Creation of densely exposed and cavity-edged single Fe active sites for enhanced oxygen electroreduction

Fantao Kong; Yifan Huang; Meixin Chen; Ge Meng; Han Tian; Yafeng Chen; Ziwei Chang; Chang Chen; Wenping Sun; Xiangzhi Cui; Jianlin Shi

doi:10.1016/j.apcatb.2022.121768

Creation of densely exposed and cavity-edged single Fe active sites for enhanced oxygen electroreduction

Fantao Kong, Yifan Huang, Meixin Chen, Ge Meng, Han Tian, Yafeng Chen, Ziwei Chang, Chang Chen, Wenping Sun, Xiangzhi Cui^*, Jianlin Shi

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

36 Scopus citations

Abstract

The performance of oxygen reduction reaction (ORR) on Fe-N-C single-atom catalysts (SACs) is still less satisfactory due to the rather low atom-utilization of active sites. Here, a novel acetate thermolysis-assisted route is proposed to create hierarchical carbon nanocages of Fe-N-C SACs (Fe_SA-N/Cs-OAc) by selective cleavage of carbon layers, which features abundant edge-sited Fe-N₄ moieties in well-defined mesoporous channels. Benefiting from the ultra-high site density and utilization of Fe-N₄ moieties, the optimized Fe_SA-N/Cs-OAc catalyst demonstrates excellent ORR activities marked by extraordinarily high half-wave potentials (E_1/2) of 0.94 V and 0.82 V in alkaline and acidic electrolytes. Zn-air battery using Fe_SA-N/Cs-OAc as cathode delivers a power density of 165 mW cm⁻², and the maximum output power in H₂-O₂ fuel cell reaches 640 mW cm⁻². The abundant mesoporosity makes most Fe-N₄ sites accessible and simultaneously produces in-plane pore defects that reduced adsorption energy of *OH (−0.72 eV), finally presenting remarkably enhanced ORR performance.

Original language	English
Article number	121768
Journal	Applied Catalysis B: Environmental
Volume	317
DOIs	https://doi.org/10.1016/j.apcatb.2022.121768
State	Published - 15 Nov 2022
Externally published	Yes

Keywords

Acetate-assisted thermolysis
Edge-sited Fe-Nx
Electrocatalysis
Fuel cells
Nanoporous carbon

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10.1016/j.apcatb.2022.121768

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title = "Creation of densely exposed and cavity-edged single Fe active sites for enhanced oxygen electroreduction",

abstract = "The performance of oxygen reduction reaction (ORR) on Fe-N-C single-atom catalysts (SACs) is still less satisfactory due to the rather low atom-utilization of active sites. Here, a novel acetate thermolysis-assisted route is proposed to create hierarchical carbon nanocages of Fe-N-C SACs (FeSA-N/Cs-OAc) by selective cleavage of carbon layers, which features abundant edge-sited Fe-N4 moieties in well-defined mesoporous channels. Benefiting from the ultra-high site density and utilization of Fe-N4 moieties, the optimized FeSA-N/Cs-OAc catalyst demonstrates excellent ORR activities marked by extraordinarily high half-wave potentials (E1/2) of 0.94 V and 0.82 V in alkaline and acidic electrolytes. Zn-air battery using FeSA-N/Cs-OAc as cathode delivers a power density of 165 mW cm−2, and the maximum output power in H2-O2 fuel cell reaches 640 mW cm−2. The abundant mesoporosity makes most Fe-N4 sites accessible and simultaneously produces in-plane pore defects that reduced adsorption energy of *OH (−0.72 eV), finally presenting remarkably enhanced ORR performance.",

keywords = "Acetate-assisted thermolysis, Edge-sited Fe-Nx, Electrocatalysis, Fuel cells, Nanoporous carbon",

author = "Fantao Kong and Yifan Huang and Meixin Chen and Ge Meng and Han Tian and Yafeng Chen and Ziwei Chang and Chang Chen and Wenping Sun and Xiangzhi Cui and Jianlin Shi",

note = "Publisher Copyright: {\textcopyright} 2022 Elsevier B.V.",

year = "2022",

month = nov,

day = "15",

doi = "10.1016/j.apcatb.2022.121768",

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TY - JOUR

T1 - Creation of densely exposed and cavity-edged single Fe active sites for enhanced oxygen electroreduction

AU - Kong, Fantao

AU - Huang, Yifan

AU - Chen, Meixin

AU - Meng, Ge

AU - Tian, Han

AU - Chen, Yafeng

AU - Chang, Ziwei

AU - Chen, Chang

AU - Sun, Wenping

AU - Cui, Xiangzhi

AU - Shi, Jianlin

PY - 2022/11/15

Y1 - 2022/11/15

N2 - The performance of oxygen reduction reaction (ORR) on Fe-N-C single-atom catalysts (SACs) is still less satisfactory due to the rather low atom-utilization of active sites. Here, a novel acetate thermolysis-assisted route is proposed to create hierarchical carbon nanocages of Fe-N-C SACs (FeSA-N/Cs-OAc) by selective cleavage of carbon layers, which features abundant edge-sited Fe-N4 moieties in well-defined mesoporous channels. Benefiting from the ultra-high site density and utilization of Fe-N4 moieties, the optimized FeSA-N/Cs-OAc catalyst demonstrates excellent ORR activities marked by extraordinarily high half-wave potentials (E1/2) of 0.94 V and 0.82 V in alkaline and acidic electrolytes. Zn-air battery using FeSA-N/Cs-OAc as cathode delivers a power density of 165 mW cm−2, and the maximum output power in H2-O2 fuel cell reaches 640 mW cm−2. The abundant mesoporosity makes most Fe-N4 sites accessible and simultaneously produces in-plane pore defects that reduced adsorption energy of *OH (−0.72 eV), finally presenting remarkably enhanced ORR performance.

AB - The performance of oxygen reduction reaction (ORR) on Fe-N-C single-atom catalysts (SACs) is still less satisfactory due to the rather low atom-utilization of active sites. Here, a novel acetate thermolysis-assisted route is proposed to create hierarchical carbon nanocages of Fe-N-C SACs (FeSA-N/Cs-OAc) by selective cleavage of carbon layers, which features abundant edge-sited Fe-N4 moieties in well-defined mesoporous channels. Benefiting from the ultra-high site density and utilization of Fe-N4 moieties, the optimized FeSA-N/Cs-OAc catalyst demonstrates excellent ORR activities marked by extraordinarily high half-wave potentials (E1/2) of 0.94 V and 0.82 V in alkaline and acidic electrolytes. Zn-air battery using FeSA-N/Cs-OAc as cathode delivers a power density of 165 mW cm−2, and the maximum output power in H2-O2 fuel cell reaches 640 mW cm−2. The abundant mesoporosity makes most Fe-N4 sites accessible and simultaneously produces in-plane pore defects that reduced adsorption energy of *OH (−0.72 eV), finally presenting remarkably enhanced ORR performance.

KW - Acetate-assisted thermolysis

KW - Edge-sited Fe-Nx

KW - Electrocatalysis

KW - Fuel cells

KW - Nanoporous carbon

UR - https://www.scopus.com/pages/publications/85134902260

U2 - 10.1016/j.apcatb.2022.121768

DO - 10.1016/j.apcatb.2022.121768

M3 - 文章

AN - SCOPUS:85134902260

SN - 0926-3373

VL - 317

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 121768

ER -

Creation of densely exposed and cavity-edged single Fe active sites for enhanced oxygen electroreduction

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Keywords

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