A macroporous carbon nanoframe for hosting Mott–Schottky Fe–Co/Mo<sub>2</sub>C sites as an outstanding bi-functional oxygen electrocatalyst

Hong, Jie; Zhang, Lei; Zhu, Qiliang; Du, Ziang; Zhou, Yingtang; Wågberg, Thomas; Hu, Guangzhi

doi:10.1039/d3mh01237a

Cited by 14 publications

(1 citation statement)

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“…20,21 Microscopic pores and defects in SACs provide a confinement effect that stabilizes metal sites and prevents the spatial migration and agglomeration of metal atoms, 22,23 while the mesoscale structure features multiple cavities or regions that efficiently direct reactants to the active sites. 24,25 The three-dimensional (3D) porous carbon support of Fe SACs is expected to play a role similar to the 3D amino acid structure of enzymes for peroxidase-like catalysis. 13 A 3D FeN 4 structure has been demonstrated to emulate natural enzymes' distal heme pocket residues, which is different from the conventional 2D FeN 4 structure.…”

Section: Introductionmentioning

confidence: 99%

Linking atomic to mesoscopic scales in multilevel structural tailoring of single-atom catalysts for peroxide activation

Yu,

Xin,

et al. 2024

Mater. Horiz.

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Section: Introductionmentioning

confidence: 99%

Linking atomic to mesoscopic scales in multilevel structural tailoring of single-atom catalysts for peroxide activation

Yu,

Xin,

et al. 2024

Mater. Horiz.

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Oxophilic Low‐Coordination Gd‐N₃ Single Atom Sites With P‐Enhanced Second Coordination for High‐Performance Al‐Air Batteries

Liu,

Zhang,

et al. 2024

Adv Funct Materials

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The development of efficient rare earth single‐atom (SA) catalysts for the oxygen reduction reaction (ORR) is essential yet challenging for high‐performance aluminum‐air batteries (AABs). This study introduces a concept‐to‐proof strategy for synthesizing a hollow carbon‐supported gadolinium (Gd) SA catalyst using low‐coordination and second‐coordination sphere engineering. In this design, Gd atoms are coordinated to three nitrogen (N) atoms in N‐doped carbon and surrounded by six phosphorus (P) atoms, forming Gd‐N3‐P6 sites. These catalysts demonstrated exceptional ORR performance, achieving a half‐wave potential of 0.895 V and superior durability compared to the commercial Pt/C benchmark. When integrated into AABs, they delivered impressive performance, with a peak power density of 257 mW/cm2 and an energy density of 2916 Wh/kg, alongside enhanced cycling stability. In situ characterization and theoretical calculations revealed that the strategic placement of P atoms in the second coordination sphere significantly enhanced the valence state of the Gd site. This enhancement improved the adsorption capacity for O2 and H2O while facilitating the rapid desorption of *OH intermediates during the ORR. This study offers valuable insights into the development of cost‐effective ORR catalysts, emphasizing the significance of modulating the local coordination environment of metal SA sites.

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Harnessing Multi‐Asymmetric Engineering: A New Horizon in Bifunctional Oxygen Electrocatalysis with Iron‐Group Atom‐Cluster Nanohybrid

Xu,

Zhang,

et al. 2024

Adv Funct Materials

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Integrating active sites for oxygen reduction and evolution reactions (ORR and OER) is pivotal for advancing bifunctional oxygen electrodes. Addressing the geometric/electronic properties of these sites is essential to disrupt the linear scaling relationship between the adsorption and desorption of complex intermediates. Herein, a proof‐of‐concept is presented for constructing asymmetric trinuclear sites employing both composition‐ and size‐based asymmetric coupling strategies. These sites comprise ORR‐active Fe single atom (FeSA), OER‐active atomically clustered Fe species (FeAC), and NiSA sites as modulators. This FeAC‐SA‐NiSA@N‐doped carbon exhibits excellent bifunctional catalytic activities, with a narrow potential gap of 0.661 V between an ORR half‐wave potential of 0.931 V and an OER potential of 1.592 V at 10 mA cm−2. The Zn‐air battery employing this material achieves a peak power density of 293 mW cm−2, a specific capacity of 748 mAh gZn−1, and remarkable stability. Experimental findings and theoretical simulations reveal that NiSA sites induced strong electronic coupling among the trinuclear centers, facilitating charge redistribution and optimizing the adsorption and desorption barriers for intermediates. This enhances the rapid release of *OH during ORR and the efficient transformation from *O to *OOH during OER. This study presents a novel strategy for developing robust bifunctional oxygen electrodes.

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A macroporous carbon nanoframe for hosting Mott–Schottky Fe–Co/Mo₂C sites as an outstanding bi-functional oxygen electrocatalyst

Abstract: Simultaneously optimizing the d-band center of the catalyst and the mass/charge transport processes during the oxygen catalytic reaction is an essential but arduous task in the pursuit of creating effective...

Cited by 14 publications

References 86 publications

Linking atomic to mesoscopic scales in multilevel structural tailoring of single-atom catalysts for peroxide activation

Linking atomic to mesoscopic scales in multilevel structural tailoring of single-atom catalysts for peroxide activation

Oxophilic Low‐Coordination Gd‐N₃ Single Atom Sites With P‐Enhanced Second Coordination for High‐Performance Al‐Air Batteries

Harnessing Multi‐Asymmetric Engineering: A New Horizon in Bifunctional Oxygen Electrocatalysis with Iron‐Group Atom‐Cluster Nanohybrid

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A macroporous carbon nanoframe for hosting Mott–Schottky Fe–Co/Mo2C sites as an outstanding bi-functional oxygen electrocatalyst

Abstract: Simultaneously optimizing the d-band center of the catalyst and the mass/charge transport processes during the oxygen catalytic reaction is an essential but arduous task in the pursuit of creating effective...

Cited by 14 publications

References 86 publications

Linking atomic to mesoscopic scales in multilevel structural tailoring of single-atom catalysts for peroxide activation

Linking atomic to mesoscopic scales in multilevel structural tailoring of single-atom catalysts for peroxide activation

Oxophilic Low‐Coordination Gd‐N3 Single Atom Sites With P‐Enhanced Second Coordination for High‐Performance Al‐Air Batteries

Harnessing Multi‐Asymmetric Engineering: A New Horizon in Bifunctional Oxygen Electrocatalysis with Iron‐Group Atom‐Cluster Nanohybrid

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A macroporous carbon nanoframe for hosting Mott–Schottky Fe–Co/Mo₂C sites as an outstanding bi-functional oxygen electrocatalyst

Oxophilic Low‐Coordination Gd‐N₃ Single Atom Sites With P‐Enhanced Second Coordination for High‐Performance Al‐Air Batteries