Single-Layered Imine-Linked Porphyrin-Based Two-Dimensional Covalent Organic Frameworks Targeting CO2 Reduction,Advanced Energy Materials

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Single-Layered Imine-Linked Porphyrin-Based Two-Dimensional Covalent Organic Frameworks Targeting CO2 Reduction
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2024-02-28 , DOI: 10.1002/aenm.202304371
Nicolás Arisnabarreta ₁ , Yansong Hao _{2,

3} , Enquan Jin _{4,

5} , Aude Salamé ₆ , Klaus Muellen ₄ , Marc Robert _{6,

7} , Roberto Lazzaroni ₃ , Sandra Van Aert ₂ , Kunal S. Mali ₁ , Steven De Feyter ₁

Affiliation

The reduction of carbon dioxide (CO₂) using porphyrin-containing 2D covalent organic frameworks (2D-COFs) catalysts is widely explored nowadays. While these framework materials are normally fabricated as powders followed by their uncontrolled surface heterogenization or directly grown as thin films (thickness >200 nm), very little is known about the performance of substrate-supported single-layered (≈0.5 nm thickness) 2D-COFs films (s2D-COFs) due to its highly challenging synthesis and characterization protocols. In this work, a fast and straightforward fabrication method of porphyrin-containing s2D-COFs is demonstrated, which allows their extensive high-resolution visualization via scanning tunneling microscopy (STM) in liquid conditions with the support of STM simulations. The as-prepared single-layered film is then employed as a cathode for the electrochemical reduction of CO₂. Fe porphyrin-containing s2D-COF@graphite used as a single-layered heterogeneous catalyst provided moderate-to-high carbon monoxide selectivity (82%) and partial CO current density (5.1 mA cm⁻²). This work establishes the value of using single-layered films as heterogene ous catalysts and demonstrates the possibility of achieving high performance in CO₂ reduction even with extremely low catalyst loadings.

中文翻译：

基于单层亚胺连接的卟啉的二维共价有机框架靶向二氧化碳减排

如今，使用含卟啉的2D共价有机骨架(2D-COF)催化剂还原二氧化碳(CO ₂ )被广泛探索。虽然这些框架材料通常被制造为粉末，然后进行不受控制的表面异质化或直接生长为薄膜（厚度> 200 nm），但人们对基底支撑的单层（约0.5 nm厚度）2D-的性能知之甚少。 COF 薄膜 (s2D-COF) 因其极具挑战性的合成和表征协议而闻名。在这项工作中，展示了一种快速、简单的含卟啉 s2D-COF 的制造方法，该方法允许在液体条件下在 STM 模拟的支持下通过扫描隧道显微镜 (STM) 对其进行广泛的高分辨率可视化。然后将所制备的单层膜用作CO ₂电化学还原的阴极。含铁卟啉的s2D-COF@石墨用作单层多相催化剂，提供中等到高的一氧化碳选择性（82%）和部分CO电流密度（5.1 mA cm ^-2）。这项工作确立了使用单层膜作为多相催化剂的价值，并证明了即使在极低的催化剂负载量下也能实现高性能 CO _{2还原的可能性。}

更新日期：2024-02-28

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