Promoting Atomically Dispersed MnN4 Sites via Sulfur Doping for Oxygen Reduction: Unveiling Intrinsic Activity and Degradation in Fuel Cells
Abstract
Carbon supported and nitrogen coordinated single Mn site catalysts (Mn-N-C) catalysts are the most desirable platinum group metal (PGM)-free cathode catalysts for proton exchange membrane fuel cells (PEMFCs) due to their insignificant Fenton reactions (vs. Fe), earth abundances (vs. Co) and encouraging activity and stability. However, current Mn-N-C catalysts suffer from high over-potential due to low intrinsic activity and less dense MnN4 sites. Herein, we present sulfur-doped Mn-N-C catalyst (Mn-N-C-S) synthesized through an effective adsorption-pyrolysis process. Using electron microscopy and X-ray absorption spectroscopy (XAS) techniques, we verify the uniform dispersion of MnN4 sites and confirm the effect of S doping on the Mn-N coordination. The Mn-N-C-S catalyst exhibits a favorable oxygen reduction reaction (ORR) activity in acidic media relative to the S-free Mn-N-C catalyst. The corresponding membrane electrode assembly (MEA) generated a remarkable performance with a peak power density of 500 mW cm-2 under a realistic H2/air environment. The constant voltage tests of fuel cells confirm the much-enhanced stability of the Mn-N-C-S catalyst compared to the Fe-N-C and Fe-N-C-S catalysts. The electron microscopy and Fourier transform XAS analysis provide insights into catalyst degradation associated with Mn oxidation and agglomeration. The theoretical calculation elucidates that the promoted ORR activity is mainlymore »
- Authors:
-
[2];
[6];
[2];
[5];
[3];
[1];
- State Univ. of New York (SUNY), Buffalo, NY (United States). Dept. of Chemical and Biological Engineering
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Univ. of Pittsburgh, PA (United States). Dept. of Mechanical Engineering and Materials Science
- Giner, Inc., Newton, MA (United States)
- Oregon State Univ., Corvallis, OR (United States). School of Chemical, Biological, and Environmental Engineering
- Univ. of South Carolina, Columbia, SC (United States). Dept. of Chemical Engineering
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Giner, Inc., Newton, MA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1777436
- Alternate Identifier(s):
- OSTI ID: 1813191; OSTI ID: 1873084
- Report Number(s):
- BNL-221266-2021-JAAM
Journal ID: ISSN 1936-0851
- Grant/Contract Number:
- SC0012704; EE0008075; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 15; Journal Issue: 4; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; sulfur doping; single metal site; oxygen reduction; electrocatalysis; fuel cells; catalysts; doping; extended x-ray absorption fine structure; redox reactions; transition metals
Citation Formats
Guo, Lin, Hwang, Sooyeon, Li, Boyang, Yang, Fan, Wang, Maoyu, Chen, Mengjie, Yang, Xiaoxuan, Karakalos, Stavros G., Cullen, David A., Feng, Zhenxing, Wang, Guofeng, Wu, Gang, and Xu, Hui. Promoting Atomically Dispersed MnN4 Sites via Sulfur Doping for Oxygen Reduction: Unveiling Intrinsic Activity and Degradation in Fuel Cells. United States: N. p., 2021.
Web. doi:10.1021/acsnano.0c10637.
Guo, Lin, Hwang, Sooyeon, Li, Boyang, Yang, Fan, Wang, Maoyu, Chen, Mengjie, Yang, Xiaoxuan, Karakalos, Stavros G., Cullen, David A., Feng, Zhenxing, Wang, Guofeng, Wu, Gang, & Xu, Hui. Promoting Atomically Dispersed MnN4 Sites via Sulfur Doping for Oxygen Reduction: Unveiling Intrinsic Activity and Degradation in Fuel Cells. United States. https://doi.org/10.1021/acsnano.0c10637
Guo, Lin, Hwang, Sooyeon, Li, Boyang, Yang, Fan, Wang, Maoyu, Chen, Mengjie, Yang, Xiaoxuan, Karakalos, Stavros G., Cullen, David A., Feng, Zhenxing, Wang, Guofeng, Wu, Gang, and Xu, Hui. Wed .
"Promoting Atomically Dispersed MnN4 Sites via Sulfur Doping for Oxygen Reduction: Unveiling Intrinsic Activity and Degradation in Fuel Cells". United States. https://doi.org/10.1021/acsnano.0c10637. https://www.osti.gov/servlets/purl/1777436.
@article{osti_1777436,
title = {Promoting Atomically Dispersed MnN4 Sites via Sulfur Doping for Oxygen Reduction: Unveiling Intrinsic Activity and Degradation in Fuel Cells},
author = {Guo, Lin and Hwang, Sooyeon and Li, Boyang and Yang, Fan and Wang, Maoyu and Chen, Mengjie and Yang, Xiaoxuan and Karakalos, Stavros G. and Cullen, David A. and Feng, Zhenxing and Wang, Guofeng and Wu, Gang and Xu, Hui},
abstractNote = {Carbon supported and nitrogen coordinated single Mn site catalysts (Mn-N-C) catalysts are the most desirable platinum group metal (PGM)-free cathode catalysts for proton exchange membrane fuel cells (PEMFCs) due to their insignificant Fenton reactions (vs. Fe), earth abundances (vs. Co) and encouraging activity and stability. However, current Mn-N-C catalysts suffer from high over-potential due to low intrinsic activity and less dense MnN4 sites. Herein, we present sulfur-doped Mn-N-C catalyst (Mn-N-C-S) synthesized through an effective adsorption-pyrolysis process. Using electron microscopy and X-ray absorption spectroscopy (XAS) techniques, we verify the uniform dispersion of MnN4 sites and confirm the effect of S doping on the Mn-N coordination. The Mn-N-C-S catalyst exhibits a favorable oxygen reduction reaction (ORR) activity in acidic media relative to the S-free Mn-N-C catalyst. The corresponding membrane electrode assembly (MEA) generated a remarkable performance with a peak power density of 500 mW cm-2 under a realistic H2/air environment. The constant voltage tests of fuel cells confirm the much-enhanced stability of the Mn-N-C-S catalyst compared to the Fe-N-C and Fe-N-C-S catalysts. The electron microscopy and Fourier transform XAS analysis provide insights into catalyst degradation associated with Mn oxidation and agglomeration. The theoretical calculation elucidates that the promoted ORR activity is mainly attributed to the spatial effect stemmed from the repulsive interaction between the ORR intermediates and adjacent S do-pants.},
doi = {10.1021/acsnano.0c10637},
journal = {ACS Nano},
number = 4,
volume = 15,
place = {United States},
year = {Wed Mar 31 00:00:00 EDT 2021},
month = {Wed Mar 31 00:00:00 EDT 2021}
}
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