Dataset Information

Electrochemical ?-Selective Hydrocarboxylation of Styrene Using CO2 and Water.

ABSTRACT: The carboxylation of hydrocarbons using CO2 as a one-carbon building block is an attractive route for the synthesis of carboxylic acids and their derivatives. Until now, chemical carboxylation catalyzed by organometallic nucleophiles and reductants has been generally adopted particularly for the precise selectivity control of carboxylation sites. As another approach, electrochemical carboxylation has been attempted but these carboxylation reactions are limited to only a few pathways. In the case of styrene, dicarboxylation at the ?- and ?-positions is mostly observed with electrochemical carboxylation while site-selective hydrocarboxylations are hardly achieved. In this study, electrochemical ?-selective hydrocarboxylation of styrene using CO2 and water is developed, in which the site selectivity can be precisely controlled between ?-hydrocarboxylation and dicarboxylation without the aid of homogeneous catalysts. In this platform, water is used as proton source in the ?-hydrocarboxylation of styrene where its addition results in significant enhancement of the selectivity toward ?-hydrocarboxylation. This work provides insights into new strategies for site-selectivity-controllable carboxylation with CO2 using an electrochemical platform.

SUBMITTER: Kim Y

PROVIDER: S-EPMC7001630 | biostudies-literature | 2020 Feb

REPOSITORIES: biostudies-literature

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Publications

Electrochemical β-Selective Hydrocarboxylation of Styrene Using CO<sub>2</sub> and Water.

Kim Younghye Y Park Gyeong Do GD Balamurugan Mani M Seo Jiwon J Min Byoung Koun BK Nam Ki Tae KT

Advanced science (Weinheim, Baden-Wurttemberg, Germany) 20191217 3

The carboxylation of hydrocarbons using CO<sub>2</sub> as a one-carbon building block is an attractive route for the synthesis of carboxylic acids and their derivatives. Until now, chemical carboxylation catalyzed by organometallic nucleophiles and reductants has been generally adopted particularly for the precise selectivity control of carboxylation sites. As another approach, electrochemical carboxylation has been attempted but these carboxylation reactions are limited to only a few pathways. ...[more]

PMID: 32042549

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Project description:Metal-organic frameworks (MOFs) have been an excellent platform for carbon dioxide reduction reactions (CO2RR). In this work, the feasibility of electrochemical reduction of CO2 to obtain C2-deep value-added products was investigated by the preparation of Mg-containing MOF-74 samples combined with transition metal cations (Ni2+, Co2+ and Zn2+). The prepared MOFs were used as electrocatalysts in CO2RR. Chronoamperometric analysis coupled to ATR-FTIR spectroscopy was employed to characterize the CO2 reduction products and subsequently via 1H NMR. Although an isostructural crystalline structure was observed in all synthesized MOFs, the pore diameter distribution was significantly affected due to the Mg coordination along with each transition metal nuclei with the organic ligand to form the MOF-74. Our results showed that Mg-containing MOF-74 electrocatalysts combined with Ni, Co and Zn ions successfully reduced CO2 to C2-deep products, while the monometallic Mg-MOF-74 showed only CO2 mineralization. An ester acetate, isopropyl alcohol, and formic acid were produced by Mg/Ni-MOF-74; isopropyl alcohol was provided by Mg/Co-MOF-74, and ethanol was generated by Mg/Zn-MOF-74. We observed that the change of the transition cation was a key factor in the selectivity of the obtained products, while the degree of Mg ions effectively incorporated into the MOF structure tuned the porosity and the electrocatalytic activity. Among them, Mg/Zn-MFOF-74 showed the highest Mg content loaded after synthesis and thus the most favorable electrocatalytic behavior towards CO2 reduction. Highlights • CO2-derived C2-deep reduction products were obtained by Mg-containing MOF-74 bimetallic electrocatalysts.• Mg-containing MOF-74 bimetallic electrocatalysts reduced CO2 to ester acetate, isopropanol, formic acid, and ethanol.• Mg/Zn-MOF-74 displayed the highest current density at a lower onset potential in CO2-saturated electrolyte.• The pore network could be tuned by the effective Mg content on a MOF-74 bimetallic sample.• Mg/Zn-MOF-74 showed the highest Mg content among all bimetallic electrocatalysts after the synthesis.

Dataset Information

Electrochemical ?-Selective Hydrocarboxylation of Styrene Using CO2 and Water.

Publications

Electrochemical β-Selective Hydrocarboxylation of Styrene Using CO<sub>2</sub> and Water.

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