Efficient Electrocatalytic Conversion of CO2 to Ethanol Enabled by Imidazolium-Functionalized Ionomer Confined Molybdenum Phosphide
Efficient Electrocatalytic Conversion of CO2 to Ethanol Enabled by Imidazolium-Functionalized Ionomer Confined Molybdenum Phosphide
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DOI：
10.1016/j.apcatb.2022.121681
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发表时间：
2022-06
期刊：
影响因子：
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通讯作者：
Mohammadreza Esmaeilirad;A. Kondori;Nannan Shan;Mahmoud Tamadoni Saray;Sreya Sarkar;A. M. Harzandi;
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文献类型：
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作者：
Mohammadreza Esmaeilirad;A. Kondori;Nannan Shan;Mahmoud Tamadoni Saray;Sreya Sarkar;A. M. Harzandi;
有效的电化学二氧化碳还原反应（eCO 2 RR）需要发现对多碳产物具有高活性和选择性的催化体系，以及在催化剂层处的上级CO2扩散以使还原障碍最小化。在这里，我们发现了一种催化体系，该体系使用磷化钼（MoP）纳米颗粒覆盖的咪唑功能化的离聚物（Im），促进CO2扩散在催化剂层朝向催化剂表面，其中CO2被还原为乙醇（C2 H5 OH）。使用MoP-Im助催化剂的电化学结果显示，在低至− 200 mVvs. RHE的电势下，C2 H5 OH的法拉第效率和阴极能量效率分别为77.4%和63.3%。电化学实验沿着物理化学表征表明，Im改善了催化剂层中CO2的扩散，平衡了催化剂层中的水含量，提高了催化剂层中的CO2/水比，并微调了MoP表面Mo原子的电子性质。原位拉曼光谱表明，在MoP表面吸附了大量的 *CO中间体，并提高了 * CO的结合强度。在咪唑分子存在下，Mo表面位点上的CO中间体是上级C-C偶联的主要原因，从而改善了C2 H5 OH的形成。
An effective electrochemical carbon dioxide reduction reaction (eCO2RR) requires the discovery of a catalytic system that is highly active and selective for multi-carbon products together with superior CO2diffusion at a catalyst layer to minimize the reduction barriers. Here, we found a catalytic system that uses molybdenum phosphide (MoP) nanoparticles covered by imidazolium-functionalized ionomer (Im) that promotes CO2diffusion at the catalyst layer toward the catalyst surface, where CO2is reduced to ethanol (C2H5OH). The electrochemical results with the MoP-Im co-catalyst show a C2H5OH production Faradaic efficiency and a cathodic energy efficiency of 77.4% and 63.3%, respectively, at a potential as low as − 200 mVvs.RHE. The electrochemical experiments along with our physicochemical characterizations indicate that the Im improves CO2diffusion and balances water content resulting in a higher CO2-to-water ratio at the catalyst layer and fine-tunes the electronic properties of Mo atoms at the MoP surface.In-situRaman spectroscopy reveals that a high number of adsorbed *CO intermediates on the surface and a higher binding strength of *CO intermediates on the Mo surface sites in the presence of imidazolium molecules are the main reasons for a superior C-C coupling and thereby the improved C2H5OH formation.