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http://hdl.handle.net/10397/88365
Title: | Lattice oxygen activation enabled by high-valence metal sites for enhanced water oxidation | Authors: | Zhang, N Feng, X Rao, D Deng, X Cai, L Qiu, B Long, R Xiong, Y Lu, Y Chai, Y |
Issue Date: | 2020 | Source: | Nature communications, 2020, v. 11, no. 1, 4066 | Abstract: | Anodic oxygen evolution reaction (OER) is recognized as kinetic bottleneck in water electrolysis. Transition metal sites with high valence states can accelerate the reaction kinetics to offer highly intrinsic activity, but suffer from thermodynamic formation barrier. Here, we show subtle engineering of highly oxidized Ni4+ species in surface reconstructed (oxy)hydroxides on multicomponent FeCoCrNi alloy film through interatomically electronic interplay. Our spectroscopic investigations with theoretical studies uncover that Fe component enables the formation of Ni4+ species, which is energetically favored by the multistep evolution of Ni2+→Ni3+→Ni4+. The dynamically constructed Ni4+ species drives holes into oxygen ligands to facilitate intramolecular oxygen coupling, triggering lattice oxygen activation to form Fe-Ni dual-sites as ultimate catalytic center with highly intrinsic activity. As a result, the surface reconstructed FeCoCrNi OER catalyst delivers outstanding mass activity and turnover frequency of 3601 A gmetal−1 and 0.483 s−1 at an overpotential of 300 mV in alkaline electrolyte, respectively. | Publisher: | Nature Publishing Group | Journal: | Nature communications | EISSN: | 2041-1723 | DOI: | 10.1038/s41467-020-17934-7 | Rights: | © The Author(s) 2020. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. The following publication Zhang, N., Feng, X., Rao, D. et al. Lattice oxygen activation enabled by high-valence metal sites for enhanced water oxidation. Nat Commun 11, 4066 (2020), is available at https://doi.org/10.1038/s41467-020-17934-7 |
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