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Upcycling Single-Use Polyethylene into High-Quality Liquid Products
ACS Central Science ( IF 18.2 ) Pub Date : 2019-10-23 , DOI: 10.1021/acscentsci.9b00722
Gokhan Celik 1 , Robert M. Kennedy 1 , Ryan A. Hackler 1 , Magali Ferrandon 1 , Akalanka Tennakoon 2, 3 , Smita Patnaik 2, 3 , Anne M. LaPointe 4 , Salai C. Ammal 5 , Andreas Heyden 5 , Frédéric A. Perras 2 , Marek Pruski 2, 3 , Susannah L. Scott 6 , Kenneth R. Poeppelmeier 7 , Aaron D. Sadow 2, 3 , Massimiliano Delferro 1
Affiliation  

Our civilization relies on synthetic polymers for all aspects of modern life; yet, inefficient recycling and extremely slow environmental degradation of plastics are causing increasing concern about their widespread use. After a single use, many of these materials are currently treated as waste, underutilizing their inherent chemical and energy value. In this study, energy-rich polyethylene (PE) macromolecules are catalytically transformed into value-added products by hydrogenolysis using well-dispersed Pt nanoparticles (NPs) supported on SrTiO3 perovskite nanocuboids by atomic layer deposition. Pt/SrTiO3 completely converts PE (Mn = 8000–158,000 Da) or a single-use plastic bag (Mn = 31,000 Da) into high-quality liquid products, such as lubricants and waxes, characterized by a narrow distribution of oligomeric chains, at 170 psi H2 and 300 °C under solvent-free conditions for reaction durations up to 96 h. The binding of PE onto the catalyst surface contributes to the number averaged molecular weight (Mn) and the narrow polydispersity (Đ) of the final liquid product. Solid-state nuclear magnetic resonance of 13C-enriched PE adsorption studies and density functional theory computations suggest that PE adsorption is more favorable on Pt sites than that on the SrTiO3 support. Smaller Pt NPs with higher concentrations of undercoordinated Pt sites over-hydrogenolyzed PE to undesired light hydrocarbons.

中文翻译:

将一次性聚乙烯升级为优质液体产品

我们的文明在现代生活的各个方面都依赖合成聚合物。然而,塑料的低效回收利用和极其缓慢的环境退化正在引起人们对其广泛使用的关注。一次使用后,许多此类材料目前都被当作废物,利用不到其固有的化学和能量价值。在这项研究中,富集能量的聚乙烯(PE)大分子通过氢解反应被催化水解为增值产品,该分散作用是通过原子层沉积将SrTiO 3钙钛矿纳米立方体支撑在分散良好的Pt纳米颗粒(NPs)上进行的。Pt / SrTiO 3完全转化为PE(M n = 8000–158,000 Da)或一次性塑料袋(M n= 31,000 Da)到高质量的液体产品中,例如润滑剂和蜡,其特征是低聚物链分布窄,在170 psi H 2和300°C的无溶剂条件下,反应时间长达96小时。PE的在催化剂表面有助于数目的结合均分子量(中号Ñ)和窄的多分散(Đ最终液体产物)。13 C富集PE吸附的固态核磁共振研究和密度泛函理论计算表明,Pt位上的PE吸附比SrTiO 3上的PE吸附更有利支持。较小的Pt NP和较高浓度的Pt配位不足的位置会过度水解,从而使PE过度生成不希望的轻烃。
更新日期:2019-11-28
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