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通过铜电极与p区元素的界面工程开辟直接电化学费托合成路径

Opening Direct Electrochemical Fischer-Tropsch Synthesis Path by Interfacial Engineering of Cu Electrode with P-Block Elements.

作者信息

Yang Ju Hyun, Hwang Seon Young, Maeng Ju Young, Park Go Eun, Yang Seo Young, Rhee Choong Kyun, Sohn Youngku

机构信息

Department of Chemical Engineering and Applied Chemistry, Chungnam National University, Daejeon 34134, Republic of Korea.

Department of Chemistry, Chungnam National University, Daejeon 34134, Republic of Korea.

出版信息

ACS Appl Mater Interfaces. 2024 Jan 24;16(3):3368-3387. doi: 10.1021/acsami.3c15596. Epub 2024 Jan 12.

Abstract

The electrochemical synthesis of syngas (CO and H) has garnered considerable attention in the context of Fischer-Tropsch (FT) synthesis employing thermal catalysts. Nonetheless, the need for a novel, cost-effective technique persists. In this investigation, we introduce a direct electrochemical (dEC) approach for FT synthesis that functions under ambient conditions by utilizing a p-block element (Sn and In) overlaid Cu electrode. Surface CO and H species were obtained in an electrolytic medium through the CO + H + e → HOOC → CO (or direct CO adsorption) and H + e → H reactions, respectively. We have observed C long-chain hydrocarbons with a CH/CH ratio of 1-3, and this observation can be explained through the process of C-C coupling chain growth of the conventional FT synthesis, based on the linearity of the Anderson-Schulz-Flory equation plots. Thick Sn and In overlayers resulted in the dominant production of formate, while CO and CH production were found to be proportional and inversely correlated to H, CH, and C hydrocarbon production. The EC CO/CO reduction used in dEC FT synthesis offers valuable insights into the mechanism of C production and holds promise as an eco-friendly approach to producing long-chain hydrocarbons for energy and environmental purposes.

摘要

在使用热催化剂的费托(FT)合成背景下,合成气(CO和H)的电化学合成已引起了相当大的关注。尽管如此,对一种新颖、具有成本效益的技术的需求仍然存在。在本研究中,我们引入了一种用于FT合成的直接电化学(dEC)方法,该方法通过使用覆盖在Cu电极上的p区元素(Sn和In)在环境条件下运行。在电解介质中,分别通过CO + H + e → HOOC → CO(或直接CO吸附)和H + e → H反应获得了表面CO和H物种。我们观察到了CH/CH比为1 - 3的C长链烃,基于安德森 - 舒尔茨 - 弗洛里方程图的线性关系,这一观察结果可以通过传统FT合成的C - C偶联链增长过程来解释。厚的Sn和In覆盖层导致甲酸盐的大量生成,而CO和CH的生成被发现与H、CH和C烃的生成成比例且呈负相关。dEC FT合成中使用的EC CO/CO还原为C生成机制提供了有价值的见解,并有望成为一种用于能源和环境目的生产长链烃的环保方法。

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