Mechanistic insight into the Fe-atom-pairs for breaking the scaling relation in ORR

Liu, Rongrong; Tang, Ranxiao; Feng, Jizheng; Meng, Tao

doi:10.1016/j.cej.2023.144261

Cited by 18 publications

(12 citation statements)

References 47 publications

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“…Theoretical calculations and experimental studies have demonstrated that different coordination configurations of Fe-N x sites can influence the 3d electron distribution of iron centers, thus regulating the adsorption and desorption energy barriers of the ORR intermediate on Fe-N x sites to adjust the catalytic performance of Fe-N/C materials. , Different coordination configurations could be obtained by modulating the coordination numbers of Fe-N x sites (e.g., Fe-N 2 , Fe-N 3 , and Fe-N 5 , ), grafting axial ligands to Fe-N 4 sites (e.g., PFePc-I, Fe-N 4 -Cl, , and Fe-N 4 -OH), introducing dual-metal sites (e.g., Fe 2 -N 6 , Fe-Cu-N 6 , and Fe-N 4 -Bi-O), and coupling carbon defect to Fe-N x sites (e.g., edge Fe-N 4 and pentagon-bonded-Fe-N 4 ). Among them, edge Fe-N 4 sites have aroused wide concern among people for their structural stability as well as excellent catalytic activity. − To form edge Fe-N 4 sites in Fe, N codoped carbon, the formation of edge carbon and construction of Fe-N 4 sites are essential steps.…”

Section: Introductionmentioning

confidence: 99%

Atomic Edge Fe-N₄ Active Sites on N-Doped Porous Carbon Nanosheets Derived from Zeolitic-Imidazolate Frameworks for High-Efficiency Oxygen Reduction

Jiang,

Ye,

Zhu

et al. 2023

ACS Sustainable Chem. Eng.

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Defect and morphology engineering of metalnitrogen codoped carbon (M-N/C) has been proven to be efficacious in promoting the oxygen reduction reaction (ORR) catalytic activity, yet the simultaneous construction of active sites with high intrinsic activity and efficient exposure is a challenge. Herein, an Fe-N/C catalyst consisting of edge Fe-N 4 sites atomically dispersed on porous carbon nanosheets (e-Fe-N/C NS ) is designed for high intrinsic catalytic active as well as efficient utilization. By combining an edge-doping process and an I 2 -etching effect, the edge Fe-N 4 sites are constructed preferentially and the interior active sites are fully exposed. The edge Fe-N 4 sites endow e-Fe-N/C NS with high intrinsic activity, which originated from the local electronic redistribution of the Fe-N 4 configuration induced by the edge carbon, while the enriched porous nanosheet structure enhances the edge Fe-N 4 sites utilization efficiency for high mass activity. The as-synthesized e-Fe-N/C NS exhibits a remarkable halfwave potential (E 1/2 , 0.90 V RHE ) under alkaline conditions. This work provides a novel synthetic method for designing highly active defective sites in catalysts for energy conversion systems.

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Section: Introductionmentioning

confidence: 99%

Atomic Edge Fe-N₄ Active Sites on N-Doped Porous Carbon Nanosheets Derived from Zeolitic-Imidazolate Frameworks for High-Efficiency Oxygen Reduction

Jiang,

Ye,

Zhu

et al. 2023

ACS Sustainable Chem. Eng.

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“…S4e† and 2f), the signal is decomposed into four peaks at ∼710.6 eV, ∼713 eV, ∼716 eV, and ∼718.8 eV, which are typical for Fe 3+ and Fe 2+ , respectively. 36,37…”

Section: Resultsmentioning

confidence: 99%

Interfacial microenvironment modulation enhancing catalytic kinetics of CoNiP@NiFe LDH heterostructures for highly efficient oxygen evolution reaction

Zhang,

Guo

2023

RSC Adv.

