Detection of Spontaneous FeOOH Formation at the Hematite/Ni(Fe)OOH Interface During Photoelectrochemical Water Splitting by Operando X‑ray Absorption Spectroscopy

The role that the α-Fe2O3/NiFeOOH interface plays in dictating the oxygen evolution reaction (OER) mechanism on hematite has been a source of intense debate for decades, but the chemical characteristics of this interface and its function are still ambiguous and subject to speculation. In this study,...

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Published inACS catalysis Vol. 11; no. 19; pp. 12324 - 12335
Main Authors Ismail, Ahmed S. M, Garcia-Torregrosa, Ivan, Vollenbroek, Jeroen C, Folkertsma, Laura, Bomer, Johan G, Haarman, Ties, Ghiasi, Mahnaz, Schellhorn, Meike, Nachtegaal, Maarten, Odijk, Mathieu, van den Berg, Albert, Weckhuysen, Bert M, de Groot, Frank M. F
Format Journal Article
LanguageEnglish
Published American Chemical Society 01.10.2021
Subjects
iron oxyhydroxide
water splitting
catalysts
hematite
interface
operando X-ray spectroscopy
nickel iron oxyhydroxide
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Abstract The role that the α-Fe2O3/NiFeOOH interface plays in dictating the oxygen evolution reaction (OER) mechanism on hematite has been a source of intense debate for decades, but the chemical characteristics of this interface and its function are still ambiguous and subject to speculation. In this study, we employed operando X-ray absorption spectroscopy to investigate the interfacial dynamics at the α-Fe2O3/NiFeOOH interface. We uncovered the spontaneous formation of a FeOOH interfacial layer under (photo)­electrochemical conditions. This FeOOH interfacial layer plays a role in the surface passivation of hematite and in accumulating the (photo)­generated holes upon external potential application. This hole-accumulation process leads to the extraction of more (photo)­generated holes from hematite before releasing them to NiFeOOH to carry out the water-splitting reaction, and it also explains the reason for the delay in the nickel oxidation process. Based on these observations, we propose a model where NiFeOOH acts mainly as an OER catalyst and a facilitator of holes extraction from hematite, while the interfacial FeOOH layer acts as a surface passivation and hole-accumulation overlayer.
AbstractList The role that the α-Fe2O3/NiFeOOH interface plays in dictating the oxygen evolution reaction (OER) mechanism on hematite has been a source of intense debate for decades, but the chemical characteristics of this interface and its function are still ambiguous and subject to speculation. In this study, we employed operando X-ray absorption spectroscopy to investigate the interfacial dynamics at the α-Fe2O3/NiFeOOH interface. We uncovered the spontaneous formation of a FeOOH interfacial layer under (photo)­electrochemical conditions. This FeOOH interfacial layer plays a role in the surface passivation of hematite and in accumulating the (photo)­generated holes upon external potential application. This hole-accumulation process leads to the extraction of more (photo)­generated holes from hematite before releasing them to NiFeOOH to carry out the water-splitting reaction, and it also explains the reason for the delay in the nickel oxidation process. Based on these observations, we propose a model where NiFeOOH acts mainly as an OER catalyst and a facilitator of holes extraction from hematite, while the interfacial FeOOH layer acts as a surface passivation and hole-accumulation overlayer.
Author Vollenbroek, Jeroen C
Bomer, Johan G
Ismail, Ahmed S. M
Nachtegaal, Maarten
de Groot, Frank M. F
Schellhorn, Meike
Odijk, Mathieu
Weckhuysen, Bert M
Haarman, Ties
Ghiasi, Mahnaz
Folkertsma, Laura
van den Berg, Albert
Garcia-Torregrosa, Ivan
AuthorAffiliation Optics/Short Wavelengths Department
BIOS Lab on a Chip Group, MESA+ Institute of Nanotechnology
Paul Scherrer Institute
Inorganic Chemistry and Catalysis Group
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Keywords iron oxyhydroxide
water splitting
catalysts
hematite
interface
operando X-ray spectroscopy
nickel iron oxyhydroxide
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Snippet The role that the α-Fe2O3/NiFeOOH interface plays in dictating the oxygen evolution reaction (OER) mechanism on hematite has been a source of intense debate...
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Title Detection of Spontaneous FeOOH Formation at the Hematite/Ni(Fe)OOH Interface During Photoelectrochemical Water Splitting by Operando X‑ray Absorption Spectroscopy
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