了解反应参数对CO2电化学还原制甲醇的影响:cuprite@polyaniline电极的活性关系

IF 4.5 3区 化学 Q1 Chemical Engineering
Atul A. Pawar, Harshad A. Bandal, Anand Rajkamal, Hern Kim
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引用次数: 0

摘要

二氧化碳还原反应(CO2RR)是有效利用二氧化碳生产增值化学品的关键反应。然而,该反应的主要限制是其选择性低,导致形成各种副产物。因此,目前CO2RR面临的挑战是高效形成具有高法拉第效率(FE)的产品。我们的主要目标是用更丰富的过渡金属/导电载体混合催化剂取代贵金属电催化剂。在此,我们合成了铜-聚苯胺(Cu2O@PANI)复合材料。在活性和选择性方面,优异的催化活性可归因于Cu2O和PANI之间的协同作用,使其能够减少多种物质,在电荷/质量传递过程中具有更高的电导率和最低的电阻。这些特性通过电化学阻抗谱(EIS)、电子传递速率常数(Ks)、Mott-Schottky (MS)、双层电容(DLC)和密度泛函理论(DFT)分析得到证实。基于这些发现Cu2O@PANI基质容易形成许多中间(CO)物质,并在整个实验过程中在电极表面周围保持较高的CO2浓度。实验结果表明,在整个实验过程中,Cu2O@PANI基质显著抑制了副产物的产生,在90 min内获得了45.21%的MeOH FE。考虑到这些优点,该催化体系适合CO2RR。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Understanding the impact of reaction parameters on electrochemical reduction of CO2 to methanol: Activity relationship of cuprite@polyaniline electrodes

Understanding the impact of reaction parameters on electrochemical reduction of CO2 to methanol: Activity relationship of cuprite@polyaniline electrodes

The carbon dioxide reduction reaction (CO2RR) is a key reaction that efficiently uses CO2 to produce value-added chemicals. However, the main limitation of this reaction is its low selectivity which results in the formation of a variety of by-products. As a result, the current challenge for CO2RR is the efficient formation of product with high Faradaic efficiency (FE). Our main goal is to replace precious metal electrocatalysts with more abundant transition metal/conducting support hybrid catalysts. Herein, we’ve synthesized a cuprite-polyaniline (Cu2O@PANI) composites. The superior catalytic activity in terms of activity and selectivity for methanol (MeOH) synthesis could be attributed to the synergism between Cu2O and PANI that enables it to scale back multiple species, higher electrical conductivity, and lowest resistance during the charge/mass transfer processes. These properties were confirmed using Electrochemical impedance spectroscopy (EIS), Electron transfer rate constant (Ks), Mott-Schottky (MS), Double-layer capacitance (DLC), and Density-functional theory (DFT) analysis. Based on these findings Cu2O@PANI matrix easily forms many intermediate (CO) species and maintains a higher CO2 concentration around the electrode surface throughout the experiment. The results of the given electrocatalytic system show that the Cu2O@PANI matrix significantly suppressed the by-product throughout the experiment, resulting in MeOH (45.21%) FE within 90 min. Given these benefits, the catalytic system is appropriate for CO2RR.

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来源期刊
Journal of Electroanalytical Chemistry
Journal of Electroanalytical Chemistry Chemical Engineering-General Chemical Engineering
CiteScore
7.50
自引率
6.70%
发文量
912
审稿时长
>12 weeks
期刊介绍: The Journal of Electroanalytical Chemistry is the foremost international journal devoted to the interdisciplinary subject of electrochemistry in all its aspects, theoretical as well as applied. Electrochemistry is a wide ranging area that is in a state of continuous evolution. Rather than compiling a long list of topics covered by the Journal, the editors would like to draw particular attention to the key issues of novelty, topicality and quality. Papers should present new and interesting electrochemical science in a way that is accessible to the reader. The presentation and discussion should be at a level that is consistent with the international status of the Journal. Reports describing the application of well-established techniques to problems that are essentially technical will not be accepted. Similarly, papers that report observations but fail to provide adequate interpretation will be rejected by the Editors. Papers dealing with technical electrochemistry should be submitted to other specialist journals unless the authors can show that their work provides substantially new insights into electrochemical processes.
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