Improving Yields and Catalyst Reuse for Palmitic Acid Aromatization in the Presence of Pressurized Water

Jeffrey Page, Heather LeClerc, Philip Smolitsky, Joseph Esposito, Douglas Theberge, Azadeh Zaker, Alex Maag, Sanket Sabnis, Edward Ledford, John Coleman, Wei Fan, Siwen Wang, Jesse Bond, Bernardo Castro Dominguez, Michael Timko

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Abstract

ZSM-5 was evaluated for chemical production in a reaction mixture consisting of palmitic acid and water at conditions near the critical point of water (400 °C, 23 ± 2 MPa). Two types of ZSM-5, a microscale variety with particle diameters determined by scanning electron microscopy in the range from 1.66 to 2.56 μm (micro-ZSM-5) and a nanoscale variety with 350–730 nm diameters (nano-ZSM-5), and three water loadings (0, 15, and 65 wt %) were evaluated for their effects on conversion and product selectivity. Palmitic acid conversion and yields of one-ring aromatics, including toluene and xylenes, were greatest for the combination of nano-ZSM-5 and 15 wt % water loadings, showing that reducing particle size and optimizing water content help achieve desired reaction outcomes. Subsequently, the use of nano-ZSM-5 combined with 15 wt % water loading was studied in greater detail, finding that the catalyst could be reused up to four times at these conditions without reduction of aromatic yields and while retaining a fraction of the original acid sites. Time-resolved studies and molecular-level analysis using two-dimensional gas chromatography and isotopic resolution mass spectrometry provided information on the reaction pathway, which consists of a combination of homogeneous and heterogeneous steps. The results of this study motivate future work on water-promoted catalytic cracking of oils to produce valuable chemicals.
Original languageEnglish
Pages (from-to)5659–5673
Number of pages15
JournalACS Sustainable Chemisty and Engineering
Volume10
Issue number17
Early online date18 Apr 2022
DOIs
Publication statusPublished - 2 May 2022

Acknowledgements

Dr. Selva Pereda (PLAPIQUI-UNS-CONICE) provided useful suggestions about reaction mixture phase behavior.

Funding

Saudi Aramco provided partial funding for this study (6600023444). J.R.P., P.S., D.P.T., and J.P.E performed parts of this work in fulfillment of the degree requirements of Worcester Polytechnic Institute. The U.S. National Science Foundation (award #1605114) supported J.Q.B.’s and S.W.’s contributions to this study. H.O.L. was partially supported by the National Science Foundation GRF Program under award #2038257.

Keywords

  • BTEX
  • aromatic hydrocarbons
  • pressurized water
  • zeolites

ASJC Scopus subject areas

  • General Chemistry
  • Environmental Chemistry
  • General Chemical Engineering
  • Renewable Energy, Sustainability and the Environment

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