Self-Sacrificial Template Synthesis of Fe-N-C Catalysts with Dense Active Sites Deposited on A Porous Carbon Network for High Performance in PEMFC

Li Jiao; Tanvir Alam Arman; Sooyeon Hwang; Javier Fonseca; Norbert Okolie; Ehab Shaaban; Gonghu Li; Ershuai Liu; Ugur Pasaogullari; Siddharth Komini Babu; Sanjeev Mukerjee; Jacob Schatz Spendelow; David A. Cullen; Frédéric Jaouen; Qingying Jia

doi:10.1002/aenm.202303952

Self-Sacrificial Template Synthesis of Fe-N-C Catalysts with Dense Active Sites Deposited on A Porous Carbon Network for High Performance in PEMFC

Li Jiao, Tanvir Alam Arman, Sooyeon Hwang, Javier Fonseca, Norbert Okolie, Ehab Shaaban, Gonghu Li, Ershuai Liu, Ugur Pasaogullari, Siddharth Komini Babu, Sanjeev Mukerjee, Jacob Schatz Spendelow, David A. Cullen, Frédéric Jaouen, Qingying Jia

Materials MicroAnalysis

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11 Scopus citations

Abstract

Iron-nitrogen-carbon (Fe-N-C) single-atom catalysts are promising sustainable alternatives to the costly and scarce platinum (Pt) to catalyze the oxygen reduction reactions (ORR) at the cathode of proton exchange membrane fuel cells (PEMFCs). However, Fe-N-C cathodes for PEMFC are made thicker than Pt/C ones, in order to compensate for the lower intrinsic ORR activity and site density of Fe-N-C materials. The thick electrodes are bound with mass transport issues that limit their performance at high current densities, especially in H₂/air PEMFCs. Practical Fe-N-C electrodes must combine high intrinsic ORR activity, high site density, and fast mass transport. Herein, it has achieved an improved combination of these properties with a Fe-N-C catalyst prepared via a two-step synthesis approach, constructing first a porous zinc-nitrogen-carbon (Zn-N-C) substrate, followed by transmetallating Zn by Fe via chemical vapor deposition. A cathode comprising this Fe-N-C catalyst has exhibited a maximum power density of 0.53 W cm⁻² in H₂/air PEMFC at 80 °C. The improved power density is associated with the hierarchical porosity of the Zn-N-C substrate of this work, which is achieved by epitaxial growth of ZIF-8 onto g-C₃N₄, leading to a micro-mesoporous substrate.

Original language	English
Article number	2303952
Journal	Advanced Energy Materials
Volume	14
Issue number	20
DOIs	https://doi.org/10.1002/aenm.202303952
State	Published - May 24 2024

Funding

The US Department of Energy supported this work under award numbers DE\u2010EE0008416 and the Northeastern University Dissertation Completion Fellowship. The ex\u2010situ XAS experiments were performed at the beamlines 7\u2010BM of the National Synchrotron Light Source II, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory. This research used the Center for Functional Nanomaterials, a US DOE Office of Science Facility, at Brookhaven National Laboratory. G.L. acknowledges the support of the US National Science Foundation through Award 2102655 (N adsorption/desorption analysis). T.A.A., S.K.B. and J.S.S. gratefully acknowledge support from the Laboratory Directed Research and Development program at Los Alamos National Laboratory through project 20200200DR. 2

Keywords

Fe-N-C
chemical vapor deposition
oxygen reduction reaction
proton exchange membrane fuel cells

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10.1002/aenm.202303952

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Jiao, L., Arman, T. A., Hwang, S., Fonseca, J., Okolie, N., Shaaban, E., Li, G., Liu, E., Pasaogullari, U., Babu, S. K., Mukerjee, S., Spendelow, J. S., Cullen, D. A., Jaouen, F., & Jia, Q. (2024). Self-Sacrificial Template Synthesis of Fe-N-C Catalysts with Dense Active Sites Deposited on A Porous Carbon Network for High Performance in PEMFC. Advanced Energy Materials, 14(20), Article 2303952. https://doi.org/10.1002/aenm.202303952

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title = "Self-Sacrificial Template Synthesis of Fe-N-C Catalysts with Dense Active Sites Deposited on A Porous Carbon Network for High Performance in PEMFC",

abstract = "Iron-nitrogen-carbon (Fe-N-C) single-atom catalysts are promising sustainable alternatives to the costly and scarce platinum (Pt) to catalyze the oxygen reduction reactions (ORR) at the cathode of proton exchange membrane fuel cells (PEMFCs). However, Fe-N-C cathodes for PEMFC are made thicker than Pt/C ones, in order to compensate for the lower intrinsic ORR activity and site density of Fe-N-C materials. The thick electrodes are bound with mass transport issues that limit their performance at high current densities, especially in H2/air PEMFCs. Practical Fe-N-C electrodes must combine high intrinsic ORR activity, high site density, and fast mass transport. Herein, it has achieved an improved combination of these properties with a Fe-N-C catalyst prepared via a two-step synthesis approach, constructing first a porous zinc-nitrogen-carbon (Zn-N-C) substrate, followed by transmetallating Zn by Fe via chemical vapor deposition. A cathode comprising this Fe-N-C catalyst has exhibited a maximum power density of 0.53 W cm−2 in H2/air PEMFC at 80 °C. The improved power density is associated with the hierarchical porosity of the Zn-N-C substrate of this work, which is achieved by epitaxial growth of ZIF-8 onto g-C3N4, leading to a micro-mesoporous substrate.",

