A Stable and Conductive Metallophthalocyanine Framework for Electrocatalytic Carbon Dioxide Reduction in Water. (13th July 2020)

• Record Type: Journal Article
• Authors: Huang, Ning; Lee, Ka Hung; Yue, Yan; Xu, Xiaoyi; Irle, Stefan; Jiang, Qiuhong; Jiang, Donglin
• Is Part Of: Angewandte Chemie. Volume 132:Number 38(2020)
• Page Start: 16730
• Page End: 16736
• Publication Date: 2020-07-13
• Subjects: 2D polymers -- CO2 reduction -- covalent organic frameworks -- electrocatalysis -- π conjugation; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202005274
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: Transformation of carbon dioxide to high value‐added chemicals becomes a significant challenge for clean energy studies. Here a stable and conductive covalent organic framework was developed for electrocatalytic carbon dioxide reduction to carbon monoxide in aqueous solution. The cobalt(II) phthalocyanine catalysts are topologically connected via robust phenazine linkage into a two‐dimensional tetragonal framework that is stable under boiling water, acid, or base conditions. The 2D lattice enables full π conjugation along x and y directions as well as π conduction along the z axis across the π columns. With these structural features, the electrocatalytic framework exhibits a faradaic efficiency of 96 %, an exceptional turnover number up to 320 000, and a long‐term turnover frequency of 11 412 hour −1, which is a 32‐fold improvement over molecular catalyst. The combination of catalytic activity, selectivity, efficiency, and durability is desirable for clean energy production. Abstract : Pumping electrons to produce fuel : A fully π‐conjugated 2D covalent organic framework with aligned metallophthalocyanine electrocatalytic sites enables electron pumping to CO2 reduction centers. The 2D π lattice catalyzes two‐electron reduction of CO2 to CO in water to achieve an exceptional turnover number up to 320 000 hour −1 and a faraday efficiency of 96 %.