Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Heterogeneous Diels–Alder tandem catalysis for converting cellulose and polyethylene into BTX

Journal Article · · Journal of Hazardous Materials
 [1];  [1];  [2];  [3];  [4];  [5];  [3];  [6]
  1. Nanjing Forestry Univ. (China); Chinese Academy of Forestry (CAF), Nanjing (China)
  2. Chinese Academy of Forestry (CAF), Nanjing (China)
  3. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Nanjing Xiaozhuang Univ. (China)
  5. Univ. of Minnesota, St. Paul, MN (United States)
  6. The Hong Kong Polytechnic Univ. (China)

Producing biomass-derived aromatic hydrocarbons via controllable Diels–Alder reactions is a promising approach to recover energy and chemicals from waste streams. A tandem Diels–Alder catalysis consisting of SAPO-34 and Fe/HZSM-5 (stacked catalysis or mixed catalysis) was evaluated for thermochemical conversion of cellulose and polyethylene blends into benzene, toluene, and xylenes (BTX). Aromatization catalyst type significantly affected the activity of tandem catalysis, and the BTX obtained from the HZSM-5 stacked catalysis was ~2.3 times higher than that of the USY stacked one. An introduction of Fe active promoters into HZSM-5 increased the Lewis to Brønsted acid sites molar ratio (L/B) from 0.4 to 4.1. The comparison between Fe/HZSM-5 stacked catalysis and parent HZSM-5 single catalysis indicated that the former was more effective for BTX production, obtaining a nearly two-fold increase in yield with a high selectivity of 82.8%. A close proximity between Fe/HZSM-5 and SAPO-34 in the mixed catalysis increased the BTX enhancement to 1.8. A synergistic effect was provided by the coordination of Lewis and Brønsted acid sites in the Fe/HZSM-5 mixed catalysts for facilitating BTX generation, achieving a maximum of 25.9% at a Fe/HZSM-5 to SAPO-34 mass ratio of 1:1 with a theoretical L/B of 7.2. Finally, this work provides a sustainable strategy to produce biomass-derived aromatic hydrocarbons.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE; National Natural Science Foundation of China (NSFC); Natural Science Foundation of Jiangsu Province; China Postdoctoral Science Foundation; Hong Kong Research Grants Council; Jiangsu Province Key Laboratory of Biomass Energy and Materials
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1783015
Journal Information:
Journal of Hazardous Materials, Journal Name: Journal of Hazardous Materials Journal Issue: n/a Vol. 414; ISSN 0304-3894
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (46)

