Amino-metalloporphyrin polymers derived Fe single atom catalysts for highly efficient oxygen reduction reaction

Qian He; Yuying Meng; Hao Zhang; Ying Zhang; Qingdi Sun; Tao Gan; Huajian Xiao; Xiaohui He; Hongbing Ji

doi:10.1007/s11426-019-9703-7

SCIENCE CHINA Chemistry

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SCIENCE CHINA Chemistry, Volume 63 , Issue 6 : 810-817(2020) https://doi.org/10.1007/s11426-019-9703-7

Amino-metalloporphyrin polymers derived Fe single atom catalysts for highly efficient oxygen reduction reaction

Qian He ¹, Yuying Meng ², Hao Zhang ³, Ying Zhang ³, Qingdi Sun ¹, Tao Gan ¹, Huajian Xiao ³, Xiaohui He ^1,*, Hongbing Ji ^1,4,*

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Affiliations：

1. Fine Chemical Industry Research Institute, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China

2. Institute of Advanced Wear & Corrosion Resistant and Functional Materials, Jinan University, Guangzhou 510632, China

3. Fine Chemical Industry Research Institute, School of Chemical Engineering and Technology, Sun Yat-sen University, Zhuhai 519082, China

4. School of Chemical Engineering, Guangdong University of Petrochemical Technology, Maoming 525000, China

* Corresponding authors (email: hexiaohui@mail.sysu.edu.cn; jihb@mail.sysu.edu.cn)

ReceivedNov 6, 2019
AcceptedFeb 18, 2020
PublishedMar 27, 2020

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Abstract

Funded by

the National Natural Science Foundation of China(21938001,21606260,21576302,21376278,21425627,21701199)

the National Natural Science Foundation of China-SINOPEC Joint Fund(U1663220)

the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01C102)

the Natural Science Foundation of Guang-dong Province(2015A030313104)

the Fundamental Research Funds for the Central Universities of Sun Yat-sen University(15lgjc33,19lgpy129)

porphyrin

precursor-dilution

active site

single atom catalysts

oxygen reduction reaction

Acknowledgment

This work was supported by the National Natural Science Foundation of China (21938001, 21606260, 21576302, 21376278, 21425627, 21701199), the National Natural Science Foundation of China-SINOPEC Joint Fund (U1663220), the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (2017BT01C102), the Natural Science Foundation of Guang-dong Province (2015A030313104), the Fundamental Research Funds for the Central Universities of Sun Yat-sen University (15lgjc33, 19lgpy129).

Interest statement

The authors declare that they have no conflict of interest.

Contributions statement

These authors contributed equally to this work.

Supplement

Supporting Information

The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Figure 1
The morphology of Fe-N-C-900: (a) TEM image, (b) STEM image, (c) AC HAADF-STEM image (Fe single atoms were highlighted by yellow circles), and (d) corresponding element mappings (color online).
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Scheme 1
Schematic illustration of the preparation of Fe-N-C-type catalysts. The molar ratio of FeTAPP:TAPP is 1:20 (color online).
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Figure 2
High-resolution XPS spectra of (a) N 1s and (b) Fe 2p of Fe-N-C-900. (c) Normalized XANES and (d) magnitudes of Fourier-transforms of k³-weighted EXAFS data of Fe-N-C-900 with reference compounds (Fe foil, Fe₂O₃ and FeTPPCl). (e) Fe K-edge wavelet transformed (WT) EXAFS for Fe foil and Fe-N-C-900. (f) The corresponding EXAFS R space fitting curves for Fe-N-C-900 (the red sphere symbolizes an iron atom whereas cyan spheres are oxygen atoms, blue spheres are nitrogen atoms and gray spheres are carbon atoms) (color online).
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Figure 3
Physical characterizations of Fe-N-C-T materials (T=700, 800, 900 or 1000, 1100 °C). (a) XRD patterns; (b) Raman spectra; (c) N₂ adsorption/desorption isotherms and (d) BJH pore size distributions (color online).
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Figure 4
Electrochemical performance of catalysts toward ORR. (a) CV curves of Fe-N-C-900 in O₂- or N₂-saturated 0.1 M KOH solution. (b) Polarization curves of Fe-N-C-900 on RDE rotating at different rotation speeds (the insert n value based on the K-L equation). (c) The n and H₂O₂ yield of Fe-N-C-900, obtained from RRDE technique at 1600 r min⁻¹. (d) Polarization curves of ORR over 20 wt% Pt/C, N-C-900, and Fe-N-C-900 catalysts at 1600 r min⁻¹. (e) Tafel plots of Fe-N-C-900 and 20 wt% Pt/C at 1600 r min⁻¹. (f) Current densities at three different potentials of Fe-N-C-T catalysts at 1600 r min⁻¹ (T=700–1100 °C) (color online).
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Figure 5
(a) ORR polarization curves for the Fe-N-C-900 electrocatalyst and the catalyst with 10 mM KSCN or 3.0 M methanol in O₂-saturated 0.1 M KOH solution. b) Chronoamperometric curves for Fe-N-C-900 and commercial 20 wt% Pt/C in O₂-saturated 0.1 KOH solution at a constant potential of 0.45 V at 1600 r min⁻¹ (color online).