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Title: | Intrinsic spin shielding effect in platinum-rare-earth alloy boosts oxygen reduction activity | Authors: | Zhu, SY Sun, MZ Mei, BB Yang, LT Chu, YY Shi, ZP Bai, JS Wang, X Jiang, Z Liu, CP Huang, BL Ge, JJ Xing, W |
Issue Date: | Sep-2023 | Source: | National science review, Sept 2023, v. 10, no. 9, nwad162 | Abstract: | Oxygen reduction reactions (ORRs) involve a multistep proton-coupled electron process accompanied by the conversion of the apodictic spin configuration. Understanding the role of spin configurations of metals in the adsorption and desorption of oxygen intermediates during ORRs is critical for the design of efficient ORR catalysts. Herein, a platinum-rare-earth-metal-based alloy catalyst, Pt2Gd, is introduced to reveal the role of spin configurations in the catalytic activity of materials. The catalyst exhibits a unique intrinsic spin reconfiguration because of interactions between the Gd-4f and Pt-5d orbitals. The adsorption and desorption of the oxygen species are optimized by modifying the spin symmetry and electronic structures of the material for increased ORR efficiency. The Pt2Gd alloy exhibits a half-wave potential of 0.95 V and a superior mass activity of 1.5 A center dot mgPt-1 in a 0.1 M HClO4 electrolyte, as well as higher durability than conventional Pt/C catalysts. Theoretical calculations have proven that the spin shielding effect of Gd pairs increases the spin symmetry of Pt-5d orbitals and adsorption preferences toward spin-polarized intermediates to facilitate ORR. This work clarifies the impact of modulating the intrinsic spin state of Pt through the interaction with the local high spin 4f orbital electrons in rare-earth metals, with the aim of boosting the spin-related oxygen reduction reaction, thus fundamentally contributing to the understanding of new descriptors that control ORR activity. Deliberately constructing the model for manipulating ORR performance of spin polarized catalysts and accurately decoupling the relationship between the spin state in spin reconfigured alloy and the adsorption strength of the oxide intermediate species. | Keywords: | Oxygen reduction reaction Intermetallic compound Spin effect Rare-earth metal Electrocatalysis |
Publisher: | Oxford University Press | Journal: | National science review | ISSN: | 2095-5138 | EISSN: | 2053-714X | DOI: | 10.1093/nsr/nwad162 | Rights: | © The Author(s) 2023. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd. This is an Open Access article distributed under the terms of the Creative Commons Attribution License (https://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse, distribution, and reproduction in any medium, provided the original work is properly cited. The following publication Siyuan Zhu, Mingzi Sun, Bingbao Mei, Liting Yang, Yuyi Chu, Zhaoping Shi, Jingsen Bai, Xian Wang, Zheng Jiang, Changpeng Liu, Bolong Huang, Junjie Ge, Wei Xing, Intrinsic spin shielding effect in platinum–rare-earth alloy boosts oxygen reduction activity, National Science Review, Volume 10, Issue 9, September 2023, nwad162 is available at https://dx.doi.org/10.1093/nsr/nwad162. |
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