Active sites identification and engineering of M-N-C electrocatalysts toward oxygen reduction reaction

Li, Xiaosong; Wang, Dan; Zha, Sujuan; Cheng, Yuan; Peng, Lin; Wu, Min; Liu, Changhai; Wang, Wenchang; Mitsuzaki, Naotoshi; Chen, Zhidong

doi:10.1016/j.ijhydene.2023.07.161

Cited by 18 publications

(1 citation statement)

References 101 publications

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“…With the consumption of fossil fuels and global warming, developing renewable energy sources is more and more urgent. 1–3 Among them, wind and solar energy are the most promising renewable energy sources. However, wind and solar energy are intermittent.…”

Section: Introductionmentioning

confidence: 99%

Morphological control and performance engineering of Co-based materials for supercapacitors

Pan,

Wang,

Wang

et al. 2024

Phys. Chem. Chem. Phys.

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Section: Introductionmentioning

confidence: 99%

Morphological control and performance engineering of Co-based materials for supercapacitors

Pan,

Wang,

Wang

et al. 2024

Phys. Chem. Chem. Phys.

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Investigation of Single Atom Catalysts by X‐Ray Absorption Spectroscopy

Lützenkirchen‐Hecht,

Yuan,

Eckelt

et al. 2024

Physica Status Solidi (a)

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Recently, Pt‐free and highly efficient, nanostructured M–N–C catalysts employing earth‐abundant metals (M = Fe, Co, Ni, Mn, Cu, etc.) have been recognized as a very promising alternative to noble metal (in particular platinum)‐ based oxygen reduction reaction materials. Structural engineering of the M–N–C catalysts is expected to further boost their catalytic performance, and thus, intense efforts are currently ongoing. Herein, a report is prepared on X‐ray absorption fine structure (EXAFS) studies of different carbon‐based catalyst materials. EXAFS with its intrinsic sensitivity toward the local atomic arrangement around the X‐ray absorbing element allows to characterize isolated, active single‐atom transition metal centers and their atomic environments. In the case of Co and Fe, the analysis suggests in particular asymmetric, penta‐coordinated Co‐N5 and dual‐coordinated Fe–N–P sites. In both cases, a symmetric environment of the metals with only four nitrogen atoms appears to be unfavorable for the catalytic activity. In addition, for Fe–N4 centers embedded in a graphene host matrix, the EXAFS analysis allows to precisely determine the atomic arrangement around the iron atom, and thereby the geometry of the catalytic site. A discussion will be done on how EXAFS investigations can support the further development of single‐atom catalysts.

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Modulating the Iron Microenvironment for a Cooperative Interplay Between Fe‐N‐C Single Atoms and Fe₃C Nanoclusters on the Oxygen Reduction Reaction

Dessalle,

Quílez‐Bermejo,

Hounfodji

et al. 2024

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The coexistence of single atoms and nanoparticles is shown to increase the oxygen reduction performance in Fe‐N‐C electrocatalysts, but the mechanisms underlying this synergistic effect remain elusive. In this study, model Fe‐N‐C electrocatalysts with controlled ratios of FeN4 sites and Fe3C nanoclusters is systematically designed and synthesized. Experiments and density functional theory (DFT) computations reveal that Fe3C nanoclusters near FeN4 sites modulate the electron density of the Fe single‐atom microenvironment through an electron withdrawing effect. This substantially alters the oxygen reduction reaction (ORR) mechanisms and boosts the catalytic performance of FeN4 sites. This study provides fundamental insights into the dynamic catalytic impact of single atoms and nanoparticle coexistence in advanced Fe‐N‐C electrocatalysts for the ORR, paving the way for further refinement through various combinations.

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Active sites identification and engineering of M-N-C electrocatalysts toward oxygen reduction reaction

Cited by 18 publications

References 101 publications

Morphological control and performance engineering of Co-based materials for supercapacitors

Morphological control and performance engineering of Co-based materials for supercapacitors

Investigation of Single Atom Catalysts by X‐Ray Absorption Spectroscopy

Modulating the Iron Microenvironment for a Cooperative Interplay Between Fe‐N‐C Single Atoms and Fe₃C Nanoclusters on the Oxygen Reduction Reaction

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Active sites identification and engineering of M-N-C electrocatalysts toward oxygen reduction reaction

Cited by 18 publications

References 101 publications

Morphological control and performance engineering of Co-based materials for supercapacitors

Morphological control and performance engineering of Co-based materials for supercapacitors

Investigation of Single Atom Catalysts by X‐Ray Absorption Spectroscopy

Modulating the Iron Microenvironment for a Cooperative Interplay Between Fe‐N‐C Single Atoms and Fe3C Nanoclusters on the Oxygen Reduction Reaction

Contact Info

Product

Resources

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Modulating the Iron Microenvironment for a Cooperative Interplay Between Fe‐N‐C Single Atoms and Fe₃C Nanoclusters on the Oxygen Reduction Reaction