二氧化铈诱导丰富的 Cu+/Cu0 位点,用于电催化将二氧化碳还原为 C2+ 产物。

IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
ChemSusChem Pub Date : 2024-11-18 DOI:10.1002/cssc.202402097
Yuwen Wang, Jiajun Wang, Shuang Liu, Xuan Zhang, Lin Jin, Lanlan Feng, Demeng Kong, Chenxi Zhang, Yajuan Wei, Jingbo Zhang
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引用次数: 0

摘要

近年来,二氧化碳的电化学还原(CO2RR)在 C2+ 生产方面取得了许多进展。Cu+/Cu0 位点有利于 C-C 偶联过程,但铜的氧化态在反应过程中不能很好地保持,导致催化剂活性下降。基于这一考虑,本研究引入了具有中空立方体结构和氧空位的过渡金属氧化物 CeO2 来稳定和增加 Cu+/Cu0 活性位点(Ce1Cu2)。该催化剂具有优异的 CO2RR 性能,在 1.26 V(相对于 RHE)电压下,FEC2+ 达到 73.52%,jC2+ > 280 mA/cm2。实验结果表明,CeO2 的存在提供了大量的氧空位,并通过 CeO2 和 Cu NPs 的强相互作用形成了 Cu+-O2-Ce4+ 结构。Cu+-O2-Ce4+ 结构和丰富的氧空位为二氧化碳的吸附奠定了良好的基础。此外,它还增加了 Cu+/Cu0 位点的含量,有效抑制了氢进化反应,促进了 C-C 偶联作用,从而促进了 C2+ 产物的生成。DFT 理论计算进一步证明,Ce1Cu2 更倾向于乙醇途径,证实了它对乙醇的高选择性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Cerium Dioxide-Induced Abundant Cu+/Cu0 Sites for Electrocatalytic Reduction of Carbon Dioxide to C2+ Products.

In recent years, the electrochemical reduction of carbon dioxide (CO2RR) has made many advances in C2+ production. Cu+/Cu0 site is beneficial for C-C coupling process, but the oxidation state of copper cannot be well maintained during the reaction process, resulting in a decrease in catalyst activity. Based on this consideration, in this work, transition metal oxide CeO2 with a hollow cube structure and oxygen vacancies was introduced to stabilize and increase Cu+/Cu0 active sites (Ce1Cu2). The catalyst exhibits excellent CO2RR performance, with FEC2+ achieving 73.52 % and jC2+ >280 mA/cm2 at 1.26 V (vs. RHE). Ethanol is the main C2+ product and FEethanol reaches 39 % at 1.26 V. The experimental results indicate that the presence of CeO2 provides a large number of oxygen vacancies and forming Cu+-O2--Ce4+ structure by the strong interaction of CeO2 and Cu NPs. The structure of Cu+-O2--Ce4+ and abundant oxygen vacancies lay a good foundation for the CO2 adsorption. Moreover, it increases the content of Cu+/Cu0 sites, effectively inhibiting hydrogen evolution reaction, promoting the C-C coupling interaction, thereby facilitating the generation of C2+ products. The DFT theoretical calculation further demonstrates that Ce1Cu2 is more inclined towards the ethanol pathway, confirming its high selectivity for ethanol.

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来源期刊
ChemSusChem
ChemSusChem 化学-化学综合
CiteScore
15.80
自引率
4.80%
发文量
555
审稿时长
1.8 months
期刊介绍: ChemSusChem Impact Factor (2016): 7.226 Scope: Interdisciplinary journal Focuses on research at the interface of chemistry and sustainability Features the best research on sustainability and energy Areas Covered: Chemistry Materials Science Chemical Engineering Biotechnology
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