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Integrated CO₂ capture-fixation chemistry via interfacial ionic liquid catalyst in laminar gas/liquid flow.

ABSTRACT: Simultaneous capture of carbon dioxide (CO₂) and its utilization with subsequent work-up would significantly enhance the competitiveness of CO₂-based sustainable chemistry over petroleum-based chemistry. Here we report an interfacial catalytic reaction platform for an integrated autonomous process of simultaneously capturing/fixing CO₂ in gas-liquid laminar flow with subsequently providing a work-up step. The continuous-flow microreactor has built-in silicon nanowires (SiNWs) with immobilized ionic liquid catalysts on tips of cone-shaped nanowire bundles. Because of the superamphiphobic SiNWs, a stable gas-liquid interface maintains between liquid flow of organoamines in upper part and gas flow of CO₂ in bottom part of channel. The intimate and direct contact of the binary reagents leads to enhanced mass transfer and facilitating reactions. The autonomous integrated platform produces and isolates 2-oxazolidinones and quinazolines-2,4(1H,3H)-diones with 81-97% yields under mild conditions. The platform would enable direct CO₂ utilization to produce high-valued specialty chemicals from flue gases without pre-separation and work-up steps.

SUBMITTER: Vishwakarma NK

PROVIDER: S-EPMC5343516 | biostudies-literature | 2017 Mar

REPOSITORIES: biostudies-literature

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Integrated CO2 capture-fixation chemistry via interfacial ionic liquid catalyst in laminar gas/liquid flow.

Vishwakarma Niraj K NK Singh Ajay K AK Hwang Yoon-Ho YH Ko Dong-Hyeon DH Kim Jin-Oh JO Babu A Giridhar AG Kim Dong-Pyo DP

Nature communications 20170306

Simultaneous capture of carbon dioxide (CO2) and its utilization with subsequent work-up would significantly enhance the competitiveness of CO2-based sustainable chemistry over petroleum-based chemistry. Here we report an interfacial catalytic reaction platform for an integrated autonomous process of simultaneously capturing/fixing CO2 in gas-liquid laminar flow with subsequently providing a work-up step. The continuous-flow microreactor has built-in silicon nano ...[more]

PMID: 28262667

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Project description:Electrochemical amperometric sensors require a constant or varying potential at the working electrode that drives redox reactions of the analyte for detection. The interfacial redox reaction(s) can result in the formation of new chemical products that could change the initial condition of the electrode/electrolyte interface. If the products are not inert and/or cannot be removed from the system such that the initial condition of the electrode/electrolyte interface cannot be restored, the sensor signal baseline would consequently drift, which is problematic for the continuous and real-time sensors. By setting the electrode potential with the periodical ON-OFF mode, electrolysis can be forestalled during the off mode which can minimize the sensor signal baseline drift and reduce the power consumption of the sensor. However, it is known that the relaxation of the structure in the electrical double layer at the ionic liquid/electrode interface to the steps of the electrode potential is slow. This work characterized the electrode/electrolyte interfacial relaxation process of an ionic liquid based electrochemical gas (IL-EG) sensor by performing multiple potential step experiments in which the potential is stepped from an open circuit potential (OCP) to the amperometric sensing potential at various frequencies with different time periods. Our results showed that by shortening the sensing period as well as extending the idle period (i.e., enlarge the ratio of idle period versus sensing period) of the potential step experiments, the electrode/electrolyte interface is prone to relax to its original state, and thus reduces the baseline drift. Additionally, the high viscosity of the ionic liquids is beneficial for electrochemical regeneration via the implementation of a conditioning step at zero volts at the electrode/electrolyte. By setting the working electrode at zero volts instead of OCP, our results showed that it could further minimize the baseline drift, enhance the sensing signal stability, and extend the functioning lifetime of a continuous IL-EG oxygen sensor.

Dataset Information

Integrated CO₂ capture-fixation chemistry via interfacial ionic liquid catalyst in laminar gas/liquid flow.

Publications

Integrated CO<sub>2</sub> capture-fixation chemistry via interfacial ionic liquid catalyst in laminar gas/liquid flow.

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