Stratingh Institute for Chemistry, University of Groningen, Groningen, The Netherlands.
University of Graz, Institute of Systems Sciences, Innovation and Sustainability Research, Merangasse 18/I, 8010, Graz, Austria.
Nat Commun. 2022 Jun 13;13(1):3376. doi: 10.1038/s41467-022-30735-4.
Polyethylene terephthalate is one of the most abundantly used polymers, but also a significant pollutant in oceans. Due to growing environmental concerns, polyethylene terephthalate alternatives are highly sought after. Here we present readily recyclable polyethylene terephthalate analogues, made entirely from woody biomass. Central to the concept is a two-step noble metal free catalytic sequence (Cu20-PMO catalyzed reductive catalytic fractionation and Raney Ni mediated catalytic funneling) that allows for obtaining a single aliphatic diol 4-(3-hydroxypropyl) cyclohexan-1-ol in high isolated yield (11.7 wt% on lignin basis), as well as other product streams that are converted to fuels, achieving a total carbon yield of 29.5%. The diol 4-(3-hydroxypropyl) cyclohexan-1-ol is co-polymerized with methyl esters of terephthalic acid and furan dicarboxylic acid, both of which can be derived from the cellulose residues, to obtain polyesters with competitive Mw and thermal properties (T of 70-90 °C). The polymers show excellent chemical recyclability in methanol and are thus promising candidates for the circular economy.
聚对苯二甲酸乙二醇酯是使用最广泛的聚合物之一，但也是海洋中的一种重要污染物。由于环境问题日益受到关注，人们迫切需要寻找聚对苯二甲酸乙二醇酯的替代品。在这里，我们提出了一种可回收的聚对苯二甲酸乙二醇酯类似物，它完全由木质生物质制成。该概念的核心是两步非贵金属催化序列（Cu20-PMO 催化的还原催化分级和 Raney Ni 介导的催化缩合），该序列可以获得高分离产率的单一脂肪二醇 4-(3-羟丙基)环己烷-1-醇（基于木质素的 11.7wt%），以及其他转化为燃料的产物流，总碳收率达到 29.5%。二醇 4-(3-羟丙基)环己烷-1-醇与均苯三甲酸甲酯和呋喃二甲酸甲酯共聚，这两种酸甲酯都可以从纤维素残渣中得到，从而获得具有竞争力的Mw 和热性能（70-90°C 的 Tg）的聚酯。这些聚合物在甲醇中表现出优异的化学可回收性，因此是循环经济的有前途的候选材料。
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