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

Ahmed S.M. Ismail; Ivan Garcia-Torregrosa; Jeroen C. Vollenbroek; Laura Folkertsma; Johan G. Bomer; Ties Haarman; Mahnaz Ghiasi; Meike Schellhorn; Maarten Nachtegaal; Mathieu Odijk; Albert van den Berg; Bert M. Weckhuysen; Frank M.F. De Groot

doi:10.1021/acscatal.1c02566

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

Ahmed S.M. Ismail^*, Ivan Garcia-Torregrosa, Jeroen C. Vollenbroek, Laura Folkertsma, Johan G. Bomer, Ties Haarman, Mahnaz Ghiasi, Meike Schellhorn, Maarten Nachtegaal, Mathieu Odijk, Albert van den Berg, Bert M. Weckhuysen, Frank M.F. De Groot^*

^*Corresponding author for this work

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

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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.

Original language	English
Pages (from-to)	12324-12335
Number of pages	12
Journal	ACS catalysis
Volume	11
Issue number	19
Early online date	20 Sept 2021
DOIs	https://doi.org/10.1021/acscatal.1c02566
Publication status	Published - 1 Oct 2021

Keywords

2022 OA procedure
hematite
interface
iron oxyhydroxide
nickel iron oxyhydroxide
operando X-ray spectroscopy
water splitting
catalysts

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10.1021/acscatal.1c02566

Ismail-2021-Detection-of-spontaneous-feooh-formFinal published version, 3.03 MBLicence: Taverne

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Ismail, A. S. M., Garcia-Torregrosa, I., Vollenbroek, J. C., Folkertsma, L., Bomer, J. G., Haarman, T., Ghiasi, M., Schellhorn, M., Nachtegaal, M., Odijk, M., van den Berg, A., Weckhuysen, B. M., & De Groot, F. M. F. (2021). Detection of Spontaneous FeOOH Formation at the Hematite/Ni(Fe)OOH Interface during Photoelectrochemical Water Splitting by Operando X-ray Absorption Spectroscopy. ACS catalysis, 11(19), 12324-12335. https://doi.org/10.1021/acscatal.1c02566

@article{3a57d77d537249ac920004d7f28a230e,

title = "Detection of Spontaneous FeOOH Formation at the Hematite/Ni(Fe)OOH Interface during Photoelectrochemical Water Splitting by Operando X-ray Absorption Spectroscopy",

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. ",

keywords = "2022 OA procedure, hematite, interface, iron oxyhydroxide, nickel iron oxyhydroxide, operando X-ray spectroscopy, water splitting, catalysts",

author = "Ismail, {Ahmed S.M.} and Ivan Garcia-Torregrosa and Vollenbroek, {Jeroen C.} and Laura Folkertsma and Bomer, {Johan G.} and Ties Haarman and Mahnaz Ghiasi and Meike Schellhorn and Maarten Nachtegaal and Mathieu Odijk and {van den Berg}, Albert and Weckhuysen, {Bert M.} and {De Groot}, {Frank M.F.}",

note = "Funding Information: This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation programme funded by the Ministry of Education, Culture, and Science of the Government of the Netherlands. This project has also received partial funding from the EU-H2020 Research and Innovation Programme under Grant Agreement No. 654360, having benefitted from the access provided by the Paul Scherrer Institute, Villigen, Switzerland, to the SuperXAS beamline at the SLS within the framework of the NFFA-Europe Transnational Access Activity. Publisher Copyright: {\textcopyright} 2021 American Chemical Society.",

year = "2021",

month = oct,

day = "1",

doi = "10.1021/acscatal.1c02566",

language = "English",

volume = "11",

pages = "12324--12335",

journal = "ACS catalysis",

issn = "2155-5435",

publisher = "American Chemical Society",

number = "19",

}

Ismail, ASM, Garcia-Torregrosa, I, Vollenbroek, JC, Folkertsma, L, Bomer, JG, Haarman, T, Ghiasi, M, Schellhorn, M, Nachtegaal, M, Odijk, M , van den Berg, A, Weckhuysen, BM & De Groot, FMF 2021, 'Detection of Spontaneous FeOOH Formation at the Hematite/Ni(Fe)OOH Interface during Photoelectrochemical Water Splitting by Operando X-ray Absorption Spectroscopy', ACS catalysis, vol. 11, no. 19, pp. 12324-12335. https://doi.org/10.1021/acscatal.1c02566

Detection of Spontaneous FeOOH Formation at the Hematite/Ni(Fe)OOH Interface during Photoelectrochemical Water Splitting by Operando X-ray Absorption Spectroscopy. / Ismail, Ahmed S.M.; Garcia-Torregrosa, Ivan; Vollenbroek, Jeroen C. et al.
In: ACS catalysis, Vol. 11, No. 19, 01.10.2021, p. 12324-12335.

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

TY - JOUR

T1 - Detection of Spontaneous FeOOH Formation at the Hematite/Ni(Fe)OOH Interface during Photoelectrochemical Water Splitting by Operando X-ray Absorption Spectroscopy

AU - Ismail, Ahmed S.M.

AU - Garcia-Torregrosa, Ivan

AU - Vollenbroek, Jeroen C.

AU - Folkertsma, Laura

AU - Bomer, Johan G.

AU - Haarman, Ties

AU - Ghiasi, Mahnaz

AU - Schellhorn, Meike

AU - Nachtegaal, Maarten

AU - Odijk, Mathieu

AU - van den Berg, Albert

AU - Weckhuysen, Bert M.

AU - De Groot, Frank M.F.

N1 - Funding Information: This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation programme funded by the Ministry of Education, Culture, and Science of the Government of the Netherlands. This project has also received partial funding from the EU-H2020 Research and Innovation Programme under Grant Agreement No. 654360, having benefitted from the access provided by the Paul Scherrer Institute, Villigen, Switzerland, to the SuperXAS beamline at the SLS within the framework of the NFFA-Europe Transnational Access Activity. Publisher Copyright: © 2021 American Chemical Society.

PY - 2021/10/1

Y1 - 2021/10/1

N2 - 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.

AB - 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.

KW - 2022 OA procedure

KW - hematite

KW - interface

KW - iron oxyhydroxide

KW - nickel iron oxyhydroxide

KW - operando X-ray spectroscopy

KW - water splitting

KW - catalysts

UR - http://www.scopus.com/inward/record.url?scp=85116698132&partnerID=8YFLogxK

U2 - 10.1021/acscatal.1c02566

DO - 10.1021/acscatal.1c02566

M3 - Article

AN - SCOPUS:85116698132

SN - 2155-5435

VL - 11

SP - 12324

EP - 12335

JO - ACS catalysis

JF - ACS catalysis

IS - 19

ER -

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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