?Designer Acids?: Combined Acid Catalysis for Asymmetric Synthesis journal March 2005
Production of p -Xylene from Biomass by Catalytic Fast Pyrolysis Using ZSM-5 Catalysts with Reduced Pore Openings journal October 2012
From Biomass-Derived Furans to Aromatics with Ethanol over Zeolite journal October 2016
Tandem Diels-Alder Reaction of Dimethylfuran and Ethylene and Dehydration to para -Xylene Catalyzed by Zeotypic Lewis Acids journal May 2017
Catalytic degradation of high-density polyethylene over SAPO-34 synthesized with various templates journal August 2010
Hydrogen and Carbon Nanotubes from Pyrolysis-Catalysis of Waste Plastics: A Review journal April 2020
Pyrolysis of waste tyres with zeolite USY and ZSM-5 catalysts journal April 2007
Catalytic pyrolysis of crude glycerol over shaped ZSM-5/bentonite catalysts for bio-BTX synthesis journal November 2018
Co-precipitation, impregnation and so-gel preparation of Ni catalysts for pyrolysis-catalytic steam reforming of waste plastics journal December 2018
Catalytic co-pyrolysis of yellow poplar wood and polyethylene terephthalate over two stage calcium oxide-ZSM-5 journal September 2019
Comparative investigation of rice husk, thermoplastic bituminous coal and their blends in production of value-added gaseous and liquid products during hydropyrolysis/co-hydropyrolysis journal November 2018
Catalytic fast pyrolysis of wood plastic composite over microporous zeolites journal December 2019
Co-feeding effect of waste plastic films on the catalytic pyrolysis of Quercus variabilis over microporous HZSM-5 and HY catalysts journal December 2019
Catalytic conversion of rubber wastes to produce aromatic hydrocarbons over USY zeolites: Effect of SiO2/Al2O3 mole ratio journal October 2019
Recycling benzene and ethylbenzene from in-situ catalytic fast pyrolysis of plastic wastes journal November 2019
Characteristics of the catalytic fast pyrolysis of vegetable oil soapstock for hydrocarbon-rich fuel journal June 2020
Production of renewable toluene from biomass-derived furans via Diels-Alder and dehydration reactions: A comparative study of Lewis acid catalysts journal October 2016
Effect of iron loading on acidity and performance of Fe/HZSM-5 catalyst for direct synthesis of aromatics from syngas journal September 2018
Tuning the acidity and reducibility of Fe/ZSM-5 catalysts for methane dehydroaromatization journal January 2019
Enhanced BTEX formation via catalytic fast pyrolysis of styrene-butadiene rubber: Comparison of different catalysts journal October 2020
Improvement of aromatics production from catalytic pyrolysis of cellulose over metal-modified hierarchical HZSM-5 journal October 2018
Catalytic fast pyrolysis of cellulose over Ce0.8Zr0.2-xAlxO2 catalysts to produce aromatic hydrocarbons: Analytical Py-GC × GC/MS journal August 2020
Catalytic fast pyrolysis of cellulose to produce furan compounds with SAPO type catalysts journal January 2018
Mechanism study of aromatics production from furans with methanol over zeolite catalysts journal May 2019
A combo Zr-HY and Al-HY zeolite catalysts for the one-pot cascade transformation of biomass-derived furfural to γ-valerolactone journal July 2019
Environmental impact assessment of converting flexible packaging plastic waste to pyrolysis oil and multi-walled carbon nanotubes journal May 2020
Converting polycarbonate and polystyrene plastic wastes intoaromatic hydrocarbons via catalytic fast co-pyrolysis journal March 2020
Reduction of polycyclic compounds and biphenyls generated by pyrolysis of industrial plastic waste by using supported metal catalysts: A case study of polyethylene terephthalate treatment journal June 2020
Catalytic Pyrolysis of Polystyrene over Steel Slag under CO2 Environment journal August 2020
Different reaction behaviours of light or heavy density polyethylene during the pyrolysis with biochar as the catalyst journal November 2020
Pyrolysis dynamics of two medical plastic wastes: Drivers, behaviors, evolved gases, reaction mechanisms, and pathways journal January 2021
Microwave-assisted catalytic pyrolysis of waste printed circuit boards, and migration and distribution of bromine journal January 2021
Pyrolysis-catalytic upgrading of brominated high impact polystyrene over Fe and Ni modified catalysts: Influence of HZSM-5 and MCM-41 catalysts journal December 2017
Enhanced Methanol to Olefin Catalysis by Physical Mixtures of SAPO-34 Molecular Sieve and MgO journal July 2017
Selective Production of Aromatics by Catalytic Fast Pyrolysis of Furan with In Situ Dehydrogenation of Propane journal February 2019
Co-Aromatization of Furan and Methanol over ZSM-5—A Pathway to Bio-Aromatics journal August 2019
Tuning Hydrocarbon Pool Intermediates by the Acidity of SAPO-34 Catalysts for Improving Methanol-to-Olefins Reaction journal November 2018
Chemistry of Furan Conversion into Aromatics and Olefins over HZSM-5: A Model Biomass Conversion Reaction journal May 2011
On the Way to Biofuels from Furan: Discriminating Diels–Alder and Ring-Opening Mechanisms journal August 2013
Aromatic hydrocarbon production by catalytic pyrolysis of palm kernel shell waste using a bifunctional Fe/HBeta catalyst: effect of lignin-derived phenolics on zeolite deactivation journal January 2016
Lewis acid zeolites for tandem Diels–Alder cycloaddition and dehydration of biomass-derived dimethylfuran and ethylene to renewable p-xylene journal January 2016
Heterogeneous Diels–Alder catalysis for biomass-derived aromatic compounds journal January 2017
Catalytic conversion of furanic compounds over Ga-modified ZSM-5 zeolites as a route to biomass-derived aromatics journal January 2018
Recent advances in the selective catalytic hydrodeoxygenation of lignin-derived oxygenates to arenes journal January 2020
Tandem catalytic aromatization of volatile fatty acids journal January 2020
Production of targeted aromatics by using Diels–Alder classes of reactions with furans and olefins over ZSM-5 journal January 2012