Upcycling Single-Use Polyethylene into High-Quality Liquid Products

被引:366
作者
Celik, Gokhan [1 ]
Kennedy, Robert M. [1 ]
Hackler, Ryan A. [1 ]
Ferrandon, Magali [1 ]
Tennakoon, Akalanka [2 ,3 ]
Patnaik, Smita [2 ,3 ]
LaPointe, Anne M. [4 ]
Ammal, Salai C. [5 ]
Heyden, Andreas [5 ]
Perras, Frederic A. [2 ]
Pruski, Marek [2 ,3 ]
Scott, Susannah L. [6 ]
Poeppelmeier, Kenneth R. [7 ]
Sadow, Aaron D. [2 ,3 ]
Delferro, Massimiliano [1 ]
机构
[1] Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
[2] US DOE, Ames Lab, Ames, IA 50011 USA
[3] Iowa State Univ, Dept Chem, Ames, IA 50011 USA
[4] Cornell Univ, Dept Chem & Chem Biol, Ithaca, NY 14583 USA
[5] Univ South Carolina, Dept Chem Engn, Columbia, SC 29208 USA
[6] Univ Calif Santa Barbara, Dept Chem Engn, Santa Barbara, CA 93106 USA
[7] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
关键词
INITIO MOLECULAR-DYNAMICS; GLOBAL ENERGY-CONSUMPTION; AB-INITIO; PLATINUM NANOPARTICLES; ACROLEIN HYDROGENATION; ETHANE HYDROGENOLYSIS; SILICA-GEL; TRANSITION; ALKANES; SURFACE;
D O I
10.1021/acscentsci.9b00722
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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 (M-n = 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 H-2 and 300 degrees 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 (D) of the final liquid product. Solid-state nuclear magnetic resonance of C-13-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.
引用
收藏
页码:1795 / 1803
页数:9
相关论文
共 57 条
  • [1] Comparing Rate and Mechanism of Ethane Hydrogenolysis on Transition-Metal Catalysts
    Almithn, Abdulrahman
    Hibbitts, David
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2019, 123 (09) : 5421 - 5432
  • [2] Effects of Catalyst Model and High Adsorbate Coverages in ab Initio Studies of Alkane Hydrogenolysis
    Almithn, Abdulrahman
    Hibbitts, David
    [J]. ACS CATALYSIS, 2018, 8 (07): : 6375 - 6387
  • [3] Pauling's rules for oxide surfaces
    Andersen, Tassie K.
    Fong, Dillon D.
    Marks, Laurence D.
    [J]. SURFACE SCIENCE REPORTS, 2018, 73 (05) : 213 - 232
  • [4] [Anonymous], 2016, EPA530R1701 US EPA
  • [5] Burange AS, 2015, GREEN CHEM, V17, P146, DOI [10.1039/C4GC01760A, 10.1039/c4gc01760a]
  • [6] RELATIONSHIP BETWEEN SELF-SEEDED AND EPITAXIAL CRYSTALLIZATION FROM POLYMER SOLUTIONS - A POTENTIALLY NEW METHOD FOR MOLECULAR WEIGHT SEPARATION AND A NEW DECORATION METHOD FOR ALKALI HALIDES
    CARR, SH
    KELLER, A
    BAER, E
    [J]. JOURNAL OF POLYMER SCIENCE PART A-2-POLYMER PHYSICS, 1970, 8 (09) : 1467 - &
  • [7] THE INFLUENCE OF PARTICLE-SIZE ON THE CATALYTIC PROPERTIES OF SUPPORTED METALS
    CHE, M
    BENNETT, CO
    [J]. ADVANCES IN CATALYSIS, 1989, 36 : 55 - 172
  • [8] THE REFLECTION ABSORPTION INFRARED-SPECTRA OF N-ALKANES ADSORBED ON PT(111)
    CHESTERS, MA
    GARDNER, P
    MCCASH, EM
    [J]. SURFACE SCIENCE, 1989, 209 (1-2) : 89 - 99
  • [9] Controlled Growth of Platinum Nanoparticles on Strontium Titanate Nanocubes by Atomic Layer Deposition
    Christensen, Steven T.
    Elam, Jeffrey W.
    Rabuffetti, Federico A.
    Ma, Qing
    Weigand, Steven J.
    Lee, Byeongdu
    Seifert, Soenke
    Stair, Peter C.
    Poeppelmeier, Kenneth R.
    Hersam, Mark C.
    Bedzyk, Michael J.
    [J]. SMALL, 2009, 5 (06) : 750 - 757
  • [10] Wulff shape of strontium titanate nanocuboids
    Crosby, Lawrence
    Enterkin, James
    Rabuffetti, Federico
    Poeppelmeier, Kenneth
    Marks, Laurence
    [J]. SURFACE SCIENCE, 2015, 632 : L22 - L25