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首页> 外文期刊>Advanced Materials >Evolving Highly Active Oxidic Iron(Ⅲ) Phase from Corrosion of Intermetallic Iron Silicide to Master Efficient Electrocatalytic Water Oxidation and Selective Oxygenation of 5-Hydroxymethylfurfural
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Evolving Highly Active Oxidic Iron(Ⅲ) Phase from Corrosion of Intermetallic Iron Silicide to Master Efficient Electrocatalytic Water Oxidation and Selective Oxygenation of 5-Hydroxymethylfurfural

机译：从金属间铁硅化物的腐蚀中发展高活性氧化铁（Ⅲ）相对母催化水氧化和5-羟甲基甲基糠醛的选择性氧合

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摘要

In a green energy economy, electrocatalysis is essential for chemical energy conversion and to produce value added chemicals from regenerative resources. To be widely applicable, an electrocatalyst should comprise the Earth's crust's most abundant elements. The most abundant 3d metal, iron, with its multiple accessible redox states has been manifold applied in chemocatalytic processes. However, due to the low conductivity of (FeOxHy)-O-III phases, its applicability for targeted electrocatalytic oxidation reactions such as water oxidation is still limited. Herein, it is shown that iron incorporated in conductive intermetallic iron silicide (FeSi) can be employed to meet this challenge. In contrast to silicon-poor iron-silicon alloys, intermetallic FeSi possesses an ordered structure with a peculiar bonding situation including covalent and ionic contributions together with conducting electrons. Using in situ X-ray absorption and Raman spectroscopy, it could be demonstrated that, under the applied corrosive alkaline conditions, the FeSi partly forms a unique, oxidic iron(III) phase consisting of edge and corner sharing [FeO6] octahedra together with oxidized silicon species. This phase is capable of driving the oxyge evolution reaction (OER) at high efficiency under ambient and industrially relevant conditions (500 mA cm(-2) at 1.50 +/- 0.025 V-RHE and 65 degrees C) and to selectively oxygenate 5-hydroxymethylfurfural (HMF).
机译：在绿色能源经济中，电催化对于化学能转换至关重要，并从再生资源产生增值化学品。为了广泛适用，电催化剂应包括地壳最丰富的元素。最丰富的3D金属，铁，具有其多种可接近的氧化还原状态已经存在于化学催略过程中的歧管。然而，由于（Feoxhy）-O-III阶段的低导电性，其对靶向电催化氧化反应如水氧化的适用性仍然有限。在此，可以采用在导电金属间铁（FESI）中的铁掺入导电金属间铁硅化物（FESI）中以满足该挑战。与硅贫硅合金相比，金属间Fesi具有有序结构，其特殊的粘合情况包括共价和离子贡献以及导电电子。使用原位X射线吸收和拉曼光谱，可以证明，在施加的腐蚀性碱性条件下，FESI部分形成独特的氧化铁（III）相，包括边缘和角落分享[Feo6]八面体与氧化一起组成硅种类。该阶段能够在环境和工业相关的条件下高效地驱动氧态演化反应（OER）（500 mA cm（-2），在1.50 +/- 0.025V-rhe和65℃）下并选择性含氧化5-羟甲基糠醛（HMF）。

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