由于构建高性能吸附剂的有效方法有限,高效捕获具有高全球变暖潜能值(GWP)的强效温室气体氟碳化合物仍,然是一项艰巨的挑战。
为了解决这个问题,课题组研究人员开创了一种新的策略,开发自由基多孔材料作为氟碳捕获的有效吸附剂。由此产生的自由基共价三嗪框架(CTF)——CTF-azo-R显示出异常的氟碳吸收能力(全氟己烷,氟碳化合物中的代表性模型污染物)吸收能力为270 wt%,这是迄今报告的所有多孔材料中的最高记录。
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优越的氟碳捕获性能。此外,CTF-azo-R表现出极高的化学和热稳定性,完全满足各种环境下实际应用的要求。
他们的工作不仅确立了自由基CTF-azo-R作为碳氟化合物捕获的有希望的候选者,而且还引入了一种通过将自由基位点结合到多孔材料中,来构建先进碳氟化合物吸附剂的新方法。这一战略为自由基吸附剂的发展铺平了道路,促进了氟碳捕获和更广泛的吸附与分离科学领域的进步。
附:英文原文
Title: Efficient Fluorocarbons Capture Using Radical-Containing Covalent Triazine Frameworks
Author: 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, Xian-He Bu
Issue&Volume: October 31, 2024
Abstract: 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.
DOI: 10.1021/jacs.4c11470
Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c11470
JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:16.383
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