TY - JOUR
T1 - Improving Yields and Catalyst Reuse for Palmitic Acid Aromatization in the Presence of Pressurized Water
AU - Page, Jeffrey
AU - LeClerc, Heather
AU - Smolitsky, Philip
AU - Esposito, Joseph
AU - Theberge, Douglas
AU - Zaker, Azadeh
AU - Maag, Alex
AU - Sabnis, Sanket
AU - Ledford, Edward
AU - Coleman, John
AU - Fan, Wei
AU - Wang, Siwen
AU - Bond, Jesse
AU - Castro Dominguez, Bernardo
AU - Timko, Michael
N1 - Funding Information:
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. Dr. Selva Pereda (PLAPIQUI-UNS-CONICE) provided useful suggestions about reaction mixture phase behavior.
Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/5/2
Y1 - 2022/5/2
N2 - 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.
AB - 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.
KW - BTEX
KW - aromatic hydrocarbons
KW - pressurized water
KW - zeolites
UR - http://www.scopus.com/inward/record.url?scp=85128826256&partnerID=8YFLogxK
U2 - 10.1021/acssuschemeng.2c00665
DO - 10.1021/acssuschemeng.2c00665
M3 - Article
VL - 10
SP - 5659
EP - 5673
JO - ACS Sustainable Chemisty and Engineering
JF - ACS Sustainable Chemisty and Engineering
SN - 2168-0485
IS - 17
ER -