期刊
CHEMICAL ENGINEERING JOURNAL
卷 409, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2020.128226
关键词
Doped lanthanum nickelate; Ruddlesden-Popper structure; Bifunctional electrocatalyst; Oxygen evolution reaction; Oxygen reduction reaction; Oxygen electrode activity
资金
- Climate Change Technology Research Program [NRF-2015M1A2A2057042]
- Technology Development Program to Hydrogen Energy through the National Research Foundation -Ministry of Science and ICT of Korea [NRF-2019M3E6A1064020]
- Technology Innovation Program - Ministry of Trade, Industry & Energy of (MOTIE) Korea. [20011633]
- Korea Evaluation Institute of Industrial Technology (KEIT) [20011633] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
A systematic study was conducted on Ruddlesden-Popper structured materials for their catalytic performance in oxygen evolution and reduction reactions, resulting in the development of highly efficient bifunctional oxygen catalysts La5Ni4O13-δ and La5Ni3CoO13-δ with outstanding electrocatalytic activity.
A systematic study of the Ruddlesden-Popper structured Lan+1NinO3n+1 (n = 1, 2, 3, and 4) and its catalytic performance in oxygen evolution (OER) and oxygen reduction reactions (ORR) is carried out with a view to design a highly-efficient and cost-effective electrocatalyst. In particular, we introduce for the first time a novel La5Ni4O13-delta with a 4-layered perovskite structure (n = 4) for use as a highly active and durable bifunctional oxygen catalyst for OER/ORR. Concretely, La5Ni4O13-delta catalysts has demonstrated performance of 1.65 V at 10 mA.cm(-2) and 0.66 V at near half-wave potential (-3 mA.cm(-2)) for OER and ORR, respectively, this indicates excellent intrinsic OER/ORR kinetics. Furthermore, by controlling the fuel-to-oxidizer ratio (using extremely fuel-rich conditions) in the glycine-nitrate combustion technique, the 4-layered perovskite La5Ni4O13-delta catalysts are synthesized as a single Ruddlesden-Popper phase with various dopants to further boost its bifunctional oxygen electrode activity. Among OER/ORR catalysts, La5Ni3CoO13-delta catalysts exhibit exceptional electrocatalytic activity with low overpotential and Tafel slope (35/76 mV.dec(-1) for OER/ORR). Outstandingly, the La5Ni3CoO13-delta is able to achieve an extremely low overpotential of 370 mV at 10 mA.cm(-2) in 0.1 M KOH for OER, surpassing Ir/C catalysts and any metal oxide catalyst ever reported. The high catalytic performance of La5Ni3CoO13-delta can be attributed to its favorable electronic structure enriched with oxygen defects and electronic charge carriers (increased Ni oxidation state) as well as to the promoted lattice-oxygen oxidation mechanism pathway that comes from strong metal-oxygen covalency (high oxygen-ion diffusion rate).
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