Covalent Organic Framework Nanosheets Embedding Single Cobalt Sites for Photocatalytic Reduction of Carbon Dioxide,Chemistry of Materials

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Covalent Organic Framework Nanosheets Embedding Single Cobalt Sites for Photocatalytic Reduction of Carbon Dioxide
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-10-19 , DOI: 10.1021/acs.chemmater.0c01642
Xiaoyan Wang ₁ , Zhiwei Fu ₁ , Lirong Zheng ₂ , Chengxi Zhao _{1,

3} , Xue Wang _{1,

4} , Samantha Y. Chong ₁ , Fiona McBride ₅ , Rasmita Raval ₅ , Matthew Bilton ₆ , Lunjie Liu ₁ , Xiaofeng Wu ₁ , Linjiang Chen _{1,

4} , Reiner Sebastian Sprick _{1,

7} , Andrew I. Cooper _{1,

4}

Affiliation

Covalent organic framework nanosheets (CONs), fabricated from two-dimensional covalent organic frameworks (COFs), present a promising strategy for incorporating atomically distributed catalytic metal centers into well-defined pore structures with desirable chemical environments. Here, a series of CONs was synthesized by embedding single cobalt sites that were then evaluated for photocatalytic carbon dioxide reduction. A partially fluorinated, cobalt-loaded CON produced 10.1 μmol carbon monoxide with a selectivity of 76%, over 6 hours irradiation under visible light (TON = 28.1), and a high external quantum efficiency (EQE) of 6.6% under 420 nm irradiation in the presence of an iridium dye. The CONs appear to act as a semiconducting support, facilitating charge carrier transfer between the dye and the cobalt centers, and this results in a performance comparable with that of the state-of-the-art heterogeneous catalysts in the literature under similar conditions. The ultrathin CONs outperformed their bulk counterparts in all cases, suggesting a general strategy to enhance the photocatalytic activities of COF materials.

中文翻译：

嵌入单个钴位点的共价有机骨架纳米片，用于二氧化碳的光催化还原

由二维共价有机骨架（COF）制成的共价有机骨架纳米片（CONs），提出了一种有前途的策略，可将原子分布的催化金属中心并入具有理想化学环境的明确孔结构中。在这里，通过嵌入单个钴位点合成了一系列的CON，然后评估了其对光催化二氧化碳的还原作用。部分氟化，负载钴的CON在可见光（TON = 28.1）下经过6个小时的辐射在6小时内产生了10.1μmol一氧化碳，选择性为76％，而在420 nm辐射下，其外部量子效率（EQE）为6.6％。铱染料的存在。CON似乎起着半导体载体的作用，促进了染料和钴中心之间的载流子转移，在类似条件下，其性能可与文献中最先进的多相催化剂相媲美。在所有情况下，超薄CON的性能均优于其同类产品，这表明增强COF材料光催化活性的一般策略。

更新日期：2020-11-12

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