keywords = "Fe-N-C, chemical vapor deposition, oxygen reduction reaction, proton exchange membrane fuel cells",

author = "Li Jiao and Arman, {Tanvir Alam} and Sooyeon Hwang and Javier Fonseca and Norbert Okolie and Ehab Shaaban and Gonghu Li and Ershuai Liu and Ugur Pasaogullari and Babu, {Siddharth Komini} and Sanjeev Mukerjee and Spendelow, {Jacob Schatz} and Cullen, {David A.} and Fr{\'e}d{\'e}ric Jaouen and Qingying Jia",

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year = "2024",

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Jiao, L, Arman, TA, Hwang, S, Fonseca, J, Okolie, N, Shaaban, E, Li, G, Liu, E, Pasaogullari, U, Babu, SK, Mukerjee, S, Spendelow, JS, Cullen, DA, Jaouen, F & Jia, Q 2024, 'Self-Sacrificial Template Synthesis of Fe-N-C Catalysts with Dense Active Sites Deposited on A Porous Carbon Network for High Performance in PEMFC', Advanced Energy Materials, vol. 14, no. 20, 2303952. https://doi.org/10.1002/aenm.202303952

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T1 - Self-Sacrificial Template Synthesis of Fe-N-C Catalysts with Dense Active Sites Deposited on A Porous Carbon Network for High Performance in PEMFC

AU - Jiao, Li

AU - Arman, Tanvir Alam

AU - Hwang, Sooyeon

AU - Fonseca, Javier

AU - Okolie, Norbert

AU - Shaaban, Ehab

AU - Li, Gonghu

AU - Liu, Ershuai

AU - Pasaogullari, Ugur

AU - Babu, Siddharth Komini

AU - Mukerjee, Sanjeev

AU - Spendelow, Jacob Schatz

AU - Cullen, David A.

AU - Jaouen, Frédéric

AU - Jia, Qingying

PY - 2024/5/24

Y1 - 2024/5/24

N2 - Iron-nitrogen-carbon (Fe-N-C) single-atom catalysts are promising sustainable alternatives to the costly and scarce platinum (Pt) to catalyze the oxygen reduction reactions (ORR) at the cathode of proton exchange membrane fuel cells (PEMFCs). However, Fe-N-C cathodes for PEMFC are made thicker than Pt/C ones, in order to compensate for the lower intrinsic ORR activity and site density of Fe-N-C materials. The thick electrodes are bound with mass transport issues that limit their performance at high current densities, especially in H2/air PEMFCs. Practical Fe-N-C electrodes must combine high intrinsic ORR activity, high site density, and fast mass transport. Herein, it has achieved an improved combination of these properties with a Fe-N-C catalyst prepared via a two-step synthesis approach, constructing first a porous zinc-nitrogen-carbon (Zn-N-C) substrate, followed by transmetallating Zn by Fe via chemical vapor deposition. A cathode comprising this Fe-N-C catalyst has exhibited a maximum power density of 0.53 W cm−2 in H2/air PEMFC at 80 °C. The improved power density is associated with the hierarchical porosity of the Zn-N-C substrate of this work, which is achieved by epitaxial growth of ZIF-8 onto g-C3N4, leading to a micro-mesoporous substrate.

AB - Iron-nitrogen-carbon (Fe-N-C) single-atom catalysts are promising sustainable alternatives to the costly and scarce platinum (Pt) to catalyze the oxygen reduction reactions (ORR) at the cathode of proton exchange membrane fuel cells (PEMFCs). However, Fe-N-C cathodes for PEMFC are made thicker than Pt/C ones, in order to compensate for the lower intrinsic ORR activity and site density of Fe-N-C materials. The thick electrodes are bound with mass transport issues that limit their performance at high current densities, especially in H2/air PEMFCs. Practical Fe-N-C electrodes must combine high intrinsic ORR activity, high site density, and fast mass transport. Herein, it has achieved an improved combination of these properties with a Fe-N-C catalyst prepared via a two-step synthesis approach, constructing first a porous zinc-nitrogen-carbon (Zn-N-C) substrate, followed by transmetallating Zn by Fe via chemical vapor deposition. A cathode comprising this Fe-N-C catalyst has exhibited a maximum power density of 0.53 W cm−2 in H2/air PEMFC at 80 °C. The improved power density is associated with the hierarchical porosity of the Zn-N-C substrate of this work, which is achieved by epitaxial growth of ZIF-8 onto g-C3N4, leading to a micro-mesoporous substrate.

KW - Fe-N-C

KW - chemical vapor deposition

KW - oxygen reduction reaction

KW - proton exchange membrane fuel cells

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JO - Advanced Energy Materials

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Self-Sacrificial Template Synthesis of Fe-N-C Catalysts with Dense Active Sites Deposited on A Porous Carbon Network for High Performance in PEMFC

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