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基于吡唑盐的金属有机框架用于选择性高效捕获甲醛

Metal-organic frameworks based on pyrazolates for the selective and efficient capture of formaldehyde.

作者信息

Sadovnik Nicolas, Lyu Pengbo, Nouar Farid, Muschi Mégane, Qin Menghao, Maurin Guillaume, Serre Christian, Daturi Marco

机构信息

Université de Caen Normandie, ENSICAEN, CNRS, Laboratoire Catalyse et Spectrochimie, 14000, Caen, France.

Institut des Matériaux Poreux de Paris, Ecole Normale Supérieure, ESPCI Paris, CNRS, PSL University, 75005, Paris, France.

出版信息

Nat Commun. 2024 Nov 1;15(1):9456. doi: 10.1038/s41467-024-53572-z.

Abstract

Indoor air pollution is one of the major threads in developed countries, notably due to high concentrations of formaldehyde, a harmful molecule difficult to eliminate. Addressing this purification challenge while adhering to the principles of sustainable development requires the use of innovative, advanced sustainable materials. Here we show that by combining state-of-the-art spectroscopic techniques with density-functional theory molecular simulations, we have developed an advantageous mild chemisorption synergistic mechanism using porous metal (III or IV) pyrazole- di-carboxylate based metal-organic framework (MOF) to trap formaldehyde in a reversible manner, without incurring significant energy penalties for regeneration. A straightforward, environmentally friendly, and scalable synthesis protocol was established for the porous, water-stable aluminum pyrazole dicarboxylate known as Al-3.5-PDA or MOF-303, capable of functioning as a highly efficient and reusable filter. It demonstrates selectivity and high storage capacity for formaldehyde under conditions typical of severe indoor use, such as in housing or vehicle cockpits, including varying VOC mixtures and concentrations, humidity, and temperature, without any accidental release. Furthermore, we have successfully regenerated this sorbent using a simple domestic protocol, ensuring the material reusability for at least 10 cycles.

摘要

室内空气污染是发达国家面临的主要问题之一,尤其是由于甲醛浓度过高,甲醛是一种难以消除的有害分子。在坚持可持续发展原则的同时应对这一净化挑战,需要使用创新的先进可持续材料。在此我们表明,通过将最先进的光谱技术与密度泛函理论分子模拟相结合,我们开发了一种有利的温和化学吸附协同机制,使用基于多孔金属(III或IV)吡唑二羧酸酯的金属有机框架(MOF)以可逆方式捕获甲醛,而不会因再生而产生显著的能量损失。我们为一种名为Al-3.5-PDA或MOF-303的多孔、水稳定的吡唑二羧酸铝建立了一种简单、环保且可扩展的合成方案,该材料能够作为高效且可重复使用的过滤器发挥作用。它在典型的严重室内使用条件下,如在房屋或汽车驾驶舱中,包括不同的挥发性有机化合物混合物和浓度、湿度和温度,对甲醛表现出选择性和高存储容量,且不会有任何意外释放。此外,我们已使用简单的家庭方法成功再生了这种吸附剂,确保该材料至少可重复使用10个循环。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/305b/11530664/003f49e35d5a/41467_2024_53572_Fig1_HTML.jpg

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