Single-atomic Mn sites coupled with Fe3C nanoparticles encapsulated in carbon matrixes derived from bimetallic Mn/Fe polyphthalocyanine conjugated polymer networks for accelerating electrocatalytic oxygen reduction

Pan, Yuan; Li, Min; Mi, Wanliang; Wang, Minmin; Li, Junxi; Zhao, Yilin; Ma, Xiaojing; Wang, Bin; Zhu, Wei; Cui, Zhiming; Yin, Handong; Liu, Yunqi

doi:10.1007/s12274-022-4502-4

Cited by 19 publications

(7 citation statements)

References 58 publications

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“…When the Fe ions coordinate with anions, the metal Fe with empty t 2g orbital can be used to accept the valence electrons of conjugated N atoms, further adjust the 3 d 6 electronic configuration of Fe to improve the catalytic activity. [ 25 ] Hence, the XAFS and XPS (Figures S5 and S6, Supporting Information) demonstrate the successful incorporation of Co into iron nitride and the electron transfer process from Fe to Co, in which the (Co 0.17 Fe 0.83 ) 3 N with 20 at.% Co provides optimal electronic configuration, further balance the electrocatalytic absorption properties.…”

Section: Resultsmentioning

confidence: 97%

Synergistic Effects of Phase Transition and Electron‐Spin Regulation on the Electrocatalysis Performance of Ternary Nitride

Ban

Cao

et al. 2023

Adv Funct Materials

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Transition metal nitrides (TMNs) have great potential use in energy storage and conversion owing to tunable electronic and bonding characteristics. Novel iron rich nitrides nanoparticles anchored on the N‐doped porous carbon, named as (CoxFe1–x)3N@NPC (0 ≤ x < 0.5) are designed here. The synergistic effects of phase transition and electron‐spin regulation on oxygen electrocatalysis are testified. A core–shell structure of (CoxFe1–x)3N with high dispersibility is induced by an intermediate phase transition process, which significantly suppresses coarsening of the metallic nitrides. The Co incorporation regulates d‐band electrons spin polarization. The t2g5eg1 of FeII with the ideal eg electron filling boosts intrinsic activity. (Co0.17Fe0.83)3N@NPC with optimal cobalt content holds electronic configuration with moderate eg electron filling (t2g5eg1), which balances the adsorption of *O2 and the hydrogenation of *OH, improving bifunctional catalytic performances. Both liquid and solid‐state zinc–air batteries assembled based (Co0.17Fe0.83)3N@NPC cathodes substantially deliver higher peak power density and remarkable energy density.

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Section: Resultsmentioning

confidence: 97%

Synergistic Effects of Phase Transition and Electron‐Spin Regulation on the Electrocatalysis Performance of Ternary Nitride

Ban

Cao

et al. 2023

Adv Funct Materials

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“…In addition, the G band shifts to the left as the potential decreases, which is caused by oxygen being adsorbed on the catalyst. [54] Furthermore, the different Figure 5. A) M-T curves and the calculated number of the unpaired electrons of FeCo/DA@NC, Fe/SA@NC, and Co/SA@NC.…”

Section: Resultsmentioning

confidence: 99%

“…In addition, the G band shifts to the left as the potential decreases, which is caused by oxygen being adsorbed on the catalyst. [ 54 ] Furthermore, the different intermediates formed during the ORR process are further identified by in situ FTIR spectroscopy. Figure 4C,D shows that as the potential decreases, new peaks gradually appear at 1170 and 1280 cm −1 , attributed to the O─O stretching mode of O 2 − on catalyst surface and the bending mode of *OOH vibration, respectively.…”

Section: Resultsmentioning

confidence: 99%

Revealing the Orbital Interactions between Dissimilar Metal Sites during Oxygen Reduction Process

Sheng,

Mei,

Jing

et al. 2023

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A FeCo/DA@NC catalyst with the well‐defined FeCoN6 moiety is customized through a novel and ultrafast Joule heating technique. This catalyst demonstrates superior oxygen reduction reaction activity and stability in an alkaline environment. The power density and charge–discharge cycling of znic–air batteries driven by FeCo/DA@NC also surpass those of Pt/C catalyst. The source of the excellent oxygen reduction reaction activity of FeCo/DA@NC originates from the significantly changed charge environment and 3d orbital spin state. These not only improve the bonding strength between active sites and oxygen‐containing intermediates, but also provide spare reaction sites for oxygen‐containing intermediates. Moreover, various in situ detection techniques reveal that the rate‐determining step in the four‐electron oxygen reduction reaction is *O2 protonation. This work provides strong support for the precise design and rapid preparation of bimetallic catalysts and opens up new ideas for understanding orbital interactions during oxygen reduction reactions.

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“…Fe 3 C (cementite, 6.69% C) is an interstitial compound with semi-stable phases and complex structures, acting as an electron-rich donor in the ORR. [113][114][115] However, the primary and secondary relationships between nitrogen-containing species (mainly FeN x and N x C) and Fe 3 C species formed during pyrolysis are still unclear. The ability to dissolve easily under acidic conditions is not conducive to improved stability.…”

Section: Reviewmentioning

confidence: 99%

Unified ORR mechanism criteria via charge–spin–coordination of Fe functional units

Song,

Yang,

Zou

et al. 2024

Energy Environ. Sci.

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Single-atomic Mn sites coupled with Fe3C nanoparticles encapsulated in carbon matrixes derived from bimetallic Mn/Fe polyphthalocyanine conjugated polymer networks for accelerating electrocatalytic oxygen reduction

Cited by 19 publications

References 58 publications

Synergistic Effects of Phase Transition and Electron‐Spin Regulation on the Electrocatalysis Performance of Ternary Nitride

Synergistic Effects of Phase Transition and Electron‐Spin Regulation on the Electrocatalysis Performance of Ternary Nitride

Revealing the Orbital Interactions between Dissimilar Metal Sites during Oxygen Reduction Process

Unified ORR mechanism criteria via charge–spin–coordination of Fe functional units

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