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Ultrasound-assisted synthesis and processing of carbon materials

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Title: Ultrasound-assisted synthesis and processing of carbon materials
Author(s): Fortunato, Maria E.
Director of Research: Suslick, Kenneth S.
Doctoral Committee Chair(s): Suslick, Kenneth S.
Doctoral Committee Member(s): Gewirth, Andrew A.; Scheeline, Alexander; Murphy, Catherine J.
Department / Program: Chemistry
Discipline: Chemistry
Degree Granting Institution: University of Illinois at Urbana-Champaign
Degree: Ph.D.
Genre: Dissertation
Subject(s): Porous carbon Ultrasound Spray pyrolysis Biomass Miscanthus
Abstract: Part I: Porous carbons are of interest in many applications because of their high surface areas and other physicochemical properties, and much effort has been directed towards developing new methods for controlling the porosity of carbons. Ultrasonic spray pyrolysis (USP) is an aerosol method suitable for large-scale, continuous synthesis of materials. Ultrasound is used to create aerosol droplets of a precursor solution which serve as micron-sized spherical reactors for materials synthesis. This work presents a precursor system for the template-free USP synthesis of porous carbons using low-cost precursors that do not evolve or require hazardous chemicals: sucrose was used as the carbon source, and sodium carbonate, sodium bicarbonate, or sodium nitrate was added as a decomposition catalyst and porogen. The USP carbons had macroporous interiors and microporous shells with surface areas as high as 800 m2/g and a narrow pore size distribution. It was determined that the interior porosity was a result of the gas evolution from salt decomposition and not from the presence of a salt template. Porous carbon is frequently used as a catalyst support because it provides high surface area and it is chemically and physically stable under many anoxic reaction conditions. Typically, the preparation of supported catalysts requires multiple steps for carbonization and metal impregnation. In this work, iron-impregnated porous carbon microspheres (Fe-C) were prepared by a one-step USP process by incorporating both the carbon and metal sources into the precursor solution. Carbonization, pore formation, metal impregnation, and metal activation occurred simultaneously to produce Fe-C materials with surface areas as high as 800 m2/g and up to 10 wt% Fe incorporated as nanoparticles < 20 nm in diameter. Fe-C was used as a catalyst to reduce aqueous hexavalent chromium, which demonstrated the accessibility of the iron nanoparticles despite the fact that they are likely encapsulated in the porous carbon support. Part II: The effects of high intensity ultrasound arise from acoustic cavitation: the formation, growth, and collapse of bubbles in a liquid. Bubble collapse produces intense localized heating (~5000 K), high pressures (~300 atm), and enormous heating and cooling rates (>109 K/sec). In solid-liquid slurries, surface erosion and particle fracture occur due to the shockwaves and microjets formed from asymmetric bubble collapse at extended surfaces. The chemical and physical effects of ultrasound have been studied as an adjunct to the traditional chemical pretreatment of lignocellulosic biomass for ethanol production. Lignocellulosic biomass consists of cellulose, hemicellulose, and lignin. The surface effects of ultrasound were used in this work to increase the accessibility of the cellulose, which can be converted to glucose and then fermented into ethanol. The lignocellulosic biomass used in this work was Miscanthus x giganteus (Mxg) which was grown at the University of Illinois at Urbana-Champaign. The chemical effects of NaOH pretreatment on Mxg were enhanced by ultrasound: greater delignification and a significant increase in the amount of pores >5 nm were observed. ~ 70% of the theoretical glucose yield was obtained by enzymatic saccharification of the ultrasound-assisted NaOH-pretreated Mxg; this is comparable to the yields that can be obtained by traditional alkaline pretreatments, but it was achieved in a shorter time and at a lower temperature. Because the apparatus used for laboratory studies is not a likely device for scale-up, the economics of ultrasound with regards to energy balance are not yet resolved.
Issue Date: 2011-05-25
URI: http://hdl.handle.net/2142/24304
Rights Information: Copyright 2011 Maria E. Fortunato
Date Available in IDEALS: 2011-05-25
Date Deposited: 2011-05
 

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