将 La 引入定制的双铜共价有机框架,引导二氧化碳从 C2H4 到 CH4 的电还原选择性

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Xiao-Yu Dong, Hong Chen, Shan Wang, Ru-Yi Zou, Shuang-Quan Zang, Jinmeng Cai
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引用次数: 0

摘要

定制多金属催化剂以实现可控的CO2还原反应(CO2RR)产品调整具有巨大的前景,但也面临着艰巨的挑战。传统的多金属位点合成方法是含金属前驱体的热解,具有固有的不可控性。本文采用自底向上的策略,在共价有机框架(COFs)中定制合成多金属位点,通过调节活性位点的电子结构,实现CO2还原选择性的可控切换。简而言之,La元素为操纵和微调定制的双Cu位点的电子结构提供了机会,并将CO2RR的主要催化产物从乙烯转化为甲烷。密度泛函理论计算表明,La的引入改变了Cu周围的电子结构,增强了CO2和H2O的活化,改变了关键中间体能垒的形成。据作者所知,本研究构建了首个定制化多金属位点COF催化剂的实例,为产品的可控调制提供了新的思路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Introducing La into a Customized Dual Cu Covalent Organic Framework to Steer CO2 Electroreduction Selectivity from C2H4 to CH4

Introducing La into a Customized Dual Cu Covalent Organic Framework to Steer CO2 Electroreduction Selectivity from C2H4 to CH4

Customizing multi-metal site catalysts for achieving controllable CO2 reduction reaction (CO2RR) product tuning holds immense promise yet poses formidable challenges. The traditional synthesis method of multi-metal sites is the pyrolysis of metal-containing precursors, which is inherently uncontrollable. Herein, a bottom-up strategy is employed to customize and synthesize multi-metal sites in covalent organic frameworks (COFs), aiming to controllably switch the CO2 reduction selectivity by regulating the electronic structure of active sites. Briefly, La element provides chances for manipulating and finetuning the electronic structure of the customized dual Cu sites, and converts the main catalytic product of CO2RR from ethylene to methane. Density functional theory calculations show that the introduction of La alters the electronic structure around Cu, enhances CO2 and H2O activation, and changes the formation of energy barriers of key intermediates. To the best of the author's knowledge, this study constructed the first example of customized multi-metal site COF catalysts and provided new ideas for controllable modulation of products.

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来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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