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Nano Research 2022, 15(9): 7976-7985 https://doi.org/10.1007/s12274-022-4502-4
Research Article | Issue | Published: 14 July 2022

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

Show Author's Information Yuan Pan1,2( ),  Min Li1,  Wanliang Mi3,  Minmin Wang1,  Junxi Li1,  Yilin Zhao1,  Xuelu Ma4( ),  Bin Wang5,  Wei Zhu6,  Zhiming Cui7,  Hailiang Yin8,  Yunqi Liu1
State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao 266580, China
Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, China
Research Institute of Petroleum Processing, Sinopec, Beijing 100083, China
School of Chemical & Environmental Engineering, China University of Mining & Technology, Beijing 100083, China
School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi’an 710119, China
State Key Lab of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
Key Laboratory of Fuel Cell Technology of Guangdong Province, South China University of Technology, Guangzhou 510641, China
Academy of Science & Technology, China University of Petroleum (East China), Dongying 257061, China
Keywords:
nanoparticles, oxygen reduction, electrocatalyst, single atom catalyst, zinc-air battery
Topics:
Electrocatalysis
Cite this article:
Pan Y, Li M, Mi W, et al. 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. Nano Research, 2022, 15(9): 7976-7985. https://doi.org/10.1007/s12274-022-4502-4
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Abstract Full text Electronic supplementary material About this article

The construction of robust coupling catalysts for accelerating electrocatalytic oxygen reduction reaction (ORR) through the modulation of the electronic structure and local atomic configuration is critical but remains challenging. Herein, we report a facile and effective isolation-polymerization-pyrolysis (IPP) strategy for high-precision synthesis of single-atomic Mn sites coupled with Fe3C nanoparticles encapsulated in N-doped porous carbon matrixes (Mn SAs/Fe3C NPs@NPC) catalyst derived from predesigned bimetallic Fe/Mn polyphthalocyanine (FeMn-BPPc) conjugated polymer networks by solid-phase reaction approach. Benefiting from the synergistic effects between the single-atomic Mn-N4 sites and Fe3C NPs as well as the confinement effect of NPC, the Mn SAs/Fe3C NPs@NPC catalyst exhibited excellent electrocatalytic activity and stability for ORR. The assembled Zn-air battery displayed larger power density of 186 mW·cm−2 than that of Pt/C + Ir/C-based battery. It also exhibits excellent stability without obvious voltage change after 106 cycles with 36 h. Combingin-situ Raman spectra with in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) characterization results indicated that the Mn-N4 site as an active site for the O2 adsorption–activation process, which effectively facilitates the generation of key *OOH intermediates and *OH desorption to promote the multielectron reaction kinetics. Theoretical calculation reveals that the excellent electrocatalytic performance originates from the charge redistribution and the d orbital shift resulting from Mn–Fe bond, which buffers the activity of ORR through the electron reservoir capable of electron donation or releasing. This work paves a novel IPP strategy for constructing high-performance coupling electrocatalyst towards the ORR for energy conversion devices.


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Abstract
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Electronic supplementary material
About this article

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

Show Author's information Yuan Pan1,2( ), Min Li1, Wanliang Mi3, Minmin Wang1, Junxi Li1, Yilin Zhao1, Xuelu Ma4( ), Bin Wang5, Wei Zhu6, Zhiming Cui7, Hailiang Yin8, Yunqi Liu1
State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao 266580, China
Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, China
Research Institute of Petroleum Processing, Sinopec, Beijing 100083, China
School of Chemical & Environmental Engineering, China University of Mining & Technology, Beijing 100083, China
School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi’an 710119, China
State Key Lab of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
Key Laboratory of Fuel Cell Technology of Guangdong Province, South China University of Technology, Guangzhou 510641, China
Academy of Science & Technology, China University of Petroleum (East China), Dongying 257061, China

Abstract

The construction of robust coupling catalysts for accelerating electrocatalytic oxygen reduction reaction (ORR) through the modulation of the electronic structure and local atomic configuration is critical but remains challenging. Herein, we report a facile and effective isolation-polymerization-pyrolysis (IPP) strategy for high-precision synthesis of single-atomic Mn sites coupled with Fe3C nanoparticles encapsulated in N-doped porous carbon matrixes (Mn SAs/Fe3C NPs@NPC) catalyst derived from predesigned bimetallic Fe/Mn polyphthalocyanine (FeMn-BPPc) conjugated polymer networks by solid-phase reaction approach. Benefiting from the synergistic effects between the single-atomic Mn-N4 sites and Fe3C NPs as well as the confinement effect of NPC, the Mn SAs/Fe3C NPs@NPC catalyst exhibited excellent electrocatalytic activity and stability for ORR. The assembled Zn-air battery displayed larger power density of 186 mW·cm−2 than that of Pt/C + Ir/C-based battery. It also exhibits excellent stability without obvious voltage change after 106 cycles with 36 h. Combingin-situ Raman spectra with in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) characterization results indicated that the Mn-N4 site as an active site for the O2 adsorption–activation process, which effectively facilitates the generation of key *OOH intermediates and *OH desorption to promote the multielectron reaction kinetics. Theoretical calculation reveals that the excellent electrocatalytic performance originates from the charge redistribution and the d orbital shift resulting from Mn–Fe bond, which buffers the activity of ORR through the electron reservoir capable of electron donation or releasing. This work paves a novel IPP strategy for constructing high-performance coupling electrocatalyst towards the ORR for energy conversion devices.

Keywords: nanoparticles, oxygen reduction, electrocatalyst, single atom catalyst, zinc-air battery

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Publication history
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Acknowledgements

Publication history

Received: 20 April 2022
Revised: 01 May 2022
Accepted: 04 May 2022
Published: 14 July 2022
Issue date: September 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by State Key Laboratory of Catalytic Materials and Reaction Engineering (RIPP, SINOPEC), Taishan Scholars Program of Shandong Province (No. tsqn201909065), Shandong Provincial Natural Science Foundation (Nos. ZR2021YQ15, ZR2020QB174, and ZR2019MB022), the National Natural Science Foundation of China (Nos. 22108306 and 21902182), the Fundamental Research Funds for the Central Universities (Nos. 2022YQHH01 and 22CX07009A), the State Key Laboratory of Organic-Inorganic Composites (No. oic-202101006), Post-graduate Innovation Fund of China University of Petroleum (East China) (No. YCX2021064), the Research Fund Program of Key Laboratory of Fuel Cell Technology of Guangdong Province, the Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), and the Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University), Ministry of Education.

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