Nelson Taylor F, Rothauer Dario, Sander Michael, Mecking Stefan
Department of Chemistry, University of Konstanz, Universitätstrasse 10, 78457, Konstanz, Germany.
Institute of Biogeochemistry and Pollutant Dynamics, ETH Zurich, Universitätstrasse 16, 8092, Zurich, Switzerland.
Angew Chem Int Ed Engl. 2023 Oct 23;62(43):e202310729. doi: 10.1002/anie.202310729. Epub 2023 Sep 19.
Monomers sourced from waste or biomass are often mixtures of different chain lengths; e.g. catalytic oxidation of polyethylene waste yields mixtures of dicarboxylic acids (DCAs). Yet, polyesters synthesized from such monomer mixtures have rarely been studied. We report polyesters based on multiple linear aliphatic DCAs, present in chain length distributions that vary in their centers and ranges. We demonstrate that these materials can adopt high-density polyethylene-like solid state structures, and are ductile (e.g. E 610 MPa), allowing for injection molding, or film and fiber extrusion. Melting and crystallization points of the polyesters show no odd-even effects as dipoles cannot favorably align in the crystal, similar to traditional odd carbon numbered, long-chain DCA polyesters. Biodegradation studies of C-labelled polyesters in soil reveal rapid mineralization, and depolymerization by methanolysis indicates suitability for closed-loop recycling.
源自废物或生物质的单体通常是不同链长的混合物;例如,聚乙烯废料的催化氧化会产生二元羧酸(DCA)的混合物。然而,由这种单体混合物合成的聚酯很少被研究。我们报道了基于多种线性脂肪族DCA的聚酯,这些DCA存在于中心和范围各不相同的链长分布中。我们证明这些材料可以呈现高密度聚乙烯样的固态结构,并且具有延展性(例如E = 610 MPa),可用于注塑成型、薄膜和纤维挤出。聚酯的熔点和结晶点没有奇偶效应,因为偶极子在晶体中无法良好排列,这与传统的奇数碳数长链DCA聚酯类似。对土壤中含¹⁴C标记聚酯的生物降解研究表明其能快速矿化,甲醇解解聚表明其适合闭环回收利用。