First-Principles Design of Graphene-Based Active Catalysts for Oxygen Reduction and Evolution Reactions in the Aprotic Li-O2 Battery

Joonhee Kang, Jong Sung Yu, Byungchan Han

Research output: Contribution to journalArticle

23 Citations (Scopus)

Abstract

Using first-principles density functional theory (DFT) calculations, we demonstrate that catalytic activities toward oxygen reduction and evolution reactions (ORR and OER) in a Li-O2 battery can be substantially improved with graphene-based materials. We accomplish the goal by calculating free energy diagrams for the redox reactions of oxygen to identify a rate-determining step controlling the overpotentials. We unveil that the catalytic performance is well described by the adsorption energies of the intermediates LiO2 and Li2O2 and propose that graphene-based materials can be substantially optimized through either by N doping or encapsulating Cu(111) single crystals. Furthermore, our systematic approach with DFT calculations applied to design of optimum catalysts enables screening of promising candidates for the oxygen electrochemistry leading to considerable improvement of efficiency of a range of renewable energy devices.

Original languageEnglish
Pages (from-to)2803-2808
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume7
Issue number14
DOIs
Publication statusPublished - 2016 Jul 21

Fingerprint

Graphite
Graphene
electric batteries
graphene
Oxygen
catalysts
Catalysts
Density functional theory
oxygen
density functional theory
encapsulating
renewable energy
Redox reactions
Electrochemistry
electrochemistry
Free energy
catalytic activity
Catalyst activity
Screening
screening

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

Cite this

@article{042823d2306044e4836e2f0bab72dc11,
title = "First-Principles Design of Graphene-Based Active Catalysts for Oxygen Reduction and Evolution Reactions in the Aprotic Li-O2 Battery",
abstract = "Using first-principles density functional theory (DFT) calculations, we demonstrate that catalytic activities toward oxygen reduction and evolution reactions (ORR and OER) in a Li-O2 battery can be substantially improved with graphene-based materials. We accomplish the goal by calculating free energy diagrams for the redox reactions of oxygen to identify a rate-determining step controlling the overpotentials. We unveil that the catalytic performance is well described by the adsorption energies of the intermediates LiO2 and Li2O2 and propose that graphene-based materials can be substantially optimized through either by N doping or encapsulating Cu(111) single crystals. Furthermore, our systematic approach with DFT calculations applied to design of optimum catalysts enables screening of promising candidates for the oxygen electrochemistry leading to considerable improvement of efficiency of a range of renewable energy devices.",
author = "Joonhee Kang and Yu, {Jong Sung} and Byungchan Han",
year = "2016",
month = "7",
day = "21",
doi = "10.1021/acs.jpclett.6b01071",
language = "English",
volume = "7",
pages = "2803--2808",
journal = "Journal of Physical Chemistry Letters",
issn = "1948-7185",
publisher = "American Chemical Society",
number = "14",

}

First-Principles Design of Graphene-Based Active Catalysts for Oxygen Reduction and Evolution Reactions in the Aprotic Li-O2 Battery. / Kang, Joonhee; Yu, Jong Sung; Han, Byungchan.

In: Journal of Physical Chemistry Letters, Vol. 7, No. 14, 21.07.2016, p. 2803-2808.

Research output: Contribution to journalArticle

TY - JOUR

T1 - First-Principles Design of Graphene-Based Active Catalysts for Oxygen Reduction and Evolution Reactions in the Aprotic Li-O2 Battery

AU - Kang, Joonhee

AU - Yu, Jong Sung

AU - Han, Byungchan

PY - 2016/7/21

Y1 - 2016/7/21

N2 - Using first-principles density functional theory (DFT) calculations, we demonstrate that catalytic activities toward oxygen reduction and evolution reactions (ORR and OER) in a Li-O2 battery can be substantially improved with graphene-based materials. We accomplish the goal by calculating free energy diagrams for the redox reactions of oxygen to identify a rate-determining step controlling the overpotentials. We unveil that the catalytic performance is well described by the adsorption energies of the intermediates LiO2 and Li2O2 and propose that graphene-based materials can be substantially optimized through either by N doping or encapsulating Cu(111) single crystals. Furthermore, our systematic approach with DFT calculations applied to design of optimum catalysts enables screening of promising candidates for the oxygen electrochemistry leading to considerable improvement of efficiency of a range of renewable energy devices.

AB - Using first-principles density functional theory (DFT) calculations, we demonstrate that catalytic activities toward oxygen reduction and evolution reactions (ORR and OER) in a Li-O2 battery can be substantially improved with graphene-based materials. We accomplish the goal by calculating free energy diagrams for the redox reactions of oxygen to identify a rate-determining step controlling the overpotentials. We unveil that the catalytic performance is well described by the adsorption energies of the intermediates LiO2 and Li2O2 and propose that graphene-based materials can be substantially optimized through either by N doping or encapsulating Cu(111) single crystals. Furthermore, our systematic approach with DFT calculations applied to design of optimum catalysts enables screening of promising candidates for the oxygen electrochemistry leading to considerable improvement of efficiency of a range of renewable energy devices.

UR - http://www.scopus.com/inward/record.url?scp=84979500117&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84979500117&partnerID=8YFLogxK

U2 - 10.1021/acs.jpclett.6b01071

DO - 10.1021/acs.jpclett.6b01071

M3 - Article

AN - SCOPUS:84979500117

VL - 7

SP - 2803

EP - 2808

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

SN - 1948-7185

IS - 14

ER -