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利用超亲水纳米级金属有机框架结构从水中高效分离油性污染物的节能超高通量分离技术。

Energy Efficient Ultrahigh Flux Separation of Oily Pollutants from Water with Superhydrophilic Nanoscale Metal-Organic Framework Architectures.

作者信息

Mähringer Andre, Hennemann Matthias, Clark Timothy, Bein Thomas, Medina Dana D

机构信息

Department of Chemistry and Center for NanoScience (CeNS), Ludwig-Maximilians-Universität (LMU), Butenandtstr. 5-13, 81377, Munich, Germany.

Computer-Chemistry-Center, Department of Chemistry and Pharmacy, Friedrich-Alexander-University Erlangen-Nuremberg, Naegelsbachstr. 25, 91052, Erlangen, Germany.

出版信息

Angew Chem Int Ed Engl. 2021 Mar 1;60(10):5519-5526. doi: 10.1002/anie.202012428. Epub 2021 Jan 18.

Abstract

The rising demand for clean water for a growing and increasingly urban global population is one of the most urgent issues of our time. Here, we introduce the synthesis of a unique nanoscale architecture of pillar-like Co-CAT-1 metal-organic framework (MOF) crystallites on gold-coated woven stainless steel meshes with large, 50 μm apertures. These nanostructured mesh surfaces feature superhydrophilic and underwater superoleophobic wetting properties, allowing for gravity-driven, highly efficient oil-water separation featuring water fluxes of up to nearly one million L m  h . Water physisorption experiments reveal the hydrophilic nature of Co-CAT-1 with a total water vapor uptake at room temperature of 470 cm  g . Semiempirical molecular orbital calculations shed light on water affinity of the inner and outer pore surfaces. The MOF-based membranes enable high separation efficiencies for a number of liquids tested, including the notorious water pollutant, crude oil, affording chemical oxygen demand (COD) concentrations below 25 mg L of the effluent. Our results demonstrate the great impact of suitable nanoscale surface architectures as a means of encoding on-surface extreme wetting properties, yielding energy-efficient water-selective large-aperture membranes.

摘要

全球人口不断增长且日益城市化,对清洁水的需求也在上升,这是我们这个时代最紧迫的问题之一。在此,我们介绍了一种独特的纳米级结构的合成方法,即在具有50μm大孔径的镀金编织不锈钢网上合成柱状Co-CAT-1金属有机框架(MOF)微晶。这些纳米结构的网表面具有超亲水和水下超疏油的润湿特性,可实现重力驱动的高效油水分离,水通量高达近100万L m⁻² h⁻¹。水物理吸附实验揭示了Co-CAT-1的亲水性,室温下其对水蒸气的总吸附量为470 cm³ g⁻¹。半经验分子轨道计算揭示了内外孔表面的水亲和力。基于MOF的膜对多种测试液体具有高分离效率,包括臭名昭著的水污染物原油,使流出物的化学需氧量(COD)浓度低于25 mg L⁻¹。我们的结果表明,合适的纳米级表面结构作为一种编码表面极端润湿特性的手段具有重大影响,可产生节能的水选择性大孔径膜。

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