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“…The double sulfur-vacancy can endow CoS 1.097 @MoS 2 heterojunctions with promoted electron/mass transfer to accelerate the HER kinetics. 26,27 For investigating the elemental valence state and chemical composition on the surface, XPS was used for CoS 1.097 , MoS 2 , and CoS 1.097 @MoS 2 . By analyzing the XPS survey spectrum, we found that the elemental compositions of Co, Mo, and S elements, in CoS 1.097 @MoS 2 heterojunctions, correspond to atomic percentages of 36.35, 10.85, and 56.80%, respectively.…”

Section: Resultsmentioning

confidence: 99%

Engineering Double Sulfur-Vacancy in CoS_1.097@MoS₂ Core–Shell Heterojunctions for Hydrogen Evolution in a Wide pH Range

Yang,

Wen,

Liu

et al. 2023

Inorg. Chem.

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Heterostructured nanomaterials have arisen as electrocatalysts with great potential for hydrogen evolution reaction (HER), considering their superiority in integrating different active components but are plagued by their insufficient active site density in a wide pH range. In this report, double sulfur-vacancy-decorated CoS 1.097 @MoS 2 core−shell heterojunctions are designed, which contain a primary structure of hollow CoS 1.097 nanocubes and a secondary structure of ultrathin MoS 2 nanosheets. Taking advantage of the core−shell type heterointerfaces and double sulfur-vacancy, the CoS 1.097 @MoS 2 catalyst exhibits pH-universal HER performance, achieving the overpotentials at 10 mA cm −2 of 190, 139, and 220 mV in 0.5 M H 2 SO 4 , 1.0 M KOH, and 1.0 M PBS, respectively. Systematic theoretical results show that the double sulfur-vacancy can endow the CoS 1.097 @MoS 2 core−shell heterojunctions with promoted electron/mass transfer and enhanced reactive kinetics, thus boosting HER performance. This work clearly demonstrates an indispensable role of double sulfur-vacancy in enhancing the electrocatalytic HER performance of core−shell type heterojunctions under a wide pH operating condition.

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Mechanistic insight into the Fe-atom-pairs for breaking the scaling relation in ORR

Cited by 18 publications

References 47 publications

Atomic Edge Fe-N₄ Active Sites on N-Doped Porous Carbon Nanosheets Derived from Zeolitic-Imidazolate Frameworks for High-Efficiency Oxygen Reduction

Atomic Edge Fe-N₄ Active Sites on N-Doped Porous Carbon Nanosheets Derived from Zeolitic-Imidazolate Frameworks for High-Efficiency Oxygen Reduction

Interfacial microenvironment modulation enhancing catalytic kinetics of CoNiP@NiFe LDH heterostructures for highly efficient oxygen evolution reaction

Engineering Double Sulfur-Vacancy in CoS_1.097@MoS₂ Core–Shell Heterojunctions for Hydrogen Evolution in a Wide pH Range

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Mechanistic insight into the Fe-atom-pairs for breaking the scaling relation in ORR

Cited by 18 publications

References 47 publications

Atomic Edge Fe-N4 Active Sites on N-Doped Porous Carbon Nanosheets Derived from Zeolitic-Imidazolate Frameworks for High-Efficiency Oxygen Reduction

Atomic Edge Fe-N4 Active Sites on N-Doped Porous Carbon Nanosheets Derived from Zeolitic-Imidazolate Frameworks for High-Efficiency Oxygen Reduction

Interfacial microenvironment modulation enhancing catalytic kinetics of CoNiP@NiFe LDH heterostructures for highly efficient oxygen evolution reaction

Engineering Double Sulfur-Vacancy in CoS1.097@MoS2 Core–Shell Heterojunctions for Hydrogen Evolution in a Wide pH Range

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Atomic Edge Fe-N₄ Active Sites on N-Doped Porous Carbon Nanosheets Derived from Zeolitic-Imidazolate Frameworks for High-Efficiency Oxygen Reduction

Atomic Edge Fe-N₄ Active Sites on N-Doped Porous Carbon Nanosheets Derived from Zeolitic-Imidazolate Frameworks for High-Efficiency Oxygen Reduction

Engineering Double Sulfur-Vacancy in CoS_1.097@MoS₂ Core–Shell Heterojunctions for Hydrogen Evolution in a Wide pH Range