{"title":"酶电化学二氧化碳还原甲酸盐的理论性能优化:电压、浓度、温度、压力和流速","authors":"Daniel Moreno","doi":"10.1016/j.jcou.2024.102805","DOIUrl":null,"url":null,"abstract":"<div><p>Formic acid (FA) is a notable fuel product due to its atom economy, low activation energy, and applications in flow cells and hydrogen storage. While metal catalysts are typically used, selectivity remains a challenge. Here, an enzymatic catalyst is employed to selectively convert CO<sub>2</sub> to FA as formate. This study documents the development of a computational model to examine the conversion of CO<sub>2</sub> to formate under a wide range of conditions. The model examines the electrochemical reduction of a charge carrier, ethyl viologen (EV), and its subsequent use in an enzymatic catalyst to convert CO<sub>2</sub> and protons in solution to formate. The model was first developed for a small-scale batch reactor, then later expanded to a dual-cell flow system, where the reduction of EV and production of formate are kept in separated cells, and flow rate is introduced as an additional variable parameter. While no studies have directly used all parameters addressed in the computations presented here, many of the conditions selected align with what has previously been used in experiments, and similar production rates and efficiencies are obtained. The most challenging parameters to study were charge carrier concentration and applied voltage, which showed optimal ranges in the cases studied for the batch and flow cell. While the study gives guidance toward which conditions would be favored experimentally to increase production rate and efficiency experimental studies should nonetheless be run at suggested optimal conditions to better adapt parameters made in both models.</p></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":null,"pages":null},"PeriodicalIF":7.2000,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2212982024001409/pdfft?md5=f6377c1855129e0938a9408868897a58&pid=1-s2.0-S2212982024001409-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Theoretical performance optimization of enzymatic electrochemical CO2 reduction to formate: Voltage, concentration, temperature, pressure, and flow rate\",\"authors\":\"Daniel Moreno\",\"doi\":\"10.1016/j.jcou.2024.102805\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Formic acid (FA) is a notable fuel product due to its atom economy, low activation energy, and applications in flow cells and hydrogen storage. 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While no studies have directly used all parameters addressed in the computations presented here, many of the conditions selected align with what has previously been used in experiments, and similar production rates and efficiencies are obtained. The most challenging parameters to study were charge carrier concentration and applied voltage, which showed optimal ranges in the cases studied for the batch and flow cell. 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引用次数: 0
摘要
甲酸(FA)因其原子经济性、低活化能以及在流动电池和储氢中的应用而成为一种著名的燃料产品。虽然通常使用金属催化剂,但选择性仍然是一个挑战。本研究采用酶催化剂将二氧化碳选择性地转化为甲酸甲酯。本研究记录了一个计算模型的开发过程,该模型用于研究在各种条件下将 CO2 转化为甲酸盐的过程。该模型研究了电荷载体乙基紫精(EV)的电化学还原过程,以及随后利用酶催化剂将溶液中的二氧化碳和质子转化为甲酸盐的过程。该模型最初是为一个小规模间歇式反应器开发的,后来扩展到一个双池流动系统,在该系统中,EV 的还原和甲酸盐的生成是在分离的池中进行的,并且引入了流速作为额外的可变参数。虽然没有任何研究直接使用了本文计算中涉及的所有参数,但所选的许多条件与之前实验中使用的条件一致,并获得了类似的生产率和效率。研究中最具挑战性的参数是电荷载流子浓度和外加电压,这两个参数在所研究的间歇式和流动池中均显示出最佳范围。虽然这项研究提供了实验条件方面的指导,以提高生产率和效率,但实验研究仍应在建议的最佳条件下进行,以便更好地调整两种模型中的参数。
Theoretical performance optimization of enzymatic electrochemical CO2 reduction to formate: Voltage, concentration, temperature, pressure, and flow rate
Formic acid (FA) is a notable fuel product due to its atom economy, low activation energy, and applications in flow cells and hydrogen storage. While metal catalysts are typically used, selectivity remains a challenge. Here, an enzymatic catalyst is employed to selectively convert CO2 to FA as formate. This study documents the development of a computational model to examine the conversion of CO2 to formate under a wide range of conditions. The model examines the electrochemical reduction of a charge carrier, ethyl viologen (EV), and its subsequent use in an enzymatic catalyst to convert CO2 and protons in solution to formate. The model was first developed for a small-scale batch reactor, then later expanded to a dual-cell flow system, where the reduction of EV and production of formate are kept in separated cells, and flow rate is introduced as an additional variable parameter. While no studies have directly used all parameters addressed in the computations presented here, many of the conditions selected align with what has previously been used in experiments, and similar production rates and efficiencies are obtained. The most challenging parameters to study were charge carrier concentration and applied voltage, which showed optimal ranges in the cases studied for the batch and flow cell. While the study gives guidance toward which conditions would be favored experimentally to increase production rate and efficiency experimental studies should nonetheless be run at suggested optimal conditions to better adapt parameters made in both models.
期刊介绍:
The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials.
The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications.
The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.