Thiol treatment tunes interfacial wettability for electrochemical alkynol semi-hydrogenation

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal Pub Date : 2024-08-23 DOI:10.1002/aic.18588

Xingzhou Zha, Yuan Zhao, Hongliang Jiang, Chunzhong Li

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引用次数: 0

Abstract

Electrocatalytic semi-hydrogenation of alkynols holds tremendous advantages over conventional thermocatalysis process. However, the selectivity-activity seesaw effect is a principal obstacle to its further development. Inspired by interfacial self-assembled monolayers, alkanethiols with different alkyl chain lengths are employed to modify the Cu surface for controllably modulating the activity and selectivity in the semi-hydrogenation of alkynols. 1-dodecanethiol-modified Cu nanowires (Cu NWs) exhibit the optimal electrosynthesis of 2-methyl-3-buten-2-ol with excellent specific selectivity (above 93%) in the semi-hydrogenation of 2-methyl-3-butyn-2-ol. Mechanistic studies reveal that the proportion of liquid-like water increases while the proportion of isolated water reduces at the hydrophobic interface. Moreover, we assemble a larger 3 × 100 cm² electrolyzer stack, which can deliver a single-pass alkynol conversion rate of 95% and an excellent alkenol selectivity of 94% at a 15 A stack current. Eventually, the Cu NWs catalyst with thiol treatment is also applicable to the semi-hydrogenation of various unsaturated alkynols.

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硫醇处理可调节电化学炔醇半加氢的界面润湿性

与传统的热催化工艺相比，电催化半氢化炔醇具有巨大的优势。然而，选择性-活性跷跷板效应是其进一步发展的主要障碍。受界面自组装单层的启发，我们采用了不同烷基链长的烷硫醇来修饰铜表面，从而可控地调节炔醇半加氢反应的活性和选择性。在 2-甲基-3-丁炔-2-醇的半加氢反应中，1-十二烷硫醇修饰的铜纳米线（Cu NWs）表现出了最佳的 2-甲基-3-丁烯-2-醇的电合成性能和优异的特定选择性（超过 93%）。机理研究表明，在疏水界面上，液态水的比例增加，而孤立水的比例减少。此外，我们还组装了一个更大的 3 × 100 平方厘米电解槽堆栈，在 15 A 堆栈电流条件下，单程炔醇转化率可达 95%，烯醇选择性高达 94%。最终，经硫醇处理的 Cu NWs 催化剂也适用于各种不饱和炔醇的半加氢反应。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.