利用含自由基的共价三嗪框架高效捕获碳氟化合物

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2024-10-31 DOI:10.1021/jacs.4c1147010.1021/jacs.4c11470
Zhiyuan Zhang, Shuo Zhang, Xiongli Liu, Lin Li, Shan Wang, Rufeng Yang, Laiyu Zhang, Zifeng You, Feng Shui, Shiqi Yang, Zhendong Yang, Qiao Zhao, Baiyan Li* and Xian-He Bu, 
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引用次数: 0

摘要

碳氟化合物是全球变暖潜势(GWP)很高的强效温室气体,由于构建高性能吸附剂的有效方法有限,高效捕获碳氟化合物仍然是一项艰巨的挑战。为了解决这个问题,我们开创了一种新策略,即开发自由基多孔材料,作为捕获碳氟化合物的有效吸附剂。由此产生的自由基共价三嗪框架(CTF)--CTF-azo-R 显示出卓越的碳氟化合物(全氟己烷,碳氟化合物中具有代表性的示范污染物)吸附能力,达到 270 wt %,在迄今报道的所有多孔材料中创下新高。光谱特征、实验研究和理论计算表明,CTF-azo-R 中稳定自由基的存在有助于其卓越的碳氟化合物捕获性能。此外,CTF-AZO-R 还具有极高的化学稳定性和热稳定性,完全符合在各种环境中实际应用的要求。我们的研究工作不仅将自由基 CTF-azo-R 确立为碳氟化合物捕集的理想候选材料,而且通过在多孔材料中加入自由基位点,引入了一种构建先进碳氟化合物吸附剂的新方法。这一策略为自由基吸附剂的开发铺平了道路,促进了碳氟化合物捕获以及更广泛的吸附和分离领域的进步。
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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Efficient Fluorocarbons Capture Using Radical-Containing Covalent Triazine Frameworks

Efficiently capturing fluorocarbons, potent greenhouse gases with high global warming potentials (GWP), remains a daunting challenge due to limited effective approaches for constructing high-performance adsorbents. To tackle this issue, we have pioneered a novel strategy of developing radical porous materials as effective adsorbents for fluorocarbon capture. The resulting radical covalent triazine framework (CTF), CTF-azo-R, shows exceptional fluorocarbon (perfluorohexane, a representative model pollutant among fluorocarbons) uptake capacity of 270 wt %, a record-high value among all porous materials reported to date. Spectral characteristics, experimental studies, and theoretical calculations indicate that the presence of stable radicals in CTF-azo-R contributes to its superior fluorocarbon capture performance. Furthermore, CTF-azo-R demonstrates exceptionally high chemical and thermal stabilities that fully meet the requirements for practical applications in diverse environments. Our work not only establishes radical CTF-azo-R as a promising candidate for fluorocarbon capture but also introduces a novel approach for constructing advanced fluorocarbon adsorbents by incorporating radical sites into porous materials. This strategy paves the way for the development of radical adsorbents, fostering advancements in both fluorocarbon capture and the broader field of adsorption and separation.

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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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