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表面吸附和插层(氧)阴离子对析氧反应的影响。

Effect of Surface-Adsorbed and Intercalated (Oxy)anions on the Oxygen Evolution Reaction.

作者信息

Hausmann J Niklas, Menezes Prashanth W

机构信息

Department of Chemistry: Metalorganics and Inorganic Materials, Technische Universität Berlin, Straße des 17 Juni 135, Sekr. C2, 10623, Berlin, Germany.

Material Chemistry Group for Thin Film Catalysis-CatLab, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Str. 15, 12489, Berlin, Germany.

出版信息

Angew Chem Int Ed Engl. 2022 Sep 19;61(38):e202207279. doi: 10.1002/anie.202207279. Epub 2022 Aug 4.

Abstract

As the kinetically demanding oxygen evolution reaction (OER) is crucial for the decarbonization of our society, a wide range of (pre)catalysts with various non-active-site elements (e.g., Mo, S, Se, N, P, C, Si…) have been investigated. Thermodynamics dictate that these elements oxidize during industrial operation. The formed oxyanions are water soluble and thus predominantly leach in a reconstruction process. Nevertheless, recently, it was unveiled that these thermodynamically stable (oxy)anions can adsorb on the surface or intercalate in the interlayer space of the active catalyst. There, they tune the electronic properties of the active sites and can interact with the reaction intermediates, changing the OER kinetics and potentially breaking the persisting OER *OH/*OOH scaling relations. Thus, the addition of (oxy)anions to the electrolyte opens a new design dimension for OER catalysis and the herein discussed observations deepen the understanding of the role of anions in the OER.

摘要

由于对动力学要求苛刻的析氧反应(OER)对我们社会的脱碳至关重要,人们已经研究了各种含有不同非活性位点元素(如Mo、S、Se、N、P、C、Si…)的(预)催化剂。热力学表明,这些元素在工业运行过程中会发生氧化。形成的含氧阴离子可溶于水,因此在重构过程中主要会浸出。然而,最近有研究表明,这些热力学稳定的(含氧)阴离子可以吸附在活性催化剂的表面或插入其层间空间。在那里,它们调节活性位点的电子性质,并能与反应中间体相互作用,改变OER动力学,并有可能打破持续存在的OER *OH/*OOH标度关系。因此,向电解质中添加(含氧)阴离子为OER催化开辟了一个新的设计维度,本文所讨论的观察结果加深了我们对阴离子在OER中作用的理解。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e12f/9546270/15ba034ab724/ANIE-61-0-g003.jpg

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