Active Motif Change of Ni-Fe Spinel Oxide by Ir Doping for Highly Durable and Facile Oxygen Evolution Reaction

被引：65

作者：

Hong, Sukhwa ^{[1
]}

Ham, Kahyun ^{[2
,3
,4
]}

Hwang, Jeemin ^{[5
]}

Kang, Sinwoo ^{[2
,3
]}

Seo, Min Ho ^{[6
]}

Choi, Young-Woo ^{[5
]}

Han, Byungchan ^{[7
]}

Lee, Jaeyoung ^{[2
,3
,4
]}

Cho, Kangwoo ^{[1
]}

机构：

[1] Pohang Univ Sci & Technol POSTECH, Div Environm Sci & Engn, 77 Cheongam Ro, Pohang 37673, South Korea

[2] Gwangju Inst Sci & Technol GIST, Sch Earth Sci & Environm Engn, 123 Cheomdangwagi Ro, Gwangju 61005, South Korea

[3] GIST, Int Future Res Ctr Chem Energy Storage & Convers, 123 Cheomdangwagi Ro, Gwangju 61005, South Korea

[4] GIST, Ertl Ctr Electrochem & Catalysis, 123 Cheomdangwagi Ro, Gwangju 61005, South Korea

[5] Korea Inst Energy Res KIER, Hydrogen Energy Res Div, Fuel Cell Res & Demonstrat Ctr, 20-41 Sinjaesaengene Ro, Buan Gun 56332, Jeollabuk Do, South Korea

[6] Pukyong Natl Univ, Dept Nanotechnol Engn, 45 Yongso Ro, Busan 48547, South Korea

[7] Yonsei Univ, Dept Chem & Biomol Engn, 50 Yonsei Ro Seodaemun Gu, Seoul 03722, South Korea

来源：

ADVANCED FUNCTIONAL MATERIALS | 2023年 / 33卷 / 01期

基金：

新加坡国家研究基金会;

关键词：

density functional theory calculation; doping effect; in situ X-ray absorption spectroscopy; oxygen evolution reaction; spinel oxide; REACTION DYNAMICS; WATER OXIDATION; REDOX STATES; ELECTROCATALYSTS; STABILITY; CATALYSTS; EFFICIENCY; MECHANISM; MOSSBAUER; ORIGIN;

D O I：

10.1002/adfm.202209543

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The oxygen evolution reaction (OER) is crucial for producing sustainable energy carriers. Herein, Ir (5 mol.%) doped inverse-spinel NiFe2O4 (Ir-NFO) nanoparticles deposited on Ni foam (NF) by scalable solution casting are considered a promising OER electrocatalyst for industrial deployments. The Ir-NFO/NF (with minimal lattice distortion by uniform Ir doping) provides an OER overpotential of 251 mV (intrinsically outperforming NFO/NF and benchmarking IrO2/NF) and extraordinary robustness over 130 days at 100 mA cm(-2). In situ X-ray absorption spectroscopy reveals oxidation only for Fe on NFO, whereas concurrent generation of higher-valent Ni and Fe occurs on Ir-NFO during OER. Density functional theory calculations further demonstrate that Ir substitutes the sublayer Ni octahedral site and switches the main active reaction center from Fe-Oh-Fe-Td bridge site (Fe-O-Fe) on NFO to Ni-Oh-Fe-Td bridge site (Ni-O-Fe active motif) on Ir-NFO for a co-catalytic OER. This study sheds new light on precious-metal doped Ni-Fe oxides, which may be applicable to other binary/ternary oxide electrocatalysts.

引用

页数：11

共 58 条

[1] Mossbauer, Raman and X-ray diffraction studies of superparamagnetic NiFe2O4 nanoparticles prepared by sol-gel auto-combustion method [J].