanodes are promising for the oxygen evolution reaction, however, their high overpotential (0.5-0.6 V) for water oxidation and limited photocurrent make them economically unviable at present. The work needed to orient dipoles at an electrode surface may be an overlooked contribution to the overpotential, especially regarding dipoles of water, the electron source in the oxygen evolution reaction (OER). Here, we employ second harmonic amplitude and phase measurements to quantify the number of net-aligned Stern layer water molecules and the work associated with water flipping, on hematite, an earth abundant OER semiconductor associated with a high overpotential. At zero applied bias, the pH-dependent potentials for Stern layer water molecule flipping exhibit Nernstian behavior. At positive applied potentials and pH 13, approximately one to two monolayers of water molecules points the oxygen atoms towards the electrode, favorable for the OER. The work associated with water flipping matches the cohesive energy of liquid water (44 kJ mol-1) and the OER current density is highest. This current is negligible at pH 5, where the work approaches 100 kJ mol-1. Our findings suggest a causal relationship between the need for Stern layer water flipping and the OER overpotential, which may lead to developing strategies for decreasing the latter.Using second harmonic amplitude and phase measurements the authors characterize the alignment of water molecules in the Stern-layer and the work associated with water flipping on hematite electrodes, suggesting a causal relationship between water flipping and the oxygen evolution reaction overpotential. Abstract Hematite photoanodes are promising for the oxygen evolution reaction, however, their high overpotential (0.5-0.6 V) for water oxidation and limited photocurrent make them economically unviable at present. The work needed to orient dipoles at an electrode surface may be an overlooked contribution to the overpotential, especially regarding dipoles of water, the electron source in the oxygen evolution reaction (OER). Here, we employ second harmonic amplitude and phase measurements to quantify the number of net-aligned Stern layer water molecules and the work associated with water flipping, on hematite, an earth abundant OER semiconductor associated with a high overpotential. At zero applied bias, the pH-dependent potentials for Stern layer water molecule flipping exhibit Nernstian behavior. At positive applied potentials and pH 13, approximately one to two monolayers of water molecules points the oxygen atoms towards the electrode, favorable for the OER. The work associated with water flipping matches the cohesive energy of liquid water (44 kJ mol-1) and the OER current density is highest. This current is negligible at pH 5, where the work approaches 100 kJ mol-1. Our findings suggest a causal relationship between the need for Stern layer water flipping and the OER overpotential, which may lead to developing strategies for decreasing the latter. Hematite photoanodes are promising for the oxygen evolution reaction, however, their high overpotential (0.5-0.6 V) for water oxidation and limited photocurrent make them economically unviable at present. The work needed to orient dipoles at an electrode surface may be an overlooked contribution to the overpotential, especially regarding dipoles of water, the electron source in the oxygen evolution reaction (OER). Here, we employ second harmonic amplitude and phase measurements to quantify the number of net-aligned Stern layer water molecules and the work associated with water flipping, on hematite, an earth abundant OER semiconductor associated with a high overpotential. At zero applied bias, the pH-dependent potentials for Stern layer water molecule flipping exhibit Nernstian behavior. At positive applied potentials and pH 13, approximately one to two monolayers of water molecules points the oxygen atoms towards the electrode, favorable for the OER. The work associated with water flipping matches the cohesive energy of liquid water (44 kJ mol-1) and the OER current density is highest. This current is negligible at pH 5, where the work approaches 100 kJ mol-1. Our findings suggest a causal relationship between the need for Stern layer water flipping and the OER overpotential, which may lead to developing strategies for decreasing