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

被引：25
作者：
Ismail, Ahmed S. M. [1 ]
Garcia-Torregrosa, Ivan [1 ,2 ]
Vollenbroek, Jeroen C. [3 ]
Folkertsma, Laura [2 ]
Bomer, Johan G. [3 ]
Haarman, Ties [1 ]
Ghiasi, Mahnaz [1 ]
Schellhorn, Meike [4 ]
Nachtegaal, Maarten [5 ]
Odijk, Mathieu [3 ]
van den Berg, Albert [3 ]
Weckhuysen, Bert M. [1 ]
de Groot, Frank M. F. [1 ]
机构：
[1] Univ Utrecht, Inorgan Chem & Catalysis Grp, NL-3584 CG Utrecht, Netherlands
[2] TNO Energy Transit, NL-1755 LE Petten, Netherlands
[3] Univ Twente, MESA Inst Nanotechnol, BIOS Lab Chip Grp, NL-7522 NB Enschede, Netherlands
[4] Laser Lab Gottingen eV, Opt Short Wavelengths Dept, D-37077 Gottingen, Germany
[5] Paul Scherrer Inst, CH-5232 Villigen, Switzerland
来源：
ACS CATALYSIS | 2021年 / 11卷 / 19期
关键词：
water splitting; catalysts; operando X-ray spectroscopy; nickel iron oxyhydroxide; hematite; interface; iron oxyhydroxide; OXYGEN EVOLUTION REACTION; OXIDE CATALYSTS; OXIDATION; ELECTROCATALYSTS; BIVO4; PHOTOANODES; PERFORMANCE; ORIGIN;
D O I：
10.1021/acscatal.1c02566
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
The role that the alpha-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 alpha-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.
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页码：12324 / 12335
页数：12
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