Entropy Engineering Activates Cu‐Fe Inertia Center From Prussian Blue Analogs With Micro‐Strains for Oxygen Electrocatalysis in Zn‐Air Batteries

ABSTRACT By the random distribution of metals in a single phase, entropy engineering is applied to construct dense neighboring active centers with diverse electronic and geometric structures, realizing the continuous optimization of multiple primary reactions for oxygen reduction reaction (ORR) and...

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Main Authors: Han Man, Guanyu Chen, Fengmei Wang, Jiafeng Ruan, Yihao Liu, Yang Liu, Fang Fang, Renchao Che
Format: Article
Language:English
Published: Wiley 2025-05-01
Series:Carbon Energy
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Online Access:https://doi.org/10.1002/cey2.693
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author Han Man
Guanyu Chen
Fengmei Wang
Jiafeng Ruan
Yihao Liu
Yang Liu
Fang Fang
Renchao Che
author_facet Han Man
Guanyu Chen
Fengmei Wang
Jiafeng Ruan
Yihao Liu
Yang Liu
Fang Fang
Renchao Che
author_sort Han Man
collection DOAJ
description ABSTRACT By the random distribution of metals in a single phase, entropy engineering is applied to construct dense neighboring active centers with diverse electronic and geometric structures, realizing the continuous optimization of multiple primary reactions for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Many catalysts developed through entropy engineering have been built in nearly equimolar ratios to pursue high entropy, hindering the identification of the active sites and potentially diluting the concentration of real active sites while weakening their electronic interactions with reaction intermediates. Herein, this work proposes an entropy‐engineering strategy in metal nanoparticle‐embedded nitrogen carbon electrocatalysts, implemented by entropy‐engineered Prussian blue analogs (PBA) as precursors to enhance the catalytic activity of primary Cu‐Fe active sites. Through the introduction of the micro‐strains driven by entropy engineering, density functional theory (DFT) calculations and geometric phase analysis (GPA) using Lorentz electron microscopy further elucidate the optimization of the adsorption/desorption of intermediates. Furthermore, the multi‐dimensional morphology and the size diminishment of the nanocrystals serve to expand the electrochemical area, maximizing the catalytic activity for both ORR and OER. Notably, the Zn‐air battery assembled with CuFeCoNiZn‐NC operated for over 1300 h with negligible decay. This work presents a paradigm for the design of low‐cost electrocatalysts with entropy engineering for multi‐step reactions.
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issn 2637-9368
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publisher Wiley
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spelling doaj-art-2fc0ca7eb9bf4ee5ba36fb4c36ce096a2025-08-20T02:34:27ZengWileyCarbon Energy2637-93682025-05-0175n/an/a10.1002/cey2.693Entropy Engineering Activates Cu‐Fe Inertia Center From Prussian Blue Analogs With Micro‐Strains for Oxygen Electrocatalysis in Zn‐Air BatteriesHan Man0Guanyu Chen1Fengmei Wang2Jiafeng Ruan3Yihao Liu4Yang Liu5Fang Fang6Renchao Che7Department of Materials Science Fudan University Shanghai ChinaLaboratory of Advanced Materials, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, Academy for Engineering & Technology Advanced Coatings Research Center of Ministry of Education of China Fudan University Shanghai ChinaDepartment of Materials Science Fudan University Shanghai ChinaDepartment of Materials Science Fudan University Shanghai ChinaLaboratory of Advanced Materials, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, Academy for Engineering & Technology Advanced Coatings Research Center of Ministry of Education of China Fudan University Shanghai ChinaDepartment of Materials Science Fudan University Shanghai ChinaDepartment of Materials Science Fudan University Shanghai ChinaLaboratory of Advanced Materials, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, Academy for Engineering & Technology Advanced Coatings Research Center of Ministry of Education of China Fudan University Shanghai ChinaABSTRACT By the random distribution of metals in a single phase, entropy engineering is applied to construct dense neighboring active centers with diverse electronic and geometric structures, realizing the continuous optimization of multiple primary reactions for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Many catalysts developed through entropy engineering have been built in nearly equimolar ratios to pursue high entropy, hindering the identification of the active sites and potentially diluting the concentration of real active sites while weakening their electronic interactions with reaction intermediates. Herein, this work proposes an entropy‐engineering strategy in metal nanoparticle‐embedded nitrogen carbon electrocatalysts, implemented by entropy‐engineered Prussian blue analogs (PBA) as precursors to enhance the catalytic activity of primary Cu‐Fe active sites. Through the introduction of the micro‐strains driven by entropy engineering, density functional theory (DFT) calculations and geometric phase analysis (GPA) using Lorentz electron microscopy further elucidate the optimization of the adsorption/desorption of intermediates. Furthermore, the multi‐dimensional morphology and the size diminishment of the nanocrystals serve to expand the electrochemical area, maximizing the catalytic activity for both ORR and OER. Notably, the Zn‐air battery assembled with CuFeCoNiZn‐NC operated for over 1300 h with negligible decay. This work presents a paradigm for the design of low‐cost electrocatalysts with entropy engineering for multi‐step reactions.https://doi.org/10.1002/cey2.693Prussian blue analogstrainstransition metal‐based catalystzinc‐air battery
spellingShingle Han Man
Guanyu Chen
Fengmei Wang
Jiafeng Ruan
Yihao Liu
Yang Liu
Fang Fang
Renchao Che
Entropy Engineering Activates Cu‐Fe Inertia Center From Prussian Blue Analogs With Micro‐Strains for Oxygen Electrocatalysis in Zn‐Air Batteries
Carbon Energy
Prussian blue analog
strains
transition metal‐based catalyst
zinc‐air battery
title Entropy Engineering Activates Cu‐Fe Inertia Center From Prussian Blue Analogs With Micro‐Strains for Oxygen Electrocatalysis in Zn‐Air Batteries
title_full Entropy Engineering Activates Cu‐Fe Inertia Center From Prussian Blue Analogs With Micro‐Strains for Oxygen Electrocatalysis in Zn‐Air Batteries
title_fullStr Entropy Engineering Activates Cu‐Fe Inertia Center From Prussian Blue Analogs With Micro‐Strains for Oxygen Electrocatalysis in Zn‐Air Batteries
title_full_unstemmed Entropy Engineering Activates Cu‐Fe Inertia Center From Prussian Blue Analogs With Micro‐Strains for Oxygen Electrocatalysis in Zn‐Air Batteries
title_short Entropy Engineering Activates Cu‐Fe Inertia Center From Prussian Blue Analogs With Micro‐Strains for Oxygen Electrocatalysis in Zn‐Air Batteries
title_sort entropy engineering activates cu fe inertia center from prussian blue analogs with micro strains for oxygen electrocatalysis in zn air batteries
topic Prussian blue analog
strains
transition metal‐based catalyst
zinc‐air battery
url https://doi.org/10.1002/cey2.693
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