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ATTACHMENT, SELECTION, and TRANSFORMATION of PREBIOTIC MOLECULES on BRUCITE [Mg(OH)2]

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ATTACHMENT, SELECTION, and TRANSFORMATION of PREBIOTIC MOLECULES on BRUCITE [Mg(OH)2] ATTACHMENT, SELECTION, AND TRANSFORMATION OF PREBIOTIC MOLECULES ON BRUCITE [Mg(OH)2] AND THE IMPLICATIONS FOR CHEMICAL EVOLUTION AT HYDROTHERMAL SYSTEMS by Charlene F. Estrada A dissertation submitted to The Johns Hopkins University in conformity with the requirements for the degree of Doctor of Philosophy Baltimore, Maryland September, 2014 Charlene F. Estrada All rights reserved Abstract Serpentinite-hosted hydrothermal vents may have been plausible environments for the origins of life. Mineral assemblages within hydrothermal fields may have selected and concentrated biomolecules, although little is known about molecular interactions at these mineral surfaces. I investigated the adsorption of aspartate and ribose at the surface of brucite [Mg(OH)2], a major mineral phase at serpentinite-hosted hydrothermal vents. I characterized the attachment of these molecules onto a synthetic brucite powder with Mg2+ and Ca2+ using batch adsorption experiments. I observed that Mg2+ inhibits both aspartate and ribose adsorption, whereas Ca2+ enhances adsorption onto the brucite surface. I used surface complexation modeling to predict that both aspartate and ribose attach as cooperative calcium-ligand complexes onto brucite. To further investigate the cooperative effect of Ca2+ on biomolecule adsorption, I introduced an equimolar mixture of aspartate, glycine, lysine, leucine, and phenylalanine to the brucite surface, both with and without Ca2+. Without Ca2+, up to 8.9 % aspartate and ~5 % each of the remaining four amino acids adsorbed onto brucite. When Ca2+ was added, I observed that between 5.7 to 20 times more aspartate (37.3 %) adsorbed onto brucite compared with the remaining four amino acids (~3 % each). These results, when combined with the previous study, suggest that aspartate selectively adsorbs onto brucite as a cooperative calcium-aspartate complex. The behavior of biomolecules at high temperatures is essential for evaluating whether hydrothermal systems may have been suitable environments for life’s origins. ii However, the geochemical complexities of a hydrothermal system could significantly affect this process. I characterized aspartate decomposition at 200 ºC and 15.5 bars for 24 hours in inert gold capsules with controlled redox state, added ammonia, and brucite. I determined that the initial experimental conditions significantly affect the decomposition of aspartate. Biomolecule decomposition may be a more complicated process within hydrothermal systems, which may contribute a diverse array of organic species to early Earth. First reader (thesis advisor): Dimitri A. Sverjensky Second reader: Robert M. Hazen iii Acknowledgments This work has been possible with the gracious help and support of many individuals at the Johns Hopkins University Department of Earth and Planetary Sciences and the Geophysical Laboratory at the Carnegie Institution of Washington. I particularly thank my thesis advisor, Dr. Dimitri Sverjensky whose guidance, patience, and overwhelming support in every area of this work has made my experience during this Ph. D. program both pleasant and exciting. Dimitri challenged the limits of what I expected I could do while simultaneously encouraging me that I could achieve almost anything. He has made me a stronger person and scientist, and I will always be grateful. I also thank Dr. Bob Hazen, my supervisor at the Geophysical Laboratory. Bob’s unwavering enthusiasm for science is contagious, and I always look forward to our discussions. His mentorship has been invaluable, and I feel inspired to continue my scientific career with the optimism, passion, and determination that he has imparted to me. Over the three years that I have worked at the Geophysical Laboratory, I have come to think of my colleagues at the Carnegie Institution of Washington as my second family. My experience at the Geophysical Laboratory has been one of the happiest times of my life. I particularly thank Drs. George Cody, Dionysis Foustoukos, Irena Mamajanov, Chris Glein, John Armstrong, Paul Goldey, and Tim Strobel who have taken time from their own schedules to help me with my experiments. I also thank Drs. Andrew Steele, Bjørn Mysen, Karen Rogers, Jim Cleaves, and the Carnegie Institution of Washington Support Staff for their invaluable discussions and support during this work. iv I am also grateful to the professors and staff at Johns Hopkins University who have encouraged me from the first day I began my Ph.D. program. In particular, I thank Drs. Alan Stone, Colin Norman, John Ferry, Ben Passey, and Bill Ball, who served as members on my committee. I also thank Drs. Naomi Levin, Ken Livi, Jocelyne DiRuggiero, and Tom Wright for their kind advice. I am also indebted to my current and former research group members both at the Department of Earth and Planetary Sciences and the Geophysical Laboratory for their animated discussion and advice regarding my experimental techniques, results, and theoretical predictions. I specifically thank Namhey Lee, Alyssa Adcock, Clare Flynn, Patrick Griffin, David Azzolini, Branden Harrison, Jihua Hao, Fang Huang, Katya Klochko, Adrian Villegas-Jimenez, Xiaoming Liu, and Cécile Feuillie. I also thank Caroline and Christopher Jonsson who, as my first mentors at the Geophysical Laboratory, taught me how to conduct most of the experiments presented in this work. I am unimaginably grateful for their hard work in teaching me, and their work with me has been an inspiration over these past five years. I am extremely grateful to my friend and colleague Dr. Bob Downs who was my first mentor in science. I believe that much of my success today is a result of his mentorship. If I had not walked into his office that day at the University of Arizona, my journey in science would have never been the same. My experience at the Carnegie Institution and JHU are direct results of my work with Bob Downs, and I hope that one day I can pay forward the kindness he has shown me by becoming the same type of mentor. v I thank my friends for making me a better and stranger person. I’m grateful to Jen McAlonan, Brian Olnick, Kelsey Wright, Corinne Warren, and Will Genschow. I also thank my best friend, my cat Rio, who has eaten my physical chemistry homework, sat on my laptop as I wrote these chapters, and purred in my ear (yes, my ear) as I practiced my thesis presentation. Throughout my time in this Ph.D. program, he has kept me sane, and acted as a not-so-subtle reminder that there is more to life than work. Most importantly, I thank my family for helping me every step of the way in this endeavor. I especially thank my parents, Antonio and Barbara Estrada, for their unwavering support of everything I have done. I thank my brother, Eric and his wonderful growing family, and my sister, Gloria. I thank my grandmother, Shirley Polk. I am also grateful to my grandparents, Sharon and Don Ridlen, and my mother, Janis Ridlen, who are all missed. This thesis is dedicated my family for everything they have done to make me who I am today. I love you all! All of the chapters included in this thesis were a collaborative effort. The contributions of those who have made each chapter possible are listed below. Chapter 2 This chapter was co-authored with Dimitri Sverjensky, Manuel Pelletier, Angélina Razafitianamaharavo, and Robert Hazen. In our adsorption studies, we suspected that aspartate was adsorbing onto the edge surfaces of brucite. Drs. Manuel Pelletier and Angélina Razafitianamaharavo at the Université de Lorraine measured the specific edge surface area of our synthetic brucite powder with a novel low-pressure Ar adsorption method. This enabled us to calculate the amount of aspartate adsorption per m2 of brucite. I am also grateful to Cécile Feuillie, Namhey Lee, Alyssa Adcock, Adrian vi Villegas-Jimenez, John Armstrong, Paul Goldey, Tim Strobel, Stephen Hodge, and Steven Coley for their supportive discussions and assistance in the laboratory. Chapter 3 This chapter was co-authored with Alyssa Adcock, Dimitri Sverjensky, Manuel Pelletier, Angélina Razafitianamaharavo, and Robert Hazen. As a summer intern at the Geophysical Laboratory, Alyssa conducted nearly half of the ribose adsorption experiments. Alyssa’s tremendous amount of work in a short amount of time became the foundation for this chapter. I am also grateful to Cécile Feuillie, Namhey Lee, George Cody, Adrian Villegas-Jimenez, John Armstrong, Paul Goldey, Tim Strobel, Stephen Hodge, and Steven Coley for their supportive discussions and assistance in the laboratory. Chapter 5 This chapter was co-authored with Irena Mamajanov, Dimitri Sverjensky, Jihua Hao, George Cody, and Robert Hazen. Dr. Irena Mamajanov analyzed samples with Ultra-High Performance Liquid Chromatography-Mass Spectrometry on numerous occasions and helped us determine the identity and concentration of organic species that had formed from the decomposition of aspartate. George Cody provided us with expertise on conducting high temperature experiments involving gold capsules, and during several discussions, he suggested possible reaction mechanisms and explanations to account for the products we detected. Jihua Hao calculated the speciation of the aqueous fluid in our experiments using the program EQ3 to estimate variables that we were unable to measure during our experiments, including solution pH, CO2(g) concentrations, and the extent of Mg2+ complexing, which hold important implications for our interpretation of the data. I vii am also extremely grateful to Dionysis Foustoukos who helped me with several of the experimental methods and analyzed the samples with ion chromatography. I also thank Chris Glein, Namhey Lee, Paul Goldey, and John Armstrong for useful discussions and aid in the laboratory. Thank you, everyone, for this experience. I had a wonderful time! viii Contents Abstract ii Acknowledgments iv List of Tables xiii List of Figures xv 1. Introduction. 1 References. 8 2. Interactions between L-aspartate and the brucite [Mg(OH)2]-water interface. .12 1. Introduction. 15 2. Materials and Methods. 20 2.1. Brucite Synthesis. 20 2.2.
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