Strengthening oxygen reduction activity based on the cooperation of pyridinic-N and graphitic-N for atomically dispersed Fe sites

Xing, Gengyu; Zhang, Guangying; Wang, Baoluo; Tong, Miaomiao; Tian, Chungui; Wang, Lei; Fu, Honggang

doi:10.1039/d3ta00899a

J. Mater. Chem. A

2023

DOI: 10.1039/d3ta00899a

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Strengthening oxygen reduction activity based on the cooperation of pyridinic-N and graphitic-N for atomically dispersed Fe sites

Gengyu Xing

Guangying Zhang

Baoluo Wang

et al.

Abstract: The effects of different N-types coordinated with single atomic sites (SAS) on oxygen reduction reaction (ORR) has not been deeply explored. Herein, we first predicted by density functional theory (DFT)...

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2024

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Cited by 17 publications

References 56 publications

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Synergistically Tuning Graphene Layer and Active Sites for Flexible Zn–Air Batteries

Yu,

Guo,

et al. 2024

Adv Funct Materials

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Fewer layer graphene principally has a higher surface area to support more catalytic sites for energy conversion, but it is still challenging to synthesize monolayer graphene without oxidation from graphite at a low cost. Here, a method for synergistically thinning graphene layers and constructing catalytic sites to create a superior bifunctional oxygen catalyst through vapor intercalation of multi‐layer graphene or its derivatives is described. The synthesized small sheet sizes of 1–2 layer graphene‐supported FeN4 and FeCo active sites exhibit superior reversible activity of oxygen reduction and evolution reactions with a low overall overpotential of 0.648 V. The sheet‐shaped catalyst is further used to fabricate flexible soft‐packed and wearable cable‐type quasi‐solid‐state zinc–air batteries, achieving high performances (>188 mW cm−2, >450 cycles) and enabling smartphone charging. DFT calculations reveal that fewer layer graphene coupled with atomic FeN4 and alloy FeCo sites enables lower Gibbs free energy for favorable OOH* intermediate adsorption/desorption benefiting superior oxygen redox process. This study introduces a strategy for scalable synthesis of 1–2 layer graphene from cheap microcrystalline graphite minerals for wearable and durable energy devices.

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Synergistically Tuning Graphene Layer and Active Sites for Flexible Zn–Air Batteries

Yu,

Guo,

et al. 2024

Adv Funct Materials

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Inhibiting Demetalation of Fe─N─C via Mn Sites for Efficient Oxygen Reduction Reaction in Zinc‐Air Batteries

Hu,

Xing,

Han

et al. 2024

Advanced Materials

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Demetalation caused by the electrochemical dissolution of metallic Fe atoms is a major challenge for the practical application of Fe−N−C catalysts. Herein, we construct an efficient single metallic Mn active site to improve the strength of the Fe−N bond, inhibiting the demetalation effect of Fe−N−C. Mn acts as an electron donor inducing more delocalized electrons to reduce the oxidation state of Fe by increasing the electron density, thereby enhancing the Fe−N bond and inhibiting the electrochemical dissolution of Fe. The ORR pathway for the dissociation of Fe‐Mn dual sites can overcome the high energy barriers to direct O−O bond dissociation and modulate the electronic states of Fe−N4 sites. The resulting FeMn−N−C exhibits excellent ORR activity with a high half‐wave potential (E1/2) of 0.92 V in alkaline electrolytes. FeMn−N−C as a cathode catalyst for Zn‐air batteries (ZABs) has a cycle stability of 700 h at 25 °C and a long cycle stability of more than 210 h under extremely cold conditions at ‐40 °C. These findings contribute to the development of efficient and stable metal‐nitrogen‐carbon catalysts for various energy devices.This article is protected by copyright. All rights reserved

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Innovative Air Cathode with Ni‐Doped Cobalt Sulfide in Highly Ordered Macroporous Carbon Matrix for Rechargeable Zn–Air Battery

Son,

Min,

Cheong

et al. 2024

Advanced Science

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To realize the practical application of rechargeable Zn–Air batteries (ZABs), it is imperative to develop a non‐noble metal‐based electrocatalyst with high electrochemical performance for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Herein, Ni‐doped Co9S8 nanoparticles dispersed on an inverse opal‐structured N, S co‐doped carbon matrix (IO─NixCo9‐xS8@NSC) as a bifunctional electrocatalyst is presented. The unique 3D porous structure, arranged in an inverse opal pattern, provides a large active surface area. Also, the conductive carbon substrate ensures the homogeneous dispersion of NixCo9‐xS8 nanocrystals, preventing aggregation and increasing the exposure of active sites. The introduction of heteroatom dopants into the Co9S8 structure generates defect sites and enhances surface polarity, thereby improving electrocatalytic performance in alkaline solutions. Consequently, the IO─NixCo9‐xS8@NSC shows excellent bifunctional activity with a high half‐wave potential of 0.926 V for ORR and a low overpotential of 289 mV at 10 mA cm−2 for OER. Moreover, the rechargeable ZAB assembled with prepared electrocatalyst exhibits a higher specific capacity (768 mAh gZn−1), peak power density (180.2 mW cm−2), and outstanding stability (over 160 h) compared to precious metal‐based electrocatalyst.

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Strengthening oxygen reduction activity based on the cooperation of pyridinic-N and graphitic-N for atomically dispersed Fe sites

Abstract: The effects of different N-types coordinated with single atomic sites (SAS) on oxygen reduction reaction (ORR) has not been deeply explored. Herein, we first predicted by density functional theory (DFT)...

Cited by 17 publications

References 56 publications

Synergistically Tuning Graphene Layer and Active Sites for Flexible Zn–Air Batteries

Synergistically Tuning Graphene Layer and Active Sites for Flexible Zn–Air Batteries

Inhibiting Demetalation of Fe─N─C via Mn Sites for Efficient Oxygen Reduction Reaction in Zinc‐Air Batteries

Innovative Air Cathode with Ni‐Doped Cobalt Sulfide in Highly Ordered Macroporous Carbon Matrix for Rechargeable Zn–Air Battery

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