Electronic structure regulation of the Fe-based single-atom catalysts for oxygen electrocatalysis

Wang, Xiaochen; Kang, Zhiwen; Wang, Dan; Zhao, Yafei; Xiang, Xu; Shang, Huishan; Zhang, Bing

doi:10.1016/j.nanoen.2024.109268

Cited by 24 publications

(2 citation statements)

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“…To reduce carbon emissions and satisfy the growing need for energy, there is an immediate need for inventive energy transformation methods that can replace traditional fossil fuel burning systems. − Nonetheless, the oxygen evolution reaction (OER) is hindered by slow reaction rates, and the resulting significant overpotentials, which lead to reduced efficiency across diverse energy systems. − Standard OER electrocatalysts, such as IrO 2 and RuO 2 , contain expensive noble metals, posing a barrier to their real-world application. − A promising approach to reconcile performance with affordability involves integrating these noble metals with more economical non-noble metals. Researchers have lately been successful in merging iridium and ruthenium elements with base metal oxides and hydroxides through methods like doping or surface attachment, achieving significant catalytic activity while minimizing the use of precious metals. − For instance, the construction of Ir/Co 3 O 4 exhibited potent interfacial charge accumulation due to the pseudocapacitive feature of the Co 3 O 4 , while Ir sites are crucial for enhanced reaction kinetics .…”

Section: Introductionmentioning

confidence: 99%

Synergistic Assistance of Ir Clusters and NiCo₂O₄ Nanosheets Interfaces in Direct O–O Coupling for High-Efficiency Alkaline Oxygen Evolution

Yang,

Zhou,

Zhao

et al. 2024

ACS Appl. Mater. Interfaces

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Section: Introductionmentioning

confidence: 99%

Synergistic Assistance of Ir Clusters and NiCo₂O₄ Nanosheets Interfaces in Direct O–O Coupling for High-Efficiency Alkaline Oxygen Evolution

Yang,

Zhou,

Zhao

et al. 2024

ACS Appl. Mater. Interfaces

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“…Up to now, Pt-based catalysts have been extensively utilized for electrocatalytic energy storage systems, including metal-air batteries and proton exchange membrane fuel cells. − Considering their prohibitive cost and insufficient stability, , substantial efforts have been devoted to develop cost-effective and high-activity catalysts for the oxygen reduction reaction (ORR). − Among which, metal single-atom catalysts (SACs) anchored on N-doped carbon substrate (metal–N–C), especially Fe–N–C are promising alternatives due to their maximum atom utilization and modifiable electronic structure. − …”

Section: Introductionmentioning

confidence: 99%

p-d Orbital Hybridization Induced by Asymmetrical FeSn Dual Atom Sites Promotes the Oxygen Reduction Reaction

Wang,

Zhang,

Guo

et al. 2024

J. Am. Chem. Soc.

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With more flexible active sites and intermetal interaction, dualatom catalysts (DACs) have emerged as a new frontier in various electrocatalytic reactions. Constructing a typical p-d orbital hybridization between p-block and dblock metal atoms may bring new avenues for manipulating the electronic properties and thus boosting the electrocatalytic activities. Herein, we report a distinctive heteronuclear dual-metal atom catalyst with asymmetrical FeSn dual atom sites embedded on a two-dimensional C 2 N nanosheet (FeSn−C 2 N), which displays excellent oxygen reduction reaction (ORR) performance with a half-wave potential of 0.914 V in an alkaline electrolyte. Theoretical calculations further unveil the powerful p-d orbital hybridization between p-block stannum and dblock ferrum in FeSn dual atom sites, which triggers electron delocalization and lowers the energy barrier of *OH protonation, consequently enhancing the ORR activity. In addition, the FeSn−C 2 N-based Zn−air battery provides a high maximum power density (265.5 mW cm −2 ) and a high specific capacity (754.6 mA h g −1 ). Consequently, this work validates the immense potential of p-d orbital hybridization along dual-metal atom catalysts and provides new perception into the logical design of heteronuclear DACs.

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Regulation of d‐Orbital Electron in Fe‐N₄ by High‐Entropy Atomic Clusters for Highly Active and Durable Oxygen Reduction Reaction

Yang,

Cai,

Zhang

et al. 2024

Adv Funct Materials

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Simultaneously improving activity and stability is a crucial yet challenge in the development of metallic single‐atom‐based catalysts. In current work, a novel approach is introduced to address this issue by combining post‐adsorption and secondary pyrolysis techniques to create a synergistic catalytic system, in which the single atoms (SAs) Fe sites played in the NC matrix (Fe─NC) are coupled with high‐entropy atomic clusters (HEACs). Theoretical calculations reveal that the incorporation of HEACs lead to a rehybridization of the 3d orbital configuration of Fe‐N4, which helps to balance the adsorption/desorption energy of oxygenated intermediates. In situ spectroscopy further reveals that the rate‐limiting step of OH* desorption on HEAC/Fe─NC in oxygen reduction reaction (ORR) is more facile compared to atomic Fe─NC, implying a higher ORR activity. Moreover, the synergistic effect of diffusion activation barriers and configuration entropy contributes to the structural stability of HEAC/Fe─NC, resulting in remarkable durability. Consequently, this unique catalyst exhibits half‐wave potentials of 0.927 and 0.828 V in an aqueous solution of KOH (0.1 m) and HClO4 (0.1 m), respectively, along with excellent durability. The findings propose a novel strategy for modulating the electronic structure of metallic SAs catalysts and enhancing their stability through strong interactions between SAs and HEACs.

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Electronic structure regulation of the Fe-based single-atom catalysts for oxygen electrocatalysis

Cited by 24 publications

References 218 publications

Synergistic Assistance of Ir Clusters and NiCo₂O₄ Nanosheets Interfaces in Direct O–O Coupling for High-Efficiency Alkaline Oxygen Evolution

Synergistic Assistance of Ir Clusters and NiCo₂O₄ Nanosheets Interfaces in Direct O–O Coupling for High-Efficiency Alkaline Oxygen Evolution

p-d Orbital Hybridization Induced by Asymmetrical FeSn Dual Atom Sites Promotes the Oxygen Reduction Reaction

Regulation of d‐Orbital Electron in Fe‐N₄ by High‐Entropy Atomic Clusters for Highly Active and Durable Oxygen Reduction Reaction

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Electronic structure regulation of the Fe-based single-atom catalysts for oxygen electrocatalysis

Cited by 24 publications

References 218 publications

Synergistic Assistance of Ir Clusters and NiCo2O4 Nanosheets Interfaces in Direct O–O Coupling for High-Efficiency Alkaline Oxygen Evolution

Synergistic Assistance of Ir Clusters and NiCo2O4 Nanosheets Interfaces in Direct O–O Coupling for High-Efficiency Alkaline Oxygen Evolution

p-d Orbital Hybridization Induced by Asymmetrical FeSn Dual Atom Sites Promotes the Oxygen Reduction Reaction

Regulation of d‐Orbital Electron in Fe‐N4 by High‐Entropy Atomic Clusters for Highly Active and Durable Oxygen Reduction Reaction

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Synergistic Assistance of Ir Clusters and NiCo₂O₄ Nanosheets Interfaces in Direct O–O Coupling for High-Efficiency Alkaline Oxygen Evolution

Synergistic Assistance of Ir Clusters and NiCo₂O₄ Nanosheets Interfaces in Direct O–O Coupling for High-Efficiency Alkaline Oxygen Evolution

Regulation of d‐Orbital Electron in Fe‐N₄ by High‐Entropy Atomic Clusters for Highly Active and Durable Oxygen Reduction Reaction