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探索单乙醇胺功能化氧化铜电极在电化学CO还原中的稳定性和催化活性。

Exploring the stability and catalytic activity of monoethanolamine functionalized CuO electrode in electrochemical CO reduction.

作者信息

de Almeida Jéssica C, Lopes Osmando F, Shviro Meital, da Silva Gelson T S T, Ribeiro Caue, de Mendonça Vagner R

机构信息

Federal University of São Carlos, Science and Technology Center for Sustainability, 18052-780, Sorocaba, SP, Brazil.

Laboratory of Photochemistry and Materials Science, Institute of Chemistry, Federal University of Uberlândia, Uberlândia, MG, Brazil.

出版信息

Nanoscale. 2024 Oct 10;16(39):18455-18467. doi: 10.1039/d4nr01919a.

Abstract

Electrochemical carbon dioxide reduction reactions (eCORR) have emerged as promising strategies for both mitigating CO emissions and converting them into valuable products. Despite the promise, challenges such as stability, efficiency, and availability of CO on the electrode surface, especially at high current densities, still need to be overcome. Herein, this study explores the precipitation of CuO nanoparticles with monoethanolamine to preserve nitrogen groups on the surface of the material. These groups can act by adsorbing the CO and stabilizing its catalytic performance during the electroreduction procedure. The incorporation of monoethanolamine as functionalization on the surface of the CuO catalyst was confirmed by XPS measurements. Electrodes utilizing the S-MEA catalyst demonstrated enhanced electrochemical activity, achieving a current density of -187 mA cm at a half-cell potential of -1.2 V RHE. Furthermore, long-term stability tests confirmed consistent activity for at least 100 hours in both flow cell and zero gap cell configurations. These results indicate that electrodes featuring the S-MEA catalyst display notably superior electrochemical activity and stability compared with the non-functionalized CuO (S-KOH) and commercial CuO nanopowder (c-CuO). The S-MEA enhancement is attributed to the introduction of amine functional groups that serve as CO adducts, facilitating CO adsorption and fostering electrode activation. It was evidenced by higher current densities and improved structural integrity during prolonged tests. The insights gained from the comparative performance of these electrodes provide valuable directions for future research in developing more robust and efficient catalysts for environmental remediation technologies.

摘要

电化学二氧化碳还原反应(eCORR)已成为缓解二氧化碳排放并将其转化为有价值产品的有前景策略。尽管前景广阔,但仍需克服一些挑战,如稳定性、效率以及电极表面一氧化碳的可用性,尤其是在高电流密度下。在此,本研究探索了用单乙醇胺沉淀氧化铜纳米颗粒以保留材料表面的氮基团。这些基团可通过吸附一氧化碳并在电还原过程中稳定其催化性能来发挥作用。XPS测量证实了在氧化铜催化剂表面引入了单乙醇胺作为功能化基团。使用S-MEA催化剂的电极表现出增强的电化学活性,在-1.2 V(相对于可逆氢电极)的半电池电位下实现了-187 mA cm的电流密度。此外,长期稳定性测试证实,在流通池和零间隙池配置中至少100小时内活性保持一致。这些结果表明,与未功能化的氧化铜(S-KOH)和商业氧化铜纳米粉末(c-CuO)相比,具有S-MEA催化剂的电极表现出明显优越的电化学活性和稳定性。S-MEA的增强归因于引入了作为一氧化碳加合物的胺官能团,促进了一氧化碳的吸附并促进了电极活化。在长时间测试中更高的电流密度和改善的结构完整性证明了这一点。从这些电极的比较性能中获得的见解为未来开发更强大、更高效的环境修复技术催化剂的研究提供了有价值的方向。

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