在有机金属框架UiO-66（Zr）合成中各种聚对苯二甲酸乙二醇酯废料作为链接源的可行性,Industrial & Engineering Chemistry Research

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在有机金属框架UiO-66（Zr）合成中各种聚对苯二甲酸乙二醇酯废料作为链接源的可行性
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2019-08-20 , DOI: 10.1021/acs.iecr.9b02205
Xoliswa Dyosiba _{1,

2} , Jianwei Ren _{1,

2} , Nicholas M. Musyoka ₁ , Henrietta W. Langmi ₁ , Mkhulu Mathe ₁ , Maurice S. Onyango ₂

Affiliation

聚对苯二甲酸乙二醇酯（PET）是一种化学稳定的聚酯，具有多种用途，在过去的几十年中，其制造和消费量已急剧上升。PET使用量的增加已导致大量的废弃PET堆积起来，从而增加了对健康和环境的关注。除了垃圾填埋场和焚化解决方案，常见的废PET回收实践主要集中在低价值的下游产品上。所有上述因素都导致南非的废PET回收总利用率较低，不到30％，并产生了对替代处理方案的需求。我们的早期工作证明了将透明PET瓶转换为高附加值金属有机框架（MOF）材料的可行性。工业界的反馈表明，目前认为彩色PET瓶和食品托盘在经济地回收方面存在问题。作为响应，这项工作集中于使用各种类型的PET废料作为苯二甲酸（BDC）接头的来源，以合成基于锆的MOF UiO-66（Zr）。通过糖酵解（解聚）从食物托盘，绿色瓶，棕色瓶和PETCO珠中提取BDC接头。合成后的表征表明，废PET衍生的UiO-66（Zr）MOF的织构特性可与衍生自商业化学品的MOF的织构特性相媲美，如扫描电子显微镜图像和X射线衍射图所示。商业级BDC通常观察到的衍射图谱峰位于2θ= 17.21、25.01和27。对于PET衍生的BDC样品，观察到64°，证实了样品的结晶性质。但是，由BDC合成的MOF来源于绿色和棕色的PET瓶，其Brunauer–Emmett–Teller表面积较低，范围为933–1085 m² / g，而从商业BDC接头合成的MOF则为1368 m ² / g。这种现象归因于存在于MOF孔中的有色PET瓶中包含的有机染料的存在。消费后PET衍生的BDC的红外光谱进一步证实了这一点，该光谱显示在3158 cm ^–1处的一个峰属于胺N–H官能团，并且其═C–H弯曲更强。该研究对“废旧PET成为增值MOF”的业务案例开发模型进行了补充。

"点击查看英文标题和摘要"

Feasibility of Varied Polyethylene Terephthalate Wastes as a Linker Source in Metal–Organic Framework UiO-66(Zr) Synthesis

Polyethylene terephthalate (PET), a chemically stable polyester with multiple applications, has risen dramatically in manufacturing and consumption in the past decades. The increase in PET use has resulted in considerable volumes of waste PET pilling up and thus causing increased health and environmental concerns. Apart from the landfills and incineration solutions, the common waste PET recycling practices mainly focus on low-value downstream products. All the abovementioned factors have contributed to the lower waste PET recycling overall rate of less than 30% in South Africa and created a need for alternative treatment options. Our earlier work has proven the feasibility for converting clear PET bottles into high value-added metal–organic frameworks (MOFs) materials. The feedback from industries indicated that the colorful PET bottles and food trays are currently considered problematic to be recycled economically. In response, this work focuses on the use of various types of PET wastes as sources of benzene dicarboxylic acid (BDC) linker for the synthesis of the zirconium-based MOF UiO-66(Zr). The BDC linker was extracted from food trays, green bottles, brown bottles, and PETCO beads through glycolysis (depolymerization). Post-synthesis characterization revealed that textural properties of the waste PET-derived UiO-66(Zr) MOFs were comparable to those of the MOFs derived from commercial chemicals as exemplified in the scanning electron microscope images and X-ray diffraction patterns. The diffraction pattern peaks typically observed for commercial grade BDC positioned at 2θ = 17.21, 25.01, and 27.64° were observed for the PET-derived BDC samples, confirming the crystalline nature of samples. However, the MOFs synthesized from BDC derived from green and brown PET bottles measured lower Brunauer–Emmett–Teller surface areas in the range of 933–1085 m²/g compared to 1368 m²/g for MOFs synthesized from the commercial BDC linker. This phenomenon is attributed to the presence of organic dyes contained in the colored PET bottles residing in the MOF pores. This was further confirmed by the infrared spectra of the postconsumer PET-derived BDC showing a peak at 3158 cm^–1 assigned to the amine N–H functional group, as well as the much stronger ═C–H bend. This study complements the business case development model of “waste PET to value-added MOFs”.

更新日期：2019-08-20

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