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首页> 外文期刊>Journal of Materials Chemistry, A. Materials for energy and sustainability >Selective electrochemical CO2 reduction to CO using in situ reduced In2O3 nanocatalysts
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Selective electrochemical CO2 reduction to CO using in situ reduced In2O3 nanocatalysts

机译：选择性电化学二氧化碳还原到CO使用原位降低IN2O3纳米催化剂

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Both metallic indium and indium oxide electrocatalysts typically have high selectivity for producing formate via the electrochemical reduction of CO2 in aqueous media. It has been suggested that under highly negative potentials, i.e. potentials typically sufficient to reduce indium oxide to In-0, the native oxide layer on metallic indium or indium oxide particles is not reduced to In-0 when exposed to CO2-saturated electrolytes. This meta-stable oxide layer is crucial in the mechanism for producing formate via the two-electron, two-proton reduction of CO2; however it prevents the catalysis from occurring on In-0. Herein, we report that electrochemically reducing In2O3 nanocatalysts in Ar-saturated electrolytes in situ, prior to CO2 exposure, will remove this metastable oxide layer and create an In-0-In2O3 composite. This In-0-In2O3 composite material changes the selectivity and is able to electrochemically reduce CO2 to CO with near 100% selectivity at relatively low overpotentials (c.a. -1.0 V vs. Ag/AgCl). We attribute the change in selectivity to the direct exposure of In-0 to CO2 in solution that typically does not exist due to the native oxide layer that forms on In metal. In addition, we observed that the first electron-transfer step to form the surface adsorbed intermediates is highly reversible on the In-0-In2O3 composite; however it is irreversible on an In foil electrode. We also report the utilization of Substrate Generation-Tip Collection Scanning Electrochemical Microscopy (SG-TC SECM) to measure the production of CO as a function of applied potential. This technique allows for the collection of CO in situ during the voltammetry experiment as it is produced on the catalytic electrode, which results in accurate potential dependent measurements of CO production.
机译：金属铟和氧化铟电催化剂均通常具有高选择性，用于通过水性介质中的CO 2的电化学还原生产甲酸盐。已经提出，在高负电位下，即通常足以将氧化物铟的潜在电位在-O中，当暴露于CO 2饱和电解质时，金属铟或氧化铟颗粒上的天然氧化物层不会减少到-0。该稳定的氧化物层在通过双电子的制备甲酸盐的机制中至关重要，二氧化碳的两种质子减少;然而，它可以防止催化发生在-0上。在此，我们报告说，在CO2暴露之前，原位地在Ar饱和电解质中电化学减少了In2O3纳米催化剂，将去除该亚稳氧化物层并在0-In2O3复合材料中产生。该0-In2O3复合材料中的选择性改变了选择性，并且能够在相对低的过电（C.A. -1.0V与Ag / AgCl）中以接近100％的选择性电化学减少CO 2至CO。我们将选择性的变化归因于在-0 in-0到CO 2的直接暴露于溶液中，该溶液中通常不存在由于在金属中形成的天然氧化物层。此外，我们观察到形成表面吸附的中间体的第一电子转移步骤在0-In2O3复合材料上高度可逆;然而，它在箔电极上是不可逆转的。我们还报告了基板生成尖端采集扫描电化学显微镜（SG-TC SEC）的利用率测量CO的生产作为应用势的函数。该技术允许在伏安法实验期间收集CO原位，因为它在催化电极上产生，这导致CO生产的精确潜在的测量。

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