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Title: Functionalization of 2D materials for enhancing OER/ORR catalytic activity in Li–oxygen batteries

Abstract

A major barrier toward the practical application of lithium-oxygen batteries is the high overpotential caused by the precipitation of oxygen-reduction products at the cathode, resulting in poor cyclability. By combining first-principle calculations and reactive molecular dynamics simulations, we show that surface functionalization of 2D MXene nanosheets offers a high degree of tunability of the catalytic activity for oxygen-reduction and oxygen evolution reactions (ORR/OER). We show that the controlled creation of active vacancy sites on the MXene surface enhances ORR in excess of a factor of 60 compared to graphene based cathode materials. Furthermore, we find that increasing the ratio of fluorine vs. oxygen termination of the functionalized Ti4N3-MXene catalyst reduces the charge overpotential by up to 70% and 80% compared with commercial platinum-on-carbon and graphene catalysts, respectively. These results provide direct guidance toward the rational design of functionalized 2D materials for modulating the catalytic activity for a wide range of electrocatalytic applications.

Authors:
ORCiD logo; ORCiD logo; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Mechanistic Control of Water-Hydrocarbon-Rock Interactions in Unconventional and Tight Oil Formations (CMC-UF); Stanford Univ., CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1619756
Alternate Identifier(s):
OSTI ID: 1759004
Grant/Contract Number:  
AC02-05CH11231; SC0019165
Resource Type:
Published Article
Journal Name:
Communications Chemistry
Additional Journal Information:
Journal Name: Communications Chemistry Journal Volume: 2 Journal Issue: 1; Journal ID: ISSN 2399-3669
Publisher:
Springer Nature
Country of Publication:
United Kingdom
Language:
English
Subject:
25 ENERGY STORAGE; Batteries; Two-dimensional materials

Citation Formats

Ostadhossein, Alireza, Guo, Jack, Simeski, Filip, and Ihme, Matthias. Functionalization of 2D materials for enhancing OER/ORR catalytic activity in Li–oxygen batteries. United Kingdom: N. p., 2019. Web. doi:10.1038/s42004-019-0196-2.
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Ostadhossein, Alireza, Guo, Jack, Simeski, Filip, & Ihme, Matthias. Functionalization of 2D materials for enhancing OER/ORR catalytic activity in Li–oxygen batteries. United Kingdom. https://doi.org/10.1038/s42004-019-0196-2
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Ostadhossein, Alireza, Guo, Jack, Simeski, Filip, and Ihme, Matthias. Tue . "Functionalization of 2D materials for enhancing OER/ORR catalytic activity in Li–oxygen batteries". United Kingdom. https://doi.org/10.1038/s42004-019-0196-2.
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@article{osti_1619756,
title = {Functionalization of 2D materials for enhancing OER/ORR catalytic activity in Li–oxygen batteries},
author = {Ostadhossein, Alireza and Guo, Jack and Simeski, Filip and Ihme, Matthias},
abstractNote = {A major barrier toward the practical application of lithium-oxygen batteries is the high overpotential caused by the precipitation of oxygen-reduction products at the cathode, resulting in poor cyclability. By combining first-principle calculations and reactive molecular dynamics simulations, we show that surface functionalization of 2D MXene nanosheets offers a high degree of tunability of the catalytic activity for oxygen-reduction and oxygen evolution reactions (ORR/OER). We show that the controlled creation of active vacancy sites on the MXene surface enhances ORR in excess of a factor of 60 compared to graphene based cathode materials. Furthermore, we find that increasing the ratio of fluorine vs. oxygen termination of the functionalized Ti4N3-MXene catalyst reduces the charge overpotential by up to 70% and 80% compared with commercial platinum-on-carbon and graphene catalysts, respectively. These results provide direct guidance toward the rational design of functionalized 2D materials for modulating the catalytic activity for a wide range of electrocatalytic applications.},
doi = {10.1038/s42004-019-0196-2},
journal = {Communications Chemistry},
number = 1,
volume = 2,
place = {United Kingdom},
year = {Tue Aug 13 00:00:00 EDT 2019},
month = {Tue Aug 13 00:00:00 EDT 2019}
}
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https://doi.org/10.1038/s42004-019-0196-2
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