In Situ Reconstruction of High‐Entropy Heterostructure Catalysts for Stable Oxygen Evolution Electrocatalysis under Industrial Conditions

Author:

Hu Jue123,Guo Tianqi4,Zhong Xinyu56,Li Jiong5,Mei Yunjie12,Zhang Chengxu1ORCID,Feng Yuebin7,Sun Mingzi8,Meng Lijian9,Wang Zhiyuan12,Huang Bolong8,Zhang Libo123,Wang Zhongchang4ORCID

Affiliation:

1. Faculty of Metallurgical and Energy Engineering Kunming University of Science and Technology Kunming 650093 China

2. Key Laboratory of Unconventional Metallurgy Kunming University of Science and Technology Kunming 650093 China

3. Southwest United Graduate School Kunming 650092 China

4. International Iberian Nanotechnology Laboratory (INL) Braga 4715‐330 Portugal

5. Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 China

6. University of Chinese Academy of Sciences Beijing 100049 China

7. Faculty of Science Kunming University of Science and Technology Kunming 650093 China

8. Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University Hung Hom, Kowloon Hong Kong SAR China

9. CIETI, ISEP, Polytechnic of Porto, Rua Sr. António Bernardino de Almeida Porto 4249‐015 Portugal

Abstract

AbstractDespite of urgent needs for highly stable and efficient electrochemical water‐splitting devices, it remains extremely challenging to acquire highly stable oxygen evolution reaction (OER) electrocatalysts under harsh industrial conditions. Here, a successful in situ synthesis of FeCoNiMnCr high‐entropy alloy (HEA) and high‐entropy oxide (HEO) heterocatalysts via a Cr‐induced spontaneous reconstruction strategy is reported, and it is demonstrated that they deliver excellent ultrastable OER electrocatalytic performance with a low overpotential of 320 mV at 500 mA cm−2 and a negligible activity loss after maintaining at 100 mA cm−2 for 240 h. Remarkably, the heterocatalyst holds outstanding long‐term stability under harsh industrial condition of 6 m KOH and 85 °C at a current density of as high as 500 mA cm−2 over 500 h. Density functional theory calculations reveal that the formation of the HEA‐HEO heterostructure can provide electroactive sites possessing robust valence states to guarantee long‐term stable OER process, leading to the enhancement of electroactivity. The findings of such highly stable OER heterocatalysts under industrial conditions offer a new perspective for designing and constructing efficient high‐entropy electrocatalysts for practical industrial water splitting.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Guangdong Province

European Research Executive Agency

Publisher

Wiley

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