双功能气体扩散电极可将稀流中的 CO2 原位分离并转化为乙烯,Advanced Materials

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双功能气体扩散电极可将稀流中的 CO2 原位分离并转化为乙烯
Advanced Materials ( IF 27.4 ) Pub Date : 2023-03-21 , DOI: 10.1002/adma.202300389
Shariful Kibria Nabil ₁ , Soumyabrata Roy ₂ , Wala Ali Algozeeb ₃ , Tareq Al-Attas ₁ , Md Abdullah Al Bari ₁ , Ali Shayesteh Zeraati ₁ , Karthick Kannimuthu ₁ , Pedro Guerra Demingos ₄ , Adwitiya Rao ₄ , Thien N Tran ₅ , Xiaowei Wu ₆ , Praveen Bollini ₆ , Haiqing Lin ₅ , Chandra Veer Singh ₄ , James M Tour ₃ , Pulickel M Ajayan ₂ , Md Golam Kibria ₁

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对浓缩二氧化碳 (CO _{2 ) 原料的需求显着限制了电化学 CO}₂还原 (eCO ₂ R)的经济可行性，这通常涉及多个中间过程，包括 CO ₂捕获、能源密集型再生、压缩和运输。在此，报道了用于从低浓度 CO _{2流中分离和 eCO}₂ R的双功能气体扩散电极 (BGDE) 。BGDE 用于选择性生产乙烯 (C ₂ H ₄) 通过将高密度聚乙烯衍生多孔碳 (HPC) 作为物理吸附剂与多晶铜作为转化催化剂相结合。BGDE 显示出对 10 vol% CO _{2的显着耐受性，在 80 mA cm}^-2的电流密度下表现出对 C ₂ H ₄ ≈45% 的法拉第效率，优于之前使用此类分压的报告（P _CO2 = 0.1 atm 和以上）和未改变的多晶铜。_{分子动力学模拟和混合气体渗透率评估表明，高CO 2}确保了这种选择性性能由于吸附剂边界内CO ₂和氮气 (CO ₂ |N ₂ )的二元流产生的分子扩散和浓度梯度，微孔 HPC 的吸收以及连续解吸。基于详细的技术经济分析，得出的结论是，通过排除与传统解耦过程的能源密集型中间步骤相关的C ₂ H ₄生产成本，这种原位过程在经济上具有吸引力。

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Bifunctional Gas Diffusion Electrode Enables In Situ Separation and Conversion of CO2 to Ethylene from Dilute Stream

The requirement of concentrated carbon dioxide (CO₂) feedstock significantly limits the economic feasibility of electrochemical CO₂ reduction (eCO₂R) which often involves multiple intermediate processes, including CO₂ capture, energy-intensive regeneration, compression, and transportation. Herein, a bifunctional gas diffusion electrode (BGDE) for separation and eCO₂R from a low-concentration CO₂ stream is reported. The BGDE is demonstrated for the selective production of ethylene (C₂H₄) by combining high-density-polyethylene-derived porous carbon (HPC) as a physisorbent with polycrystalline copper as a conversion catalyst. The BGDE shows substantial tolerance to 10 vol% CO₂ exhibiting a Faradaic efficiency of ≈45% toward C₂H₄ at a current density of 80 mA cm⁻², outperforming previous reports that utilized such partial pressure (P_CO2 = 0.1 atm and above) and unaltered polycrystalline copper. Molecular dynamics simulation and mixed gas permeability assessment reveal that such selective performance is ensured by high CO₂ uptake of the microporous HPC as well as continuous desorption owing to the molecular diffusion and concentration gradient created by the binary flow of CO₂ and nitrogen (CO₂|N₂) within the sorbent boundary. Based on detailed techno-economic analysis, it is concluded that this in situ process can be economically compelling by precluding the C₂H₄ production cost associated with the energy-intensive intermediate steps of the conventional decoupled process.

更新日期：2023-03-21

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