Cu?C(O) 界面在 500 mA cm−2 的工业电流密度下为 CO2 还原为 C2+ 产品提供卓越的选择性和稳定性,Small

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Cu?C(O) 界面在 500 mA cm−2 的工业电流密度下为 CO2 还原为 C2+ 产品提供卓越的选择性和稳定性
Small ( IF 13.0 ) Pub Date : 2023-03-28 , DOI: 10.1002/smll.202301289
Ruian Du ₁ , Qiqi Wu ₁ , Shiyi Zhang ₁ , Peng Wang ₁ , Zhengjian Li ₁ , Yongcai Qiu ₁ , Keyou Yan ₁ , Geoffrey I N Waterhouse ₂ , Pei Wang ₃ , Jia Li ₄ , Yun Zhao ₁ , Wei-Wei Zhao ₅ , Xue Wang ₆ , Guangxu Chen ₁

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电催化CO ₂还原反应(CO ₂ RR)对于CO ₂增值和高密度电能存储来说是一项有吸引力的技术。在高电流密度（>500 mA cm ^{-2 ）的CO}_{2 RR过程中实现对C}₂₊产物（尤其是乙烯）的高选择性是当前研究的一个重要目标，尽管在技术上仍然非常具有挑战性。_{在此，证明了可以调节Cu催化剂的表面和界面结构以及CO 2}还原流通池中气体扩散电极（GDE）上的固-气-液界面，以允许有效的CO 2 RR_到C ₂₊产品。该方法使用 CuO 纳米片/氧化石墨烯点 (CuO → C(O)) 混合物的原位电化学还原。由于CuO-C(O)杂化物中丰富的Cu-O-C界面，CuO纳米片在拓扑上选择性地转化为暴露出Cu(100)面、Cu(110)面、Cu[n(100)面的金属Cu纳米片。 × (110)] 台阶位点和电还原步骤期间的Cu ⁺ /Cu ^0界面，对 C ₂₊烃类的法拉第效率 (FE)在 500 mA cm 时达到高达 77.4%（FE_乙烯 ≈ 60%）⁻²。原位红外光谱和DFT模拟表明，还原的CuO - C(O)催化剂中丰富的Cu ⁺物种和Cu ⁰ /Cu ^{+界面提高了*CO在Cu催化剂上的吸附和表面覆盖，从而促进C}- C偶联反应。

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Cu?C(O) Interfaces Deliver Remarkable Selectivity and Stability for CO2 Reduction to C2+ Products at Industrial Current Density of 500 mA cm−2

The electrocatalytic CO₂ reduction reaction (CO₂RR) is an attractive technology for CO₂ valorization and high-density electrical energy storage. Achieving a high selectivity to C₂₊ products, especially ethylene, during CO₂RR at high current densities (>500 mA cm⁻²) is a prized goal of current research, though remains technically very challenging. Herein, it is demonstrated that the surface and interfacial structures of Cu catalysts, and the solid–gas–liquid interfaces on gas-diffusion electrode (GDE) in CO₂ reduction flow cells can be modulated to allow efficient CO₂RR to C₂₊ products. This approach uses the in situ electrochemical reduction of a CuO nanosheet/graphene oxide dots (CuOC(O)) hybrid. Owing to abundant CuOC interfaces in the CuOC(O) hybrid, the CuO nanosheets are topologically and selectively transformed into metallic Cu nanosheets exposing Cu(100) facets, Cu(110) facets, Cu[n(100) × (110)] step sites, and Cu⁺/Cu⁰ interfaces during the electroreduction step, the faradaic efficiencie (FE) to C₂₊ hydrocarbons was reached as high as 77.4% (FE_ethylene ≈ 60%) at 500 mA cm⁻² . In situ infrared spectroscopy and DFT simulations demonstrate that abundant Cu⁺ species and Cu⁰/Cu⁺ interfaces in the reduced CuOC(O) catalyst improve the adsorption and surface coverage of *CO on the Cu catalyst, thus facilitating CC coupling reactions.

更新日期：2023-03-28

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