电合成 CuMgAl 层状双氢氧化物作为 CO2 电化学还原的新型催化剂,Advanced Functional Materials

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电合成 CuMgAl 层状双氢氧化物作为 CO2 电化学还原的新型催化剂
Advanced Functional Materials ( IF 19.0 ) Pub Date : 2023-04-06 , DOI: 10.1002/adfm.202300345
Martina Serafini ₁ , Federica Mariani ₁ , Andrea Fasolini ₁ , Eleonora Tosi Brandi ₁ , Erika Scavetta ₁ , Francesco Basile ₁ , Domenica Tonelli ₁

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^{在这项研究中，新型纳米结构CuMgAl层状双氢氧化物（LDH）基材料在4 cm 2}尺寸的碳质气体扩散膜上合成。通过显微镜和光谱技术，对催化剂进行了彻底研究，揭示了同一材料中存在多种物质。通过一步、可重复的动电位沉积，可以获得一种在三元CuMgAl LDH和Cu ⁰ /Cu ₂ O物质之间紧密接触的复合材料。通过改变以下因素来研究催化剂组成：二价阳离子总量与 Al ^{3+之间的摩尔比}、负载量以及电解质中三种阳离子之间的摩尔比。每种电催化剂均根据液相中可逆氢电极在-0.4V下电化学CO ₂还原成CH _{3 COOH的催化性能进行了评估。}优化后的催化剂CuMgAl 2:1:1 LDH的产率为2.0 mmol _CH3COOH g _cat^-1 h ^-1。该结果显示了将像LDHs这样的材料与Cu ⁰ /Cu ⁺相结合的有益效果，LDHs本质上是碱性的，因此对CO _{2具有很大的亲和力。}物种，其将电极处碳源可用性的增加与能够将CO ₂转化为C ₂产品的氧化还原介体结合起来。

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Electrosynthesized CuMgAl Layered Double Hydroxides as New Catalysts for the Electrochemical Reduction of CO2

In this study, new nanostructured CuMgAl Layered Double Hydroxide (LDH) based materials are synthesized on a 4 cm² sized carbonaceous gas diffusion membrane. By means of microscopic and spectroscopic techniques, the catalysts are thoroughly investigated, revealing the presence of several species within the same material. By a one-step, reproducible potentiodynamic deposition it is possible to obtain a composite with an intimate contact between a ternary CuMgAl LDH and Cu⁰/Cu₂O species. The catalyst compositions are investigated by varying: the molar ratio between the total amount of bivalent cations and Al³⁺, the amount of loading, and the molar ratios among the three cations in the electrolyte. Each electrocatalyst has been evaluated based on the catalytic performances toward the electrochemical CO₂ reduction to CH₃COOH at −0.4 V versus reversible hydrogen electrode in liquid phase. The optimized catalyst, that is, CuMgAl 2:1:1 LDH exhibits a productivity of 2.0 mmol_CH3COOH g_cat⁻¹ h⁻¹. This result shows the beneficial effects of combining a material like the LDHs, alkaline in nature, and thus with a great affinity to CO₂, with Cu⁰/Cu⁺ species, which couples the increase of carbon sources availability at the electrode with a redox mediator capable to convert CO₂ into a C₂ product.

更新日期：2023-04-06

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