Wu Tianze, Ren Xiao, Sun Yuanmiao, Sun Shengnan, Xian Guoyu, Scherer Günther G, Fisher Adrian C, Mandler Daniel, Ager Joel W, Grimaud Alexis, Wang Junling, Shen Chengmin, Yang Haitao, Gracia Jose, Gao Hong-Jun, Xu Zhichuan J
School of Materials Science and Engineering, Nanyang Technological University, Singapore, Singapore.
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Science, Beijing, China.
Nat Commun. 2021 Jun 15;12(1):3634. doi: 10.1038/s41467-021-23896-1.
Producing hydrogen by water electrolysis suffers from the kinetic barriers in the oxygen evolution reaction (OER) that limits the overall efficiency. With spin-dependent kinetics in OER, to manipulate the spin ordering of ferromagnetic OER catalysts (e.g., by magnetization) can reduce the kinetic barrier. However, most active OER catalysts are not ferromagnetic, which makes the spin manipulation challenging. In this work, we report a strategy with spin pinning effect to make the spins in paramagnetic oxyhydroxides more aligned for higher intrinsic OER activity. The spin pinning effect is established in oxide/oxyhydroxide interface which is realized by a controlled surface reconstruction of ferromagnetic oxides. Under spin pinning, simple magnetization further increases the spin alignment and thus the OER activity, which validates the spin effect in rate-limiting OER step. The spin polarization in OER highly relies on oxyl radicals (O∙) created by 1 dehydrogenation to reduce the barrier for subsequent O-O coupling.
通过水电解制氢存在析氧反应（OER）中的动力学障碍，这限制了整体效率。由于OER中存在自旋相关动力学，操纵铁磁OER催化剂的自旋排序（例如通过磁化）可以降低动力学障碍。然而，大多数活性OER催化剂不是铁磁性的，这使得自旋操纵具有挑战性。在这项工作中，我们报告了一种具有自旋钉扎效应的策略，使顺磁性羟基氧化物中的自旋更有序，以获得更高的本征OER活性。自旋钉扎效应在氧化物/羟基氧化物界面中建立，这是通过铁磁氧化物的可控表面重构实现的。在自旋钉扎下，简单的磁化进一步增加了自旋排列，从而提高了OER活性，这验证了限速OER步骤中的自旋效应。OER中的自旋极化高度依赖于由1脱氢产生的氧自由基（O∙）来降低随后O-O耦合的势垒。
Zotero 插件
