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Geometric Occupancy and Oxidation State Requirements of Cations in Cobalt Oxides for Oxygen Reduction Reaction
Liu, Jing; Bao, Hongliang; Zhang, Bingsen; Hua, Qingfeng; Shang, Mingfeng; Wang, Jianqiang; Jiang, Luhua
2019-04-03
Source PublicationACS APPLIED MATERIALS & INTERFACES
ISSN1944-8244
Volume11Issue:13Pages:12525-12534
AbstractCobalt oxides, including spinel Co3O4 and rock-salt CoO, have been widely reported as promising catalysts for oxygen reduction reaction (ORR). However, three types of cobalt ions, i.e., Co2+ in the tetrahedral site (Co-Td(2+)), Co3+ in the octahedral site (Co-Oh(3+)), and Co2+ in the octahedral site (Co-Oh(2+)), are included in these oxides, and the roles of cobalt geometric occupancy and valance states have remained elusive. Here, for the first time, we investigated the effects of cobalt geometric occupancy on the ORR activity by substituting Co-Td(2+) and Co-Oh(3+) of Co3O4 with inactive Zn2+ and Al3+, respectively. The ORR activity decreases in the order of Co3O4 (Co-Oh(3+), Co-Td(2+)) < ZnCo2O4 (Co-Oh(3+)) << CoAl2O4 (Co-Td(2+)) in accordance with the ORR overpotentials at the current density of 0.1 mA cm(Ox)(-2). Furthermore, by comparatively investigating the activity and stability of Co3O4 (Co-Oh(3+)) and CoO (Co-Oh(2+)) nanoparticles, by virtue of the electrochemical technique, the high-resolution transmission electron microscopy, and the in operando fuel cell-X-ray absorption spectroscopy techniques, it was revealed that Co-Oh(2+), in CoO is the main active site, which under electrochemical conditions tends to transform into Co-Oh(3+), and form Co3O4 with a hollow structure due to the Kirkendall effect; nevertheless, it retains decent ORR activity due to the formation of the unique hollow structure.
Keywordcobalt oxide oxygen reduction reaction geometric occupancy valance state octahedral coordination
Indexed BySCI
Language英语
WOS IDWOS:000463843900039
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:3[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/81199
Collection中国科学院金属研究所
Recommended Citation
GB/T 7714
Liu, Jing,Bao, Hongliang,Zhang, Bingsen,et al. Geometric Occupancy and Oxidation State Requirements of Cations in Cobalt Oxides for Oxygen Reduction Reaction[J]. ACS APPLIED MATERIALS & INTERFACES,2019,11(13):12525-12534.
APA Liu, Jing.,Bao, Hongliang.,Zhang, Bingsen.,Hua, Qingfeng.,Shang, Mingfeng.,...&Jiang, Luhua.(2019).Geometric Occupancy and Oxidation State Requirements of Cations in Cobalt Oxides for Oxygen Reduction Reaction.ACS APPLIED MATERIALS & INTERFACES,11(13),12525-12534.
MLA Liu, Jing,et al."Geometric Occupancy and Oxidation State Requirements of Cations in Cobalt Oxides for Oxygen Reduction Reaction".ACS APPLIED MATERIALS & INTERFACES 11.13(2019):12525-12534.
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