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

Grewal, Simranjit; Macedo Andrade, Angela; Liu, Ziqi; Garrido Torres, Jose Antonio; Nelson, Art J.; Kulkarni, Ambarish; Bajdich, Michal; Lee, Min Hwan

doi:10.1002/adsu.202000048

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

Journal Article · Fri May 08 00:00:00 EDT 2020 · Advanced Sustainable Systems

DOI:https://doi.org/10.1002/adsu.202000048· OSTI ID:1632149

Grewal, Simranjit ^[1]; Macedo Andrade, Angela ^[1]; Liu, Ziqi ^[1]; Garrido Torres, Jose Antonio ^[1]; Nelson, Art J. ^[2]; ^[3]; ^[4]; ^[1]

Univ. of California, Merced, CA (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Univ. of California, Davis, CA (United States). Dept. of Chemical Engineering
Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis

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 (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.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231; SC0008685

OSTI ID:: 1632149

Journal Information:: Advanced Sustainable Systems, Journal Name: Advanced Sustainable Systems Journal Issue: 8 Vol. 4; ISSN 2366-7486

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
bifunctional oxygen electrocatalysts
cerium oxide
density functional theory
durability
graphene

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