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

Abstract

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 providesmore » a sustainable strategy to produce biomass-derived aromatic hydrocarbons.« less

Authors:
 [1];  [1];  [2];  [3];  [4];  [5]; ORCiD logo [3];  [6]
+ Show Author Affiliations
  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)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
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
OSTI Identifier:
1783015
Grant/Contract Number:  
AC05-00OR22725; 52006106; BK2020789; 2020TQ0154; 15217878; JSBEM-S-202002
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Hazardous Materials
Additional Journal Information:
Journal Volume: 414; Journal Issue: n/a; Journal ID: ISSN 0304-3894
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalytic pyrolysis; biomass waste; plastics waste; aromatic hydrocarbons; sustainable waste management

Citation Formats

Wang, Jia, Jiang, Jianchun, Sun, Yunjuan, Meng, Xianzhi, Wang, Xiaobo, Ruan, Roger, Ragauskas, Arthur J., and Tsang, Daniel. Heterogeneous Diels–Alder tandem catalysis for converting cellulose and polyethylene into BTX. United States: N. p., 2021. Web. doi:10.1016/j.jhazmat.2021.125418.
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Wang, Jia, Jiang, Jianchun, Sun, Yunjuan, Meng, Xianzhi, Wang, Xiaobo, Ruan, Roger, Ragauskas, Arthur J., & Tsang, Daniel. Heterogeneous Diels–Alder tandem catalysis for converting cellulose and polyethylene into BTX. United States. https://doi.org/10.1016/j.jhazmat.2021.125418
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Wang, Jia, Jiang, Jianchun, Sun, Yunjuan, Meng, Xianzhi, Wang, Xiaobo, Ruan, Roger, Ragauskas, Arthur J., and Tsang, Daniel. Fri . "Heterogeneous Diels–Alder tandem catalysis for converting cellulose and polyethylene into BTX". United States. https://doi.org/10.1016/j.jhazmat.2021.125418. https://www.osti.gov/servlets/purl/1783015.
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@article{osti_1783015,
title = {Heterogeneous Diels–Alder tandem catalysis for converting cellulose and polyethylene into BTX},
author = {Wang, Jia and Jiang, Jianchun and Sun, Yunjuan and Meng, Xianzhi and Wang, Xiaobo and Ruan, Roger and Ragauskas, Arthur J. and Tsang, Daniel},
abstractNote = {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.},
doi = {10.1016/j.jhazmat.2021.125418},
journal = {Journal of Hazardous Materials},
number = n/a,
volume = 414,
place = {United States},
year = {Fri Feb 19 00:00:00 EST 2021},
month = {Fri Feb 19 00:00:00 EST 2021}
}
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https://doi.org/10.1016/j.jhazmat.2021.125418
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