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Author Kante, M.V.; Weber, M.L.; Ni, S.; van den Bosch, I.C.G.; van der Minne, E.; Heymann, L.; Falling, L.J.; Gauquelin, N.; Tsvetanova, M.; Cunha, D.M.; Koster, G.; Gunkel, F.; Nemsak, S.; Hahn, H.; Estrada, L.V.; Baeumer, C.
Title A high-entropy oxide as high-activity electrocatalyst for water oxidation Type A1 Journal article
Year 2023 Publication ACS nano Abbreviated Journal
Volume 17 Issue 6 Pages 5329-5339
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract High-entropy materials are an emerging pathway in the development of high-activity (electro)catalysts because of the inherent tunability and coexistence of multiple potential active sites, which may lead to earth-abundant catalyst materials for energy-efficient electrochemical energy storage. In this report, we identify how the multication composition in high-entropy perovskite oxides (HEO) contributes to high catalytic activity for the oxygen evolution reaction (OER), i.e., the key kinetically limiting half-reaction in several electrochemical energy conversion technologies, including green hydrogen generation. We compare the activity of the (001) facet of LaCr0.2Mn0.2Fe0.2Co0.2Ni0.2O3-delta with the parent compounds (single B-site in the ABO3 perovskite). While the single B-site perovskites roughly follow the expected volcano-type activity trends, the HEO clearly outperforms all of its parent compounds with 17 to 680 times higher currents at a fixed overpotential. As all samples were grown as an epitaxial layer, our results indicate an intrinsic composition-function relationship, avoiding the effects of complex geometries or unknown surface composition. In-depth X-ray photoemission studies reveal a synergistic effect of simultaneous oxidation and reduction of different transition metal cations during the adsorption of reaction intermediates. The surprisingly high OER activity demonstrates that HEOs are a highly attractive, earth-abundant material class for high-activity OER electrocatalysts, possibly allowing the activity to be fine-tuned beyond the scaling limits of mono-or bimetallic oxides.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000953440900001 Publication Date 2023-03-13
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 17.1 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 17.1; 2023 IF: 13.942
Call Number UA @ admin @ c:irua:196097 Serial 7390
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Author Chen, Y.Z.; Trier, F.; Wijnands, T.; Green, R.J.; Gauquelin, N.; Egoavil, R.; Christensen, D.V.; Koster, G.; Huijben, M.; Bovet, N.; Macke, S.; He, F.; Sutarto, R.; Andersen, N.H.; Sulpizio, J.A.; Honig, M.; Prawiroatmodjo, G.E.D.K.; Jespersen, T.S.; Linderoth, S.; Ilani, S.; Verbeeck, J.; Van Tendeloo, G.; Rijnders, G.; Sawatzky, G.A.; Pryds, N.
Title Extreme mobility enhancement of two-dimensional electron gases at oxide interfaces by charge-transfer-induced modulation doping Type A1 Journal article
Year 2015 Publication Nature materials Abbreviated Journal Nat Mater
Volume 14 Issue 14 Pages 801-806
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Two-dimensional electron gases (2DEGs) formed at the interface of insulating complex oxides promise the development of all-oxide electronic devices. These 2DEGs involve many-body interactions that give rise to a variety of physical phenomena such as superconductivity, magnetism, tunable metalinsulator transitions and phase separation. Increasing the mobility of the 2DEG, however, remains a major challenge. Here, we show that the electron mobility is enhanced by more than two orders of magnitude by inserting a single-unit-cell insulating layer of polar La1−xSrxMnO3 (x = 0, 1/8, and 1/3) at the interface between disordered LaAlO3 and crystalline SrTiO3 produced at room temperature. Resonant X-ray spectroscopy and transmission electron microscopy show that the manganite layer undergoes unambiguous electronic reconstruction, leading to modulation doping of such atomically engineered complex oxide heterointerfaces. At low temperatures, the modulation-doped 2DEG exhibits Shubnikovde Haas oscillations and fingerprints of the quantum Hall effect, demonstrating unprecedented high mobility and low electron density.
Address
Corporate Author Thesis
Publisher Place of Publication London Editor
Language Wos 000358530100022 Publication Date 2015-06-01
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1476-1122;1476-4660; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor (up) 39.737 Times cited 170 Open Access
Notes 246102 IFOX; 246791 COUNTATOMS; 278510 VORTEX; Hercules; 312483 ESTEEM2; FWO G004413N; esteem2jra3 ECASJO; Approved Most recent IF: 39.737; 2015 IF: 36.503
Call Number c:irua:127184 c:irua:127184UA @ admin @ c:irua:127184 Serial 1163
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