A Caltech Library Service

Comparing the oxygen reduction reaction on selectively edge halogen doped graphene from quantum mechanics

Humphrey, Nicholas and Rodriguez, Roberto and Arias, Gabriel and Thai, Edward and Muro, Evelyn and Merinov, Boris V. and Goddard, William A. and Yu, Ted H. (2020) Comparing the oxygen reduction reaction on selectively edge halogen doped graphene from quantum mechanics. Journal of Catalysis, 381 . pp. 295-307. ISSN 0021-9517. doi:10.1016/j.jcat.2019.10.022.

[img] PDF (Supplementary data) - Supplemental Material
See Usage Policy.


Use this Persistent URL to link to this item:


Recently, edge halogenated graphene-nanosheets (EH-GNS) have been discovered to provide low cost oxygen reduction reaction (ORR) catalysis for alkaline fuel cells. Particularly important is that EH-GNS lead to water as the preferred product whereas undoped graphene leads to peroxide. In order to understand the ORR mechanism, we use density functional theory (DFT) to determine the most probable conformations of the doped graphene after synthesis by ball-milling, to calculate the binding energies of each species, and then to obtain the barriers of each step of the ORR. Our results predict that ORR occurs on the edge of the zigzag with onset potentials of 0.62 (chlorine), 0.66 (bromine), and 0.75 V (iodine) vs. the reversible hydrogen electrode (RHE). Based on our validated theoretical framework, we surveyed other molecules (TeH, BiH₂, SbH₂, OCH₃, SCH₃, SeCH₃) as graphene edge molecules to test for promising ORR catalysts, predicting that SCH₃ would be best.

Item Type:Article
Related URLs:
URLURL TypeDescription
Merinov, Boris V.0000-0002-2783-4262
Goddard, William A.0000-0003-0097-5716
Yu, Ted H.0000-0003-3202-0981
Additional Information:© 2019 Published by Elsevier Inc. Received 13 March 2019, Revised 7 October 2019, Accepted 18 October 2019, Available online 27 November 2019. This research was supported by the National Institute of General Medical Sciences of the National Institutes of Health under Award Nos. 8UL1GM118979-02, 8TL4GM118980-02, and 8RL5GM118978-02 (T.H.Y., E.T., and R.R.) and Office of Naval Research under award N000141812155 (W.A.G. and B.V.M.). The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health. This work is supported by the grants of CSULB Office of Research and Sponsored Program (ORSP) Grant, RSCA Faculty Small Grant, CSULB Start Up Grant, and Southern California Air Quality Management District Grant, Hispanic Serving Institute-STEM (T.H.Y., E.M., and N.H.). We would like to thank In-Yup Jeon for fruitful discussions. We would like to thank the members of Shahab Derakhshan’s lab for x-ray diffraction of EH-GNS. Declaration of Competing Interest: None.
Funding AgencyGrant Number
National Institute of General Medical SciencesUNSPECIFIED
Office of Naval Research (ONR)N000141812155
California State University, Long BeachUNSPECIFIED
Southern California Air Quality Management DistrictUNSPECIFIED
Hispanic Serving InstituteUNSPECIFIED
Subject Keywords:ORR; Graphene; DFT; Halogen; Doped; Fuel cells
Other Numbering System:
Other Numbering System NameOther Numbering System ID
Record Number:CaltechAUTHORS:20191127-113547020
Persistent URL:
Official Citation:Nicholas Humphrey, Roberto Rodriguez, Gabriel Arias, Edward Thai, Evelyn Muro, Boris V. Merinov, William A. Goddard, Ted H. Yu, Comparing the oxygen reduction reaction on selectively edge halogen doped graphene from quantum mechanics, Journal of Catalysis, Volume 381, 2020, Pages 295-307, ISSN 0021-9517, (
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:100104
Deposited By: Tony Diaz
Deposited On:27 Nov 2019 21:00
Last Modified:16 Nov 2021 17:51

Repository Staff Only: item control page