Conductive Phthalocyanine‐Based Covalent Organic Framework for Highly Efficient Electroreduction of Carbon Dioxide,Small

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Conductive Phthalocyanine‐Based Covalent Organic Framework for Highly Efficient Electroreduction of Carbon Dioxide
Small ( IF 13.0 ) Pub Date : 2020-12-01 , DOI: 10.1002/smll.202005254
Meng‐Di Zhang _{1,

2,

3} , Duan‐Hui Si _{1,

3} , Jun‐Dong Yi _{1,

4} , Shao‐Shuai Zhao _{1,

3} , Yuan‐Biao Huang _{1,

3,

4} , Rong Cao _{1,

3,

4}

Affiliation

The electroreduction of CO₂ to value‐added chemicals such as CO is a promising approach to realize carbon‐neutral energy cycle, but still remains big challenge including low current density. Covalent organic frameworks (COFs) with abundant accessible active single‐sites can offer a bridge between homogeneous and heterogeneous electrocatalysis, but the low electrical conductivity limits their application for CO₂ electroreduction reaction (CO₂RR). Here, a 2D conductive Ni‐phthalocyanine‐based COF, named NiPc‐COF, is synthesized by condensation of 2,3,9,10,16,17,23,24‐octa‐aminophthalocyaninato Ni(II) and tert‐butylpyrene‐tetraone for highly efficient CO₂RR. Due to its highly intrinsic conductivity and accessible active sites, the robust conductive 2D NiPc‐COF nanosheets exhibit very high CO selectivity (>93%) in a wide range of the applied potentials of −0.6 to −1.1 V versus the reversible hydrogen electrode (RHE) and large partial current density of 35 mA cm⁻² at −1.1 V versus RHE in aqueous solution that surpasses all the conventional COF electrocatalysts. The robust NiPc‐COF that is bridged by covalent pyrazine linkage can maintain its CO₂RR activity for 10 h. This work presents the implementation of the conductive COF nanosheets for CO₂RR and provides a strategy to enhance energy conversion efficiency in electrocatalysis.

中文翻译：

导电酞菁基共价有机骨架，可实现二氧化碳的高效电还原

将CO ₂电还原为增值化学品（例如CO）是实现碳中性能量循环的一种有前途的方法，但仍然存在很大的挑战，包括低电流密度。具有丰富可及活性单点的共价有机骨架（COF）可以在均相和异相电催化之间架起一座桥梁，但低电导率限制了它们在CO ₂电还原反应（CO ₂ RR）中的应用。在此，通过将2,3,9,10,16,17,23,24-八氨基氨基酞菁缩合为Ni（II）和叔丁基py的2D导电Ni-酞菁基COF合成为NiPc-COF。高效CO _2的四酮RR。由于其固有的高电导率和可访问的活性位点，因此坚固的2D NiPc-COF导电纳米片相对于可逆的氢电极（-0.6至-1.1 V）在很大的施加电势范围（-0.6至-1.1 V）下均具有很高的CO选择性（> 93％）。相对于水溶液中的RHE，RHE）和在-1.1 V时的35 mA cm ^-2的大分电流密度超过了所有常规COF电催化剂。通过共价吡嗪键桥接的坚固的NiPc-COF可以保持其CO ₂ RR活性达10小时。这项工作提出了用于CO ₂ RR的导电COF纳米片的实现，并提供了一种在电催化中提高能量转换效率的策略。

更新日期：2020-12-28

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