使用原位光谱在 Cu2O 纳米结构上原位生成表面/界面以增强电催化 CO2 还原为乙烯,Inorganic Chemistry Frontiers

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使用原位光谱在 Cu2O 纳米结构上原位生成表面/界面以增强电催化 CO2 还原为乙烯
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2022-11-11 , DOI: 10.1039/d2qi01977a
Fangfang Chang ₁ , Yongpeng Liu ₁ , Juncai Wei ₁ , Lin Yang ₁ , Zhengyu Bai ₁

Affiliation

电催化 CO ₂还原反应 (CO ₂ RRs) 是一种将二氧化碳转化为有价值的燃料和化学品的有效方法，具有吸引力和挑战性。在这项工作中，具有活性晶面的 Cu ₂ O 纳米结构（具有 (100) 晶面的凸起立方结构 (F-Cu ₂ O)、具有 (111) 晶面和边缘的八面体结构 (O-Cu ₂ O) 和具有 (100) 和 (111) 面的截角八面体结构 (T-Cu ₂ O) 通过湿化学还原法合成。原位重建Cu ₂ O 纳米结构的表面以形成 Cu ₂_{O/Cu在CO 2}转化为C ₂ H ₄过程中具有高活性界面，分别命名为F-Cu ₂ O/Cu、O-Cu ₂ O/Cu和T-Cu ₂ O/Cu。C ₂ H ₄在 Cu ₂ O/Cu 催化剂上的选择性遵循 O-Cu ₂ O/Cu < F-Cu ₂ O/Cu < T-Cu _{2 O/Cu 的顺序，以及 C}₂ H ₄的法拉第效率与可逆氢电极相比，-1.1 V 时分别为 11.2%、24.9% 和 58.0% 。实验结果结合操作数表面增强拉曼光谱显示 Cu ₂ O/Cu 界面增强了 *CO 吸附并降低了 C-C 偶联的活化能，这也得到了密度泛函理论 (DFT) 计算的支持。本研究将为通过晶面工程和界面工程进行电化学储能和转换铺平一条可行的途径。

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In situ surface/interface generation on Cu2O nanostructures toward enhanced electrocatalytic CO2 reduction to ethylene using operando spectroscopy

Electrocatalytic CO₂ reduction reactions (CO₂RRs), an efficient method of converting carbon dioxide into valuable fuels and chemicals, are attractive as well as challenging. In this work, Cu₂O nanostructures with active facets (face-raised cubic structures (F-Cu₂O) with the (100) facet, octahedral structures (O-Cu₂O) with the (111) facet and edge- and corner-truncated octahedral structures (T-Cu₂O) with both the (100) and (111) facets) were synthesized by a wet chemical reduction method. The surface of Cu₂O nanostructures was reconstructed in situ to form Cu₂O/Cu with a highly active interface during the conversion of CO₂ into C₂H₄, which is named F-Cu₂O/Cu, O-Cu₂O/Cu and T-Cu₂O/Cu. The C₂H₄ selectivity on Cu₂O/Cu catalysts follows the order of O-Cu₂O/Cu < F-Cu₂O/Cu < T-Cu₂O/Cu, and the faradaic efficiencies of C₂H₄ are 11.2%, 24.9%, and 58.0% at −1.1 V versus the reversible hydrogen electrode, respectively. The experimental results combined with operando surface-enhanced Raman spectroscopy reveal that the Cu₂O/Cu interface enhances *CO adsorption and decreases the activation energy of C–C coupling, which is also supported by density functional theory (DFT) calculations. This study will pave a feasible pathway for electrochemical energy storage and convention by crystal facet engineering and interface engineering.

更新日期：2022-11-11

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