Award Abstract # 2338497
CAREER: Engineering Circular Hydrocarbon Reactions in Zeolite-based Catalysts

NSF Org: CBET
Division of Chemical, Bioengineering, Environmental, and Transport Systems
Recipient: THE TRUSTEES OF PRINCETON UNIVERSITY
Initial Amendment Date: January 25, 2024
Latest Amendment Date: January 25, 2024
Award Number: 2338497
Award Instrument: Continuing Grant
Program Manager: Bert Chandler
bchandle@nsf.gov
 (703)292-7104
CBET
 Division of Chemical, Bioengineering, Environmental, and Transport Systems
ENG
 Directorate for Engineering
Start Date: February 1, 2024
End Date: January 31, 2029 (Estimated)
Total Intended Award Amount: $575,337.00
Total Awarded Amount to Date: $460,965.00
Funds Obligated to Date: FY 2024 = $460,965.00
History of Investigator:
  • Michele Sarazen (Principal Investigator)
Recipient Sponsored Research Office: Princeton University
1 NASSAU HALL
PRINCETON
NJ  US  08544-2001
(609)258-3090
Sponsor Congressional District: 12
Primary Place of Performance: Princeton University
Engineering Quadrangle A319
PRINCETON
NJ  US  08544-2001
Primary Place of Performance
Congressional District:
12
Unique Entity Identifier (UEI): NJ1YPQXQG7U5
Parent UEI:
NSF Program(s): Catalysis
Primary Program Source: 01002425DB NSF RESEARCH & RELATED ACTIVIT
01002526DB NSF RESEARCH & RELATED ACTIVIT
Program Reference Code(s): 1045
Program Element Code(s): 140100
Award Agency Code: 4900
Fund Agency Code: 4900
Assistance Listing Number(s): 47.041

ABSTRACT

Chemical processes that breakdown plastic waste and remanufacture the deconstructed products to valuable fuels and chemicals are attractive alternatives to fossil-fuels for hard-to-decarbonize sectors such as aviation fuels. Such plastic upcycling is especially valuable when it can be achieved at moderate temperatures in energy efficient processes. Catalysts offer a route to that end by lowering reaction temperature and selectively directing conversion of plastic to products that serve as building blocks for a broad range of fuels, consumer goods, pharmaceuticals, and building materials, to name a few. Zeolites are a class of porous crystalline catalysts that are especially suitable for waste plastic deconstruction, but further research and development is needed to improve their efficiency, product selectivity, and durability. Thus, this project investigates key design factors that affect the overall effectiveness of zeolite catalysts for the breakdown of a prevalent class of waste plastic, polyolefins. The project is supported by integrated educational and outreach activities aimed primarily at undergraduate and graduate students.

While catalysts are ubiquitous in the production of fuels and important chemical intermediates, the design of advanced catalysts that possess high reactivity, selectivity, and stability remains paramount for efficiently and sustainably abating pollution while lowering energy demands and decreasing carbon emissions. Here, this rational design is employed in the hydrocracking of polyolefins using bifunctional metal/zeolite catalysts, where zeolitic voids simultaneously provide high reactivity and tailored selectivity, but limit catalyst efficiency and stability due to diffusional constraints of bulky products. Hierarchical zeolites with hybrid pore structures can be utilized to address this inaccessibility of bulky polymer molecules, but the direct effect on reaction and deactivation mechanisms, especially of these complex multiphase systems is not well-established. The project thus aims to engineer hierarchical (bifunctional) zeolites in selective hydrocracking of waste polyolefins, based on hypotheses that enhancements of hierarchical structuring affect reaction and deactivation rates for polyolefin cracking beyond simple diffusional impacts and include effects of pore structure (i.e., zeolite framework), connectivity, communication (metal:acid balance/proximity) and reactions occurring within the mesoporous regions and surface protons. By combining synthetic protocols with detailed reaction pathway and deactivation analysis, the project will reveal new insights on how shape-selectivity and transport phenomena affect the performance of these hierarchical, bifunctional catalysts for transformation of waste polyolefins into useful products. Those insights will aid in understanding the entire catalytic lifecycle, including specific mechanistic details that can be extended to improve catalyst efficiency for reactions of various feedstocks related to hydrocarbon and oxygenate processing (i.e., biomass, renewable alcohols, or CO2) and different zeolite or zeotype architectures. Research results from this award will be proactively incorporated into an undergraduate elective entitled Green and Catalytic Chemistry that will incorporate interactive components like hands-on catalysis (plastic upcycling and aqueous pollutant degradation) and separation (CO2 capture) experiments, and ?Sustainability Spotlights? based on media articles covering energy and climate related topics. The project will also strengthen the broader catalysis community through ?CatChats? for younger graduate students in catalysis labs at various universities. These meetups will create a supportive network of peers, via initial virtual connections that will be expanded at conferences, workshops, and other in-person venues.

This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

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