Carbon dioxide (CO2) is currently considered as a waste material due to its negative impact on the environment. However, it is possible to create value from CO2 by capturing and utilizing it as a building block for commodity chemicals. Electrochemical conversion of CO2 has excellent potential for reducing greenhouse gas emissions and reaching the Paris agreement goal of zero net emissions by 2050. To date, Carbon Capture and Utilization (CCU) technologies (i.e. capture and conversion) have been studied independently. In this communication, we report a novel methodology based on the integration of CO2 capture and conversion by the direct utilization of a CO2 capture media as electrolyte for electrochemical conversion of CO2. This has a high potential for reducing capital and operational cost when compared to traditional methodologies (i.e. capture, desorption and then utilization). A novel mixture of chemical and physical absorption solvents allowed for the captured CO2 to be converted to formic acid with faradaic efficiencies up to 50 % and with carbon conversion of ca. 30 %. By increasing the temperature in the electrochemical reactor from 20 °C to 75 °C, the productivity towards formic acid increased by a factor of 10, reaching up to 0.7 mmol•m-2 •s-1. The direct conversion of captured CO2 was also demonstrated for carbon monoxide formation with faradaic efficiencies up 45 %.
The influence of CO2 partial pressure on electrochemical reduction of CO2 using oxide-derived electrodeposited copper surfaces in a conventional two compartment cell configuration, is discussed. Contrary to what has been...
Dimethyl ether (DME) is an important platform chemical and fuel that can be synthesized from CO2 and H2 directly. In particular, sorption-enhanced DME synthesis (SEDMES) is a novel process that uses the in situ removal of H2O with an adsorbent to ensure high conversion efficiency in a single unit operation. The in situ removal of steam has been shown to enhance catalyst lifetime and boost process efficiency. In addition, the hydrogen may be supplied through water electrolysis using renewable energy, making it a promising example of the (indirect) power-to-X technology. Recently, major advances have been made in SEDMES, both experimentally and in terms of modeling and cycle design. The current work presents a techno-economic evaluation of SEDMES using H2 produced by a PEM electrolyzer. A conceptual process design has been made for the conversion of CO2 and green H2 to DME, including the purification section to meet ISO fuel standards. By means of a previously developed dynamic cycle model for the SEDMES reactors, a DME yield per pass of 72.4 % and a carbon selectivity of 84.7% were achieved for the studied process design after optimization of the recycle streams. The production costs for DME by the power-to-X technology SEDMES process at 23 kt/year scale are determined at ∼€1.3 per kg. These costs are higher than the current market price but lower than the cost of conventional DME synthesis from CO2. Factors with the highest impact on the business cases are the electricity and CO2 cost price as well as the CAPEX of the electrolyzer, which is considered an important component for technology development. Furthermore, as the H2 cost constitutes the largest part of the DME production cost, SEDMES is demonstrated to be a powerful technology for efficient conversion of green H2 into DME.
Herein, we describe a study of the electrochemical reduction of oxalic and glyoxylic acids toward a feasible green and sustainable production of tartaric acid in aqueous and/or acetonitrile solvent using silver and lead electrodes. Our results show that on the silver electrode, for both oxalic acid and glyoxylic acid, the reduction reaction is more favorable toward the dimerization step, leading to tartaric acid, due to the increase in the local pH, while on the lead electrode, the step involving the protonation of the intermediate is more favorable, leading to the formation of glycolate. Techno-economic analysis shows that tartaric acid production from glyoxylic acid and from oxalic acid via electrochemical synthesis can be a potential process at the industrial scale. In the present case, the oxygen evolution reaction was chosen as the reaction at the other electrode for practical reasons, but oxygen is a low-value product. Another anodic reaction with a more valuable oxidation product can be selected to increase the profitability of the overall electrochemical process and thereby decrease the total production costs of tartaric acid.
Electrochemical processes are a promising technology for industrial production of chemicals. One of the major drawbacks of electrochemical systems is the low mass transfer of reactants toward the active surface area of the electrode. In this paper, an approach is presented to enhance the mass transfer and increase the overall performance of the reactions. The strategy comprises introduction of a pulsed electrolyte flow in the electrochemical flow cell. This pulsating behavior results in an improved mass transfer of electroactive species due to a higher instantaneous velocity driven by the pulsations. Though the net residence time of the reactants will not be altered due to the pulsation, the resulting enhancement of mass transfer leads to an increase of the conversion. The oxidation of 1,2-propanediol to lactic acid and pyruvic acid mediated by 4-acetamido-(2,2,6,6-tetramethylpiperidin-1-yl) oxidanyl (ACT-TEMPO) was chosen to study the influence of the pulsed flow. Under the pulsating regime, a yield increase of lactic acid of a factor of two and a 15−20% gain in selectivity to a total of 95% toward lactic acid can be achieved by tuning the process parameters.
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