Zeolite-Based Catalysts for Conversion of Oxygenated Polymer Waste by Positron Annihilation

被引:2
作者
Urban-Klaehn, Jagoda [1 ]
Shikhaliyev, Kanan [2 ]
Gaffney, Anne [1 ]
Martinez, Abraham [3 ]
Zaleski, Radoslaw [4 ]
Lauterbach, Jochen [2 ]
Katz, Aleksander [3 ]
Jaeshke, Andrew [2 ]
Li, Xuemin [3 ]
机构
[1] Idaho Natl Lab, Energy Environm S&T Directorate, Idaho Falls, ID 83415 USA
[2] Univ South Carolina, Dept Chem Engn, Columbia, SC USA
[3] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA USA
[4] Marie Curie Sklodowska Univ, Inst Phys, Lublin, Poland
基金
美国国家科学基金会;
关键词
INTRACRYSTALLINE MESOPOROSITY; Y-ZEOLITE; POROSITY; DESILICATION; GENERATION;
D O I
10.1002/cctc.202301282
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Positron Annihilation Lifetime Spectroscopy (PALS) has been employed to investigate the catalysts HZSM-5 and MESO-Y, which play a pivotal role in catalyzing and upgrading plastics, with a primary focus on oxygenated polymers, thereby transforming existing plastic materials into simpler, higher-quality value-added products. In this study, PALS was systematically compared with other complementary analytical techniques. The research outcomes have successfully demonstrated the efficacy of PALS in elucidating the morphology and topology of zeolites at micro/meso-meter scales.The first experiment focuses on H-ZSM-5 zeolite subjected to treatments involving polyurethane and polypropylene. The second experiment delves into H-ZSM-5 zeolites with varying Si/Al ratios, both before and after conversion. The third experiment investigates Y zeolites that are surfactant templated to induce meso-porosity, examining their fresh state as well as their post-conversion condition.The PALS analysis was supplemented by BET (Brunauer-Emmett-Teller) analysis and NMR (Nuclear Magnetic Resonance) spectroscopies. Notably, PALS exhibits superior sensitivity, at the sub-nanometer scale, suggesting its potential as a preferred complementary method for catalysis studies. In conclusion, the integration of PALS into the repertoire of analytical tools enhances our understanding of catalyst behavior and catalytic processes, offering valuable insights for the advancement of plastic recycling and catalysis research. Internal structure of HZSM-5 (with varying Si/Al ratios) and MESO-Y (with different NaOH concentration) before and after catalysis process was examined by several techniques. Positron Annihilation Lifetime Spectroscopy (PALS) was superior in determining micro-porous structure and morphology details for catalysts' before and after conversion. This technique relies on positron decays characteristics, longer positron time is related to more microporosity. Using PALS helps to predict the optimal catalyst type with the best selectivity for plastic upcycling.image
引用
收藏
页数:10
相关论文
共 38 条
  • [1] Modeling and simulation of trickle bed reactors for the purification of 1-butene
    Alves, Javier A.
    Colli, German Garcia
    Martinez, Osvaldo M.
    Barreto, Guillermo F.
    [J]. INTERNATIONAL JOURNAL OF CHEMICAL REACTOR ENGINEERING, 2023, 21 (09) : 1073 - 1090
  • [2] [Anonymous], 2023, NAT NANOTECHNOL, V18, P687
  • [3] Cejka J., 2010, Zeolites and Catalysis: Synthesis, Reactions and Applications
  • [4] Time-Resolved Dynamics of Intracrystalline Mesoporosity Generation in USY Zeolite
    Chawla, Aseem
    Linares, Noemi
    Rimer, Jeffrey D.
    Garcia-Martinez, Javier
    [J]. CHEMISTRY OF MATERIALS, 2019, 31 (14) : 5005 - 5013
  • [5] Chen N.Y., 1996, Molecular Transport and Reaction in Zeolites: Design and Application of Shape Selective Catalysis
  • [6] Coleman G.P., 2003, POSITRON POSITRONIUM
  • [7] From microporous to mesoporous molecular sieve materials and their use in catalysis
    Corma, A
    [J]. CHEMICAL REVIEWS, 1997, 97 (06) : 2373 - 2419
  • [8] Zeolite Y Crystals with Trimodal Porosity as Ideal Hydrocracking Catalysts
    de Jong, Krijn P.
    Zecevic, Jovana
    Friedrich, Heiner
    de Jongh, Petra E.
    Bulut, Metin
    van Donk, Sander
    Kenmogne, Regine
    Finiels, Annie
    Hulea, Vasile
    Fajula, Francois
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2010, 49 (52) : 10074 - 10078
  • [9] THE TEMPERATURE-DEPENDENCE OF POSITRON LIFETIMES IN SOLID PIVALIC ACID
    ELDRUP, M
    LIGHTBODY, D
    SHERWOOD, JN
    [J]. CHEMICAL PHYSICS, 1981, 63 (1-2) : 51 - 58
  • [10] Evidence of Intracrystalline Mesostructured Porosity in Zeolites by Advanced Gas Sorption, Electron Tomography and Rotation Electron Diffraction
    Garcia-Martinez, Javier
    Xiao, Changhong
    Cychosz, Katie A.
    Li, Kunhao
    Wan, Wei
    Zou, Xiaodong
    Thommes, Matthias
    [J]. CHEMCATCHEM, 2014, 6 (11) : 3110 - 3115