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Network Covalent Solids

Network Covalent Solids

Network covalent solids contain a three-dimensional network of covalently bonded atoms as found in the crystal structures of nonmetals like diamond, graphite, silicon, and some covalent compounds, such as silicon dioxide (sand) and silicon carbide (carborundum, the abrasive on sandpaper). Many minerals have networks of covalent bonds.
To break or to melt a covalent network solid, covalent bonds must be broken. Because covalent bonds are relatively strong, covalent network solids are typically...

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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction

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Published on: April 10, 2018

Atomically Thin, Ionic-Covalent Organic Nanosheets for Stable, High-Performance Carbon Dioxide Electroreduction.

Yun Song¹, Jun-Jie Zhang², Yubing Dou¹

¹Department of Chemistry and State Key Laboratory of Marine Pollution, Hong Kong Institute for Advanced Study, City University of Hong Kong, Hong Kong, 999077, P. R. China.

Advanced Materials (Deerfield Beach, Fla.)

|August 25, 2022

Summary

This summary is machine-generated.

Atomically thin, ionic nanosheets featuring cobalt porphyrins offer enhanced carbon dioxide reduction (CO2 RR) activity and stability. This electrocatalyst design prevents leaching and achieves high CO current densities for efficient CO2 conversion.

Keywords:

carbon dioxide reduction covalent organic frameworks ionic nanosheets positive charge ultrathin materials

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Area of Science:

Materials Science
Electrochemistry
Catalysis

Background:

Charged functional groups can improve molecular complex activity for CO2 reduction.
Catalyst leaching is a major challenge for long-term heterogeneous electrolysis.

Purpose of the Study:

To synthesize and characterize an electrocatalyst for high-performance CO2 to CO conversion.
To investigate the role of ionic-covalent organic nanosheets in enhancing CO2 reduction reaction (CO2 RR) activity and stability.

Main Methods:

Post-synthetic modification strategy to create atomically thin, cobalt-porphyrin-based, ionic-covalent organic nanosheets (CoTAP-iCONs).
Theoretical calculations to understand the mechanism of CO2 RR.
Electrochemical testing in a flow cell, including solar cell coupling.

Main Results:

CoTAP-iCONs demonstrated significantly higher CO current densities (870% and 480% improvement) compared to monomer and neutral nanosheets.
Achieved a low onset overpotential of 40 mV and a stable current density of 212 mA cm-2 with >95% CO Faradaic efficiency for 11 hours.
Solar-to-CO conversion efficiency of 13.89% was obtained by coupling the flow electrolyzer with solar cells.

Conclusions:

Atomically thin, ionic nanosheets are a promising structure for developing highly active and stable electrocatalysts.
The cationic quaternary ammonium groups in CoTAP-iCONs enhance CO2 RR activity and facilitate intermediate formation.
This ionic-covalent organic nanosheet design effectively addresses catalyst leaching issues in heterogeneous electrolysis.