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Research 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

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
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Graphical Abstract

A novel, high-activity single-atomic Mn sites coupled with Fe3C nanoparticles encapsulated in N-doped porous carbon matrixes (Mn SAs/Fe3C NPs@NPC) catalyst was synthesized by isolation-polymerization-pyrolysis (IPP) strategy. The coupling of Fe3C NPs and the isolation Mn atoms with Mn-N4 sites modified the electronic structure and atomic coordination environment, accelerating the electrocatalytic oxygen reduction reaction (ORR) greatly.

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

single atom catalystnanoparticleselectrocatalystoxygen reductionzinc-air battery

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Nano Research
Volume 15 Issue 9,
September 2022
Pages 7976-7985
DOI: 10.1007/s12274-022-4502-4
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
Topics:
Electrocatalysis

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Received: 20 April 2022
Revised: 01 May 2022
Accepted: 04 May 2022
Published: 14 July 2022
© Tsinghua University Press 2022
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