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Title: Highly Active Bifunctional Oxygen Electrocatalytic Sites Realized in Ceria–Functionalized Graphene

Abstract

The development of efficient, durable, and cost-effective bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is essential in the advancement of solar fuels, metal–air batteries, and unitized regenerative fuel cells. This work demonstrates an effective approach of activating 2D carbon for highly efficient bifunctional oxygen reactions without N-doping, let alone a transition metal–nitrogen (TM–N x) moiety, the usual component needed for high oxygen electrocatalytic activities. A solvothermally synthesized ceria (CeO 2)–hydroxylated graphene hybrid catalyst shows excellent bifunctional ORR/OER activities both in alkaline and acidic solutions. Density functional theory calculations reveal that the activation of graphene occurs via topmost oxygens on ceria surface, but only when low coverage of hydroxyl groups is present on graphene. Furthermore, catalytically active forms of graphene share similar hydroxylated structural motifs. Finally, a simple approach of dramatically enhancing durability even in acidic media is demonstrated.

Authors:
 [1];  [1];  [1];  [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Univ. of California, Merced, CA (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  3. Univ. of California, Davis, CA (United States). Dept. of Chemical Engineering
  4. Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1632149
Alternate Identifier(s):
OSTI ID: 1617748
Grant/Contract Number:  
AC02-76SF00515; AC02‐05CH11231; DE‐SC0008685; NNX15AW57H; NNX15AQ01A; SC0008685
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Sustainable Systems
Additional Journal Information:
Journal Name: Advanced Sustainable Systems; Journal ID: ISSN 2366-7486
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
bifunctional oxygen electrocatalysts; cerium oxide; density functional theory; durability; graphene

Citation Formats

Grewal, Simranjit, Macedo Andrade, Angela, Liu, Ziqi, Garrido Torres, Jose Antonio, Nelson, Art J., Kulkarni, Ambarish, Bajdich, Michal, and Lee, Min Hwan. Highly Active Bifunctional Oxygen Electrocatalytic Sites Realized in Ceria–Functionalized Graphene. United States: N. p., 2020. Web. doi:10.1002/adsu.202000048.
Grewal, Simranjit, Macedo Andrade, Angela, Liu, Ziqi, Garrido Torres, Jose Antonio, Nelson, Art J., Kulkarni, Ambarish, Bajdich, Michal, & Lee, Min Hwan. Highly Active Bifunctional Oxygen Electrocatalytic Sites Realized in Ceria–Functionalized Graphene. United States. https://doi.org/10.1002/adsu.202000048
Grewal, Simranjit, Macedo Andrade, Angela, Liu, Ziqi, Garrido Torres, Jose Antonio, Nelson, Art J., Kulkarni, Ambarish, Bajdich, Michal, and Lee, Min Hwan. Fri . "Highly Active Bifunctional Oxygen Electrocatalytic Sites Realized in Ceria–Functionalized Graphene". United States. https://doi.org/10.1002/adsu.202000048.
@article{osti_1632149,
title = {Highly Active Bifunctional Oxygen Electrocatalytic Sites Realized in Ceria–Functionalized Graphene},
author = {Grewal, Simranjit and Macedo Andrade, Angela and Liu, Ziqi and Garrido Torres, Jose Antonio and Nelson, Art J. and Kulkarni, Ambarish and Bajdich, Michal and Lee, Min Hwan},
abstractNote = {The development of efficient, durable, and cost-effective bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is essential in the advancement of solar fuels, metal–air batteries, and unitized regenerative fuel cells. This work demonstrates an effective approach of activating 2D carbon for highly efficient bifunctional oxygen reactions without N-doping, let alone a transition metal–nitrogen (TM–Nx) moiety, the usual component needed for high oxygen electrocatalytic activities. A solvothermally synthesized ceria (CeO2)–hydroxylated graphene hybrid catalyst shows excellent bifunctional ORR/OER activities both in alkaline and acidic solutions. Density functional theory calculations reveal that the activation of graphene occurs via topmost oxygens on ceria surface, but only when low coverage of hydroxyl groups is present on graphene. Furthermore, catalytically active forms of graphene share similar hydroxylated structural motifs. Finally, a simple approach of dramatically enhancing durability even in acidic media is demonstrated.},
doi = {10.1002/adsu.202000048},
url = {https://www.osti.gov/biblio/1632149}, journal = {Advanced Sustainable Systems},
issn = {2366-7486},
number = ,
volume = ,
place = {United States},
year = {2020},
month = {5}
}

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