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Electroreduction of carbon dioxide (CO2) to chemicals is a promising route to convert and utilize CO2 under atmospheric conditions. However, the relative poor reaction efficiency seriously hinders the practical applications of this route. In this work, flowerlike In2S3 assembled by nanoflakes was synthesized via ionothermal method and exhibited a high Faradaic efficiency (FE) of 86 % with excellent formate formation rate of 478 μmol h−1 cm−2 in ionic liquid (IL) electrolyte. Flowerlike structure can provide large electrochemically active surface area and enhance mass transfer rate. Additionally, density functional theory (DFT) calculations reveal that the origin of the improved performance can be attributed to the large adsorption energy of CO2* and OCHO* intermediate on the (440) facet which is the main exposed crystal facet of flowerlike In2S3.[f1] [ABSTRACT FROM AUTHOR]

Abstract: Electroreduction of carbon dioxide (CO2) into high value‐added products is a potential solution to a reduction in CO2 levels and its utilization. One major challenge is the lack of an efficient system that can highly selectively reduce CO2 into desirable products with low energy consumption. Ionic liquids (ILs) have been used as electrolytes for the electroreduction of CO2, and it has been proven that the CO2–cation complex results in a low‐energy pathway. In this work, an ionic microhabitat (IMH) has been built for CO2 electroreduction, and a novel anion‐functionalized IL, 1‐butyl‐3‐methylimidazolium 1,2,4triazolide ([Bmim][124Triz]), has been designed as the reaction medium. The results showed that the IMH played a key role in enhancing the performance of CO2 electroreduction, especially in dominating the product selectivity, which is recognized to be a great challenge in an electroreduction process. New insights into the role of the IMH in higher CO2 solubility, bending linear CO2 by forming the [124Triz]–CO2− adduct, and transferring activated CO2 into the cathode surface easily were revealed. The Faradaic efficiency for formic acid is as high as 95.2 %, with a current density reaching 24.5 mA cm−2. This work provides a promising way for the design of robust and highly efficient ILs for CO2 electroreduction. [ABSTRACT FROM AUTHOR]

Abstract: The increasing emission of carbon dioxide (CO2) caused by the unrestrained consumption of fossil fuels in recent hundreds of years, has caused global environmental and social problems. Meanwhile, CO2 is a cheap, abundant and renewable C1‐feedstock, which can be converted into alcohols, ethers, acids and other value‐added chemicals. Compared with the thermal reactions, electrochemical reduction of CO2 is more attractive because of its advantages by using the seasonal, geographical and intermittent energy (tide, wind and solar) under mild conditions. In recent years, taking ionic liquids (ILs) as electrolytes in the CO2 electrochemical reduction reaction has been paid much more attention due to the advantages of lowering the overpotential of CO2 electroreduction and improving the Faradaic efficiency. In this paper, we summarized the recent progresses of electrochemical reduction of CO2 in ILs electrolytes, and analyzed the reaction mechanism of CO2 reaction in the electrode‐electrolyte interface region by experimental and simulation methods. Finally, the research which needs to be highlighted in this area was proposed. [ABSTRACT FROM AUTHOR]