the latter.Hematite photoanodes are promising for the oxygen evolution reaction, however, their high overpotential (0.5-0.6 V) for water oxidation and limited photocurrent make them economically unviable at present. The work needed to orient dipoles at an electrode surface may be an overlooked contribution to the overpotential, especially regarding dipoles of water, the electron source in the oxygen evolution reaction (OER). Here, we employ second harmonic amplitude and phase measurements to quantify the number of net-aligned Stern layer water molecules and the work associated with water flipping, on hematite, an earth abundant OER semiconductor associated with a high overpotential. At zero applied bias, the pH-dependent potentials for Stern layer water molecule flipping exhibit Nernstian behavior. At positive applied potentials and pH 13, approximately one to two monolayers of water molecules points the oxygen atoms towards the electrode, favorable for the OER. The work associated with water flipping matches the cohesive energy of liquid water (44 kJ mol-1) and the OER current density is highest. This current is negligible at pH 5, where the work approaches 100 kJ mol-1. Our findings suggest a causal relationship between the need for Stern layer water flipping and the OER overpotential, which may lead to developing strategies for decreasing the latter. |
| ArticleNumber | 3585 |
| Author | Rosso, Kevin M. Martinson, Alex B. F. Boamah, Mavis D. Kupferberg, Jacob Bye, Justin Z. Zhao, Yatong Geiger, Franz M. Speelman, Raiden Marker, Ezra J. Engelhard, Mark |
| Author_xml | – sequence: 1 givenname: Raiden orcidid: 0000-0002-7856-9147 surname: Speelman fullname: Speelman, Raiden organization: Department of Chemistry, Northwestern University – sequence: 2 givenname: Ezra J. surname: Marker fullname: Marker, Ezra J. organization: Department of Chemistry, Northwestern University – sequence: 3 givenname: Mavis D. orcidid: 0000-0003-4457-4594 surname: Boamah fullname: Boamah, Mavis D. organization: Pacific Northwest National Laboratory – sequence: 4 givenname: Jacob surname: Kupferberg fullname: Kupferberg, Jacob organization: Materials Science Division, Argonne National Laboratory – sequence: 5 givenname: Justin Z. surname: Bye fullname: Bye, Justin Z. organization: Department of Chemistry, Northwestern University – sequence: 6 givenname: Mark orcidid: 0000-0002-5543-0812 surname: Engelhard fullname: Engelhard, Mark organization: Pacific Northwest National Laboratory – sequence: 7 givenname: Yatong surname: Zhao fullname: Zhao, Yatong organization: Pacific Northwest National Laboratory – sequence: 8 givenname: Alex B. F. orcidid: 0000-0003-3916-1672 surname: Martinson fullname: Martinson, Alex B. F. organization: Materials Science Division, Argonne National Laboratory – sequence: 9 givenname: Kevin M. orcidid: 0000-0002-8474-7720 surname: Rosso fullname: Rosso, Kevin M. organization: Pacific Northwest National Laboratory – sequence: 10 givenname: Franz M. orcidid: 0000-0001-8569-4045 surname: Geiger fullname: Geiger, Franz M. email: f-geiger@northwestern.edu organization: Department of Chemistry, Northwestern University |
| BackLink | https://www.osti.gov/servlets/purl/2566047$$D View this record in Osti.gov |
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| Snippet | Hematite photoanodes are promising for the oxygen evolution reaction, however, their high overpotential (0.5-0.6 V) for water oxidation and limited... Hematite photoanodes are promising for the oxygen evolution reaction, however, their high overpotential (0.5-0.6 V) for water oxidation and limited... Abstract Hematite photoanodes are promising for the oxygen evolution reaction, however, their high overpotential (0.5-0.6 V) for water oxidation and limited... |
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| SubjectTerms | 140/125 639/638/161 639/638/440/94 639/638/542 Amplitudes Dipoles Electrodes Evolution Ferric oxide Hematite Humanities and Social Sciences multidisciplinary Oxidation Oxygen Oxygen atoms Oxygen evolution reactions pH effects Phase measurement Photoanodes Photoelectric effect Science Science (multidisciplinary) Water Water chemistry |
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| Title | Water flipping and the oxygen evolution reaction on Fe2O3 nanolayers |
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