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A soft molecular 2Fe–2As precursor approach to the synthesis of nanostructured FeAs for efficient electrocatalytic water oxidation
Chemical Science ( IF 8.4 ) Pub Date : 2020-10-07 , DOI: 10.1039/d0sc04384b
Rodrigo Beltrán-Suito 1, 2, 3, 4 , Viktoria Forstner 1, 2, 3, 4 , J. Niklas Hausmann 1, 2, 3, 4 , Stefan Mebs 4, 5, 6, 7 , Johannes Schmidt 2, 4, 8, 9 , Ivelina Zaharieva 4, 5, 6, 7 , Konstantin Laun 2, 4, 9, 10, 11 , Ingo Zebger 2, 4, 9, 10, 11 , Holger Dau 4, 5, 6, 7 , Prashanth W. Menezes 1, 2, 3, 4 , Matthias Driess 1, 2, 3, 4
Affiliation  

An unprecedented molecular 2Fe–2As precursor complex was synthesized and transformed under soft reaction conditions to produce an active and long-term stable nanocrystalline FeAs material for electrocatalytic water oxidation in alkaline media. The 2Fe2As-centred β-diketiminato complex, having an unusual planar Fe2As2 core structure, results from the salt-metathesis reaction of the corresponding β-diketiminato FeIICl complex and the AsCO (arsaethynolate) anion as the monoanionic As source. The as-prepared FeAs phase produced from the precursor has been electrophoretically deposited on conductive electrode substrates and shown to act as a electro(pre)catalyst for the oxygen evolution reaction (OER). The deposited FeAs undergoes corrosion under the severe anodic alkaline conditions which causes extensive dissolution of As into the electrolyte forming finally an active two-line ferrihydrite phase (Fe2O3(H2O)x). Importantly, the dissolved As in the electrolyte can be fully recaptured (electro-deposited) at the counter electrode making the complete process eco-conscious. The results represent a new and facile entry to unexplored nanostructured transition-metal arsenides and their utilization for high-performance OER electrocatalysis, which are also known to be magnificent high-temperature superconductors.

中文翻译:

用于高效电催化水氧化的纳米结构FeAs合成的软分子2Fe–2As前体方法

合成了前所未有的分子2Fe–2As前驱体复合物,并在软反应条件下对其进行了转化,以生产出能够在碱性介质中电催化水氧化的活性且长期稳定的纳米晶FeAs材料。所述2Fe2As为中心的β-二酮亚胺基配合物,具有不寻常的平面的Fe 2作为2核心结构,由相应的β-二酮亚胺基Fe的盐复分解反应的结果II C1复合物和ASCO -(arsaethynolate)阴离子作为单阴离子如-资源。由前体制备的FeAs相已通过电泳沉积在导电电极基材上,并显示出可作为氧释放反应(OER)的电催化剂。沉积的FeAs在严重的阳极碱性条件下会受到腐蚀,这会导致As大量溶解到电解质中,最终形成活性的两线铁水合物相(Fe 2 O 3(H 2 O)x)。重要的是,电解质中溶解的As可以在对电极处完全重新捕获(电沉积),从而使整个过程具有环保意识。结果代表了一种新的和容易的进入未探索的纳米结构的过渡金属砷化物及其在高性能OER电催化中的应用的方法,而OER电催化也被称为宏伟的高温超导体。
更新日期:2020-10-13
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