Abstract

Developing efficient methods for capture and controlled release of carbon dioxide is crucial to any carbon capture and utilization technology. Herein we present an approach using an organic semiconductor electrode to electrochemically capture dissolved CO2 in aqueous electrolytes. The process relies on electrochemical reduction of a thin film of a naphthalene bisimide derivative, 2,7-bis(4-(2-(2-ethylhexyl)thiazol-4-yl)phenyl)benzo[lmn][3,8]phenanthroline-1,3,6,8(2H,7H)-tetraone (NBIT). This molecule is specifically tailored to afford one-electron reversible and one-electron quasi-reversible reduction in aqueous conditions while not dissolving or degrading. The reduced NBIT reacts with CO2 to form a stable semicarbonate salt, which can be subsequently oxidized electrochemically to release CO2. The semicarbonate structure is confirmed by in situ IR spectroelectrochemistry. This process of capturing and releasing carbon dioxide can be realized in an oxygen-free environment under ambient pressure and temperature, with uptake efficiency for CO2 capture of ∼2.3 mmol g–1. This is on par with the best solution-phase amine chemical capture technologies available today.

Highlights

  • The effects of anthropogenic carbon dioxide present a challenge to scientists in many fields today

  • Polymeric resins were investigated[2−6] and metal organic frameworks (MOFs)[7] have been optimized with respect to their ability of storing carbon dioxide.[8−10] A remarkable CO2 uptake efficiency of 33.5 mmol g−1 sorbent at 40 atm was achieved using Zn-based MOF.[9]

  • We have recently built on the earlier carbonyl redox work by studying the electrochemical addition of CO2 to an industrial carbonyl pigment quinacridone

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Summary

Introduction

The effects of anthropogenic carbon dioxide present a challenge to scientists in many fields today. Despite having high uptake efficiencies, most of the CO2 storing materials mentioned above only perform at high pressure and/or temperature conditions for capturing and releasing of carbon dioxide. Cycling between 0 and −1 V in 0.1 M Na2SO4 in water under nitrogen atmosphere (N2), NBIT film first yields a broad double-peak with its minor maximum around −0.80 V and its major maximum around −0.85 V (Figure S1).

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