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Information to Users INFORMATION TO USERS The most advanced technology has been used to photograph and reproduce this manuscript from the microfilm master. UMI films the text directly from the original or copy submitted. Thus, some thesis and dissertation copies are in typewriter face, while others may be from any type of computer printer. The quality of this reproduction is dependent upon the quality of the copy submitted. Broken or indistinct print, colored or poor quality illustrations and photographs, print bleedthrough, substandard margins, and improper alignment can adversely affect reproduction. In the unlikely event that the author did not send UMI a complete manuscript and there are missing pages, these will be noted. Also, if unauthorized copyright material had to be removed, a note will indicate the deletion. Oversize materials (e.g., maps, drawings, charts) are reproduced by sectioning the original, beginning at the upