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Mechanistic Modeling of Increased Oxygen Transport Using Functionalized Magnetic Fluids in Bioreactors

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Mechanistic Modeling of Increased Oxygen Transport Using Functionalized Magnetic Fluids in Bioreactors Mechanistic Modeling of Increased Oxygen Transport Using Functionalized Magnetic Fluids in Bioreactors by Bernat Ollé Pocurull M.S.C.E.P., Massachusetts Institute of Technology, Cambridge, MA (2005) B.Eng. Chemical Engineering, Escola Tècnica Superior d’Enginyeria Química, Universitat Rovira i Virgili, Tarragona, Spain (2002) Submitted to the Department of Chemical Engineering In partial fulfillment of the requirements for the degree of Doctor of Philosophy in Chemical Engineering Practice at the MASSACHUSETTS INSTITUTE OF TECHNOLOGY May 2007 © 2007 Massachusetts Institute of Technology. All Rights Reserved. Author:_________________________________________________________________ Department of Chemical Engineering May 2007 Certified by: ____________________________________________________________ Daniel I. C. Wang Institute Professor Thesis Supervisor Certified by:_____________________________________________________________ T. Alan Hatton Ralph Landau Professor Thesis Supervisor Accepted by:_____________________________________________________________ William M. Deen Professor of Chemical Engineering Chairman, Committee for Graduate Students 2 Mechanistic Modeling of Increased Oxygen Transport Using Functionalized Magnetic Fluids in Bioreactors by Bernat Ollé Pocurull Submitted to the Department of Chemical Engineering on August 28, 2006 In partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy in Chemical Engineering Practice ABSTRACT Absorption of gases into a liquid is of crucial importance to multiphase reactions because diffusion of a sparingly soluble gas across a gas-liquid interface generally limits the relevant reaction rates. Pertinent examples of multiphase reactions that have found application in the chemical and biochemical industries include fermentation, water treatment, and hydrogenation reactions. Gas-liquid mass transfer is of particular importance in fermentation because productivity increases in aerobic cultures are often constrained by transport of oxygen, which is only slightly soluble in water. Previous approaches to enhance oxygen transfer consisted in adding emulsified organic phases in which oxygen has a greater solubility. However, these approaches have several limitations, the most important of which is the difficult recovery of the organic phase after the fermentation. The research presented in this thesis focuses on the use of functionalized magnetic nanoparticles to enhance gas-liquid oxygen transfer. The nanoparticles have a magnetic core and an organic coating. The magnetic core makes it possible to easily recover the fluid by passing it through a magnetic field, and the coating confers colloidal stability to the particle. Oxygen transfer enhancement has been observed in the presence of nanoparticles coated with oleic acid and a polymerizable surfactant. In cell-free media, nanoparticles improve gas-liquid oxygen mass transfer up to 6-fold (600%) in an agitated, sparged reactor. Furthermore, they show remarkable stability in high-ionic strength media over a wide pH range. In a fermentation of Escherichia coli, a nanoparticle weight fraction of 0.6% increases oxygen uptake rate and cell growth by 40%. Through a combination of experiments using both physical and chemical methods to characterize mass transfer, it has been shown that both the mass transfer coefficient (kL) and the gas-liquid interfacial area are enhanced in the presence of nanoparticles, the latter accounting for a larger fraction of the total enhancement. This insight has been used to propose a model of the enhancement that involves two separate mechanisms: one of area enhancement and the other of kL enhancement. It has been proposed that (i) the nanoparticles increase interfacial area by adsorbing on the gas bubble interface and stabilizing it against coalescence and (ii) the nanoparticles increase the mass transfer coefficient by causing microconvection in the surrounding fluid through Brownian motion. 3 The methodology developed in this thesis shows several-fold gas-liquid mass transfer enhancements and at the same time allows for easier separation over previous approaches. In addition, the modeling effort resulted in correlations that can allow for extension of this methodology from laboratory-scale to industrial scale reactions across the variable space considered Thesis Supervisor: T. Alan Hatton Title: Ralph Landau Professor of Chemical Engineering Practice Thesis Supervisor: Daniel I. C. Wang Title: Institute Professor 4 ACKNOWLEDGEMENTS For some reason parents usually come last but not least in doctoral thesis acknowledgements but in my case they have been so instrumental in my education that any place other than first does not do them justice. They come first for devoting so much time to the upbringing of my brother Linus and me, first for understanding and embracing my choice to come to the US, and first for supporting me through it. For some other reason, acknowledgements to the thesis advisors tend to follow a certain template of generalities, so I will try to be as specific as I possibly can with mine. I have been fortunate to be co-advised by two unique individuals, and benefited from the best of both. I thank Danny Wang for setting my priorities straight and time and again making his decisions regarding my thesis based uniquely on what was best for me. I also thank him for his straight-talking and straight-questioning that has shown me a good way in science and life: being modest, being honest, and this too, being right –or otherwise shut up. And I thank him for setting a demanding standard for my work; never during the thesis have I had the impression of even coming close to meeting this standard but it has been a worthy goal to strive for. I am sure that with years I will look through his toughness and see a man that shaped my personality in more ways than I can appreciate now. I thank Alan Hatton above all for making the journey a fun experience. Not truly having set my heart on a specific field of research before I came to MIT, I had the privilege to choose a person to work for, rather than a field to work in. My first conversation with Alan was in late October 2002. It is hard to say what unconscious factors go into the decisions we think are rational, but I estimate that somewhere between the first and second minute in Alan’s office I made up my mind to work for him. So I could have left at that point but I stayed and nodded for the following half hour instead. I cannot stress enough how essential Alan has been in making my MIT experience something exceptional. He provided me with two unique opportunities overseas for personal growth through the Practice School in Japan and in Singapore. His welcoming smile whenever I crossed his office doorstep has fueled my will to work during the hard times. I thank the members of my thesis committee, professors Ken Smith, Greg Stephanopoulos and Bernhardt Trout, for helpful insight during the thesis, and Susan Lanza for keeping the committee meetings running smooth and giving a social life to the Wang group. I am indebted to George Morrow III, the Dupont-MIT Alliance, and the“la Caixa” Foundation for funding, and to several graduate students, undergraduate students, and post-docs, for their contributions to my work, but to Andre Ditsch more than anyone else. Andre provided helpful advice in virtually every aspect of my thesis, but above all, was a good role model to follow. Lev Bromberg developed the synthesis procedure for the nanoparticles I used in my work. Jin Yin and Bill Perry taught me the experimental techniques for fermentation, and Brad Ciccarelli the technique for surface tension measurement. Evita Grant, as a UROP, and Tracy Holmes, as a BPEC-REU student, also contributed to this work. Fred Ngantung had the patience to listen to the miseries and triumphs of my thesis, and I was glad to listen to his in exchange. 5 I am grateful to Professor Bob Cohen for pioneering the PhDCEP program. I knew it was the right program for me the first time I read about it and this is what brought me to MIT. I hope the future accomplishments of the students in the program will prove Bob (and the rest of ChemE professors that believed in the program) right. My MIT experience would not have been the same without Practice School; and Practice School would not have been the same without the company of classmate and travel mate Pete Colvin. It would not have been the same if we had not had a flat tire in a bike in the middle of the Kibi rice plains in Japan, miles from the closest village and without a patch kit. It would not have been the same without the strenuous badminton games at 40oC against the Japanese employees at Mitsubishi either. Undoubtedly the best memories I will take with me from MIT are from the friends I have made. I thank Joel Moxley for organizing course 10.24, a.k.a. American Adolescent Studies Program, designed to give me (the Spaniard) an exposure to the high points of growing up in the U.S. in the 80s and 90s. This included watching the likes of Office Space, Caddyshack, and the final of the Super Bowl, while eating pizza. This course has been an essential part of my integration to the United States –seriously– and I cannot be thankful enough. One day Joel will be a big shot wherever he goes, and I shall be telling this with a sigh. Gregg –with two g’s– Beckham, was my first friend at MIT, the one who put his arm around my shoulder to show me how that first 10.40 problem set wasn’t that hard after all. Gregg proofread my thesis and papers with laser precision. Jose Aleman was my treasured Spanish speaking connection at MIT. Joe Shuga, long-time lab mate, was a supporting comrade at work and a worthy companion for long runs around the Charles River. My favorite couple, fine-looking, eloquent Kris Wood, and beautiful and talented Jane Rempel, made sure I got out of the lab on Friday evenings and shared many great times.
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