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.
| Original language | English |
|---|---|
| Pages (from-to) | 16587-16593 |
| Number of pages | 7 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 59 |
| Issue number | 38 |
| DOIs | |
| State | Published - Sep 14 2020 |
Funding
N.H. acknowledges support by the research start‐up fund of Zhejiang University. K.H.L. was supported by an Energy Science and Engineering Fellowship by the Bredesen Centre for Interdisciplinary Research and Graduate Education at the University of Tennessee, Knoxville. S.I. acknowledges support by the Laboratory Directed Research and Development (LDRD) Program of Oak Ridge National Laboratory. ORNL is managed by UT‐Battelle, LLC, for DOE under contract DE‐AC05‐00OR22725. D.J. acknowledges supports by MOE tier 1 grant (R‐143‐000‐A71‐114) and NUS start‐up grant (R‐143‐000‐A28‐133).
Keywords
- 2D polymers
- CO reduction
- covalent organic frameworks
- electrocatalysis
- π conjugation
