Coordination Chemistry of [Co(acac)2 ] with N-Doped Graphene: Implications for Oxygen Reduction Reaction Reactivity of Organometallic Co-O4 -N Species.
Hybridization of organometallic complexes with graphene-based materials can give rise to enhanced catalytic performance. Understanding the chemical structures within hybrid materials is of primary importance. In this work, archetypical hybrid materials are synthesized by the reaction of an organometallic complex, [Co(II) (acac)2 ] (acac=acetylacetonate), with N-doped graphene-based materials at room temperature. Experimental characterization of the hybrid materials and theoretical calculations reveal that the organometallic cobalt-containing species is coordinated to heterocyclic groups in N-doped graphene as well as to its parental acac ligands. The hybrid material shows high electrocatalytic activity for the oxygen reduction reaction (ORR) in alkaline media, and superior durability and methanol tolerance to a Pt/C catalyst. Based on the chemical structures and ORR experiments, the catalytically active species is identified as a Co-O4 -N structure.
Department of Chemistry and Chemical Engineering, Inha University, 100 Inha-ro, Nam-gu, Incheon 402-751 (Republic of Korea).
Jongwoo
J
Han
Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulsan 689-798 (Republic of Korea).
Young Jin
YJ
Sa
Department of Chemistry and Chemical Engineering, Inha University, 100 Inha-ro, Nam-gu, Incheon 402-751 (Republic of Korea).
Yeonjun
Y
Shim
Department of Physics and Center for Multidimensional Carbon Materials, UNIST, 50 UNIST-gil, Ulsan 689-798 (Republic of Korea).
Min
M
Choi
Department of Physics and Center for Multidimensional Carbon Materials, UNIST, 50 UNIST-gil, Ulsan 689-798 (Republic of Korea).
Noejung
N
Park
Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulsan 689-798 (Republic of Korea). shjoo@unist.ac.kr.|School of Energy and Chemical Engineering, UNIST, 50 UNIST-gil, Ulsan 689-798 (Republic of Korea). shjoo@unist.ac.kr.
Sang Hoon
SH
Joo
Department of Chemistry and Chemical Engineering, Inha University, 100 Inha-ro, Nam-gu, Incheon 402-751 (Republic of Korea). sungjinpark@inha.ac.kr.
Sungjin
S
Park
cobalt; electrocatalysis; heterogeneous catalysis; nanomaterials; solid-state NMR