Constructing Palladium‐Based Crystalline@Amorphous Core–Shell Heterojunctions for Efficient Formic Acid Oxidation

Abstract Constructing crystalline@amorphous heterostructures allows nanomaterials to maintain high electrical conductivity of crystalline structures while acquiring abundant active sites from amorphous structure. This emerging strategy has attracted considerable attention in electrochemical and phot...

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Main Authors: Huiling Li, Jingkun Yu, Yongming Sui, Weibin Wang, Jiewen Liu, LiBo Sheng, Ankang Chen, Siyu Lu, Bo Zou
Format: Article
Language:English
Published: Wiley 2025-07-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202504469
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author Huiling Li
Jingkun Yu
Yongming Sui
Weibin Wang
Jiewen Liu
LiBo Sheng
Ankang Chen
Siyu Lu
Bo Zou
author_facet Huiling Li
Jingkun Yu
Yongming Sui
Weibin Wang
Jiewen Liu
LiBo Sheng
Ankang Chen
Siyu Lu
Bo Zou
author_sort Huiling Li
collection DOAJ
description Abstract Constructing crystalline@amorphous heterostructures allows nanomaterials to maintain high electrical conductivity of crystalline structures while acquiring abundant active sites from amorphous structure. This emerging strategy has attracted considerable attention in electrochemical and photoelectrochemistry applications. However, achieving crystalline@amorphous heterostructures based on palladium (Pd) remains challenging due to the difficulties in balancing the transformation between these two phases. Here, a feasible strategy is developed to manufacture Pd‐based crystalline@amorphous core–shell structures through non‐metallic element doping. The obtained core–shell structures exhibit outstanding catalytic performance for formic acid oxidation (FAO) with mass activity of up to 2.503 A mg−1Pd. Detailed theoretical and experimental analyses reveal that the construction of crystalline@amorphous core–shell structures increase surface active sites, lowers the oxidation energy barrier, and enhances the selectivity of the direct pathway, thereby effectively facilitating the FAO process. This work demonstrates the feasibility of constructing efficient FAO catalysts using crystalline@amorphous core–shell structures and provides a new platform for achieving platinum‐group metals (PGMs) based crystalline‐amorphous heterostructures.
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issn 2198-3844
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publishDate 2025-07-01
publisher Wiley
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series Advanced Science
spelling doaj-art-beefbc42e4be4510b902b19a3c6f0a2a2025-08-20T03:12:04ZengWileyAdvanced Science2198-38442025-07-011227n/an/a10.1002/advs.202504469Constructing Palladium‐Based Crystalline@Amorphous Core–Shell Heterojunctions for Efficient Formic Acid OxidationHuiling Li0Jingkun Yu1Yongming Sui2Weibin Wang3Jiewen Liu4LiBo Sheng5Ankang Chen6Siyu Lu7Bo Zou8State Key Laboratory of High Pressure and Superhard Materials College of Physics Jilin University China 2699 Qianjin Street Changchun 130012 ChinaCollege of Chemistry and Pingyuan Laboratory Zhengzhou University Zhengzhou 45000 ChinaState Key Laboratory of High Pressure and Superhard Materials College of Physics Jilin University China 2699 Qianjin Street Changchun 130012 ChinaState Key Laboratory of High Pressure and Superhard Materials College of Physics Jilin University China 2699 Qianjin Street Changchun 130012 ChinaState Key Laboratory of High Pressure and Superhard Materials College of Physics Jilin University China 2699 Qianjin Street Changchun 130012 ChinaState Key Laboratory of High Pressure and Superhard Materials College of Physics Jilin University China 2699 Qianjin Street Changchun 130012 ChinaState Key Laboratory of High Pressure and Superhard Materials College of Physics Jilin University China 2699 Qianjin Street Changchun 130012 ChinaCollege of Chemistry and Pingyuan Laboratory Zhengzhou University Zhengzhou 45000 ChinaState Key Laboratory of High Pressure and Superhard Materials College of Physics Jilin University China 2699 Qianjin Street Changchun 130012 ChinaAbstract Constructing crystalline@amorphous heterostructures allows nanomaterials to maintain high electrical conductivity of crystalline structures while acquiring abundant active sites from amorphous structure. This emerging strategy has attracted considerable attention in electrochemical and photoelectrochemistry applications. However, achieving crystalline@amorphous heterostructures based on palladium (Pd) remains challenging due to the difficulties in balancing the transformation between these two phases. Here, a feasible strategy is developed to manufacture Pd‐based crystalline@amorphous core–shell structures through non‐metallic element doping. The obtained core–shell structures exhibit outstanding catalytic performance for formic acid oxidation (FAO) with mass activity of up to 2.503 A mg−1Pd. Detailed theoretical and experimental analyses reveal that the construction of crystalline@amorphous core–shell structures increase surface active sites, lowers the oxidation energy barrier, and enhances the selectivity of the direct pathway, thereby effectively facilitating the FAO process. This work demonstrates the feasibility of constructing efficient FAO catalysts using crystalline@amorphous core–shell structures and provides a new platform for achieving platinum‐group metals (PGMs) based crystalline‐amorphous heterostructures.https://doi.org/10.1002/advs.202504469core–shell structurecrystalline@amorphousformic acid oxidationheterojunctionspalladium‐based catalyst
spellingShingle Huiling Li
Jingkun Yu
Yongming Sui
Weibin Wang
Jiewen Liu
LiBo Sheng
Ankang Chen
Siyu Lu
Bo Zou
Constructing Palladium‐Based Crystalline@Amorphous Core–Shell Heterojunctions for Efficient Formic Acid Oxidation
Advanced Science
core–shell structure
crystalline@amorphous
formic acid oxidation
heterojunctions
palladium‐based catalyst
title Constructing Palladium‐Based Crystalline@Amorphous Core–Shell Heterojunctions for Efficient Formic Acid Oxidation
title_full Constructing Palladium‐Based Crystalline@Amorphous Core–Shell Heterojunctions for Efficient Formic Acid Oxidation
title_fullStr Constructing Palladium‐Based Crystalline@Amorphous Core–Shell Heterojunctions for Efficient Formic Acid Oxidation
title_full_unstemmed Constructing Palladium‐Based Crystalline@Amorphous Core–Shell Heterojunctions for Efficient Formic Acid Oxidation
title_short Constructing Palladium‐Based Crystalline@Amorphous Core–Shell Heterojunctions for Efficient Formic Acid Oxidation
title_sort constructing palladium based crystalline amorphous core shell heterojunctions for efficient formic acid oxidation
topic core–shell structure
crystalline@amorphous
formic acid oxidation
heterojunctions
palladium‐based catalyst
url https://doi.org/10.1002/advs.202504469
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