Single-Atom Catalysts for Selective Oxygen Reduction: Transition Metals in Uniform Carbon Nanospheres with High Loadings
Abstract
Transition metal single-atom catalysts (SACs) in uniform carbon nanospheres have gained tremendous interest as electrocatalysts owing to their low cost, high activity, and excellent selectivity. However, their preparation typically involves complicated multistep processes that are not practical for industrial use. Herein, we report a facile one-pot method to produce atomically isolated metal atoms with high loadings in uniform carbon nanospheres without any templates or postsynthesis modifications. Specifically, we use a chemical confinement strategy to suppress the formation of metal nanoparticles by introducing ethylenediaminetetraacetic acid (EDTA) as a molecular barrier to spatially isolate the metal atoms and thus generate SACs. To demonstrate the versatility of this synthetic method, we produced SACs from multiple transition metals, including Fe, Co, Cu, and Ni, with loadings as high as 3.87 wt %. Among these catalytic materials, the Fe-based SACs showed remarkable catalytic activity toward the oxygen reduction reaction (ORR), achieving an onset and half-wave potential of 1.00 and 0.831 VRHE, respectively, comparable to that of commercial 20 wt % Pt/C. Significantly, we were able to steer the ORR selectivity toward either energy generation or hydrogen peroxide production by simply changing the transition metal in the EDTA-based precursor.
- Authors:
-
[1];
[3];
[4];
[5];
[6]
- School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
- School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
- Applied Materials Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
- Advanced Photon Source, Argonne National Laboratory, Lemont, Illinois 60439, United States
- Department of Chemistry and Biochemistry, Kent State University, Kent, Ohio 44242, United States
- School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, United States, The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, Atlanta, Georgia 30332, United States, School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
- Publication Date:
- Research Org.:
- Georgia Institute of Technology, Atlanta, GA (United States)
- Sponsoring Org.:
- USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
- OSTI Identifier:
- 2203179
- Alternate Identifier(s):
- OSTI ID: 2222391
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Published Article
- Journal Name:
- JACS Au
- Additional Journal Information:
- Journal Name: JACS Au Journal Volume: 3 Journal Issue: 11; Journal ID: ISSN 2691-3704
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; single-atom catalyst; carbon nanospheres; chemical confinement; one-pot; oxygen reduction reaction; catalysts; metals; nanospheres; redox reactions; transition metals
Citation Formats
Jeskey, Jacob, Ding, Yong, Chen, Yidan, Hood, Zachary D., Sterbinsky, George E., Jaroniec, Mietek, and Xia, Younan. Single-Atom Catalysts for Selective Oxygen Reduction: Transition Metals in Uniform Carbon Nanospheres with High Loadings. United States: N. p., 2023.
Web. doi:10.1021/jacsau.3c00557.
Jeskey, Jacob, Ding, Yong, Chen, Yidan, Hood, Zachary D., Sterbinsky, George E., Jaroniec, Mietek, & Xia, Younan. Single-Atom Catalysts for Selective Oxygen Reduction: Transition Metals in Uniform Carbon Nanospheres with High Loadings. United States. https://doi.org/10.1021/jacsau.3c00557
Jeskey, Jacob, Ding, Yong, Chen, Yidan, Hood, Zachary D., Sterbinsky, George E., Jaroniec, Mietek, and Xia, Younan. Thu .
"Single-Atom Catalysts for Selective Oxygen Reduction: Transition Metals in Uniform Carbon Nanospheres with High Loadings". United States. https://doi.org/10.1021/jacsau.3c00557.
@article{osti_2203179,
title = {Single-Atom Catalysts for Selective Oxygen Reduction: Transition Metals in Uniform Carbon Nanospheres with High Loadings},
author = {Jeskey, Jacob and Ding, Yong and Chen, Yidan and Hood, Zachary D. and Sterbinsky, George E. and Jaroniec, Mietek and Xia, Younan},
abstractNote = {Transition metal single-atom catalysts (SACs) in uniform carbon nanospheres have gained tremendous interest as electrocatalysts owing to their low cost, high activity, and excellent selectivity. However, their preparation typically involves complicated multistep processes that are not practical for industrial use. Herein, we report a facile one-pot method to produce atomically isolated metal atoms with high loadings in uniform carbon nanospheres without any templates or postsynthesis modifications. Specifically, we use a chemical confinement strategy to suppress the formation of metal nanoparticles by introducing ethylenediaminetetraacetic acid (EDTA) as a molecular barrier to spatially isolate the metal atoms and thus generate SACs. To demonstrate the versatility of this synthetic method, we produced SACs from multiple transition metals, including Fe, Co, Cu, and Ni, with loadings as high as 3.87 wt %. Among these catalytic materials, the Fe-based SACs showed remarkable catalytic activity toward the oxygen reduction reaction (ORR), achieving an onset and half-wave potential of 1.00 and 0.831 VRHE, respectively, comparable to that of commercial 20 wt % Pt/C. Significantly, we were able to steer the ORR selectivity toward either energy generation or hydrogen peroxide production by simply changing the transition metal in the EDTA-based precursor.},
doi = {10.1021/jacsau.3c00557},
journal = {JACS Au},
number = 11,
volume = 3,
place = {United States},
year = {Thu Oct 19 00:00:00 EDT 2023},
month = {Thu Oct 19 00:00:00 EDT 2023}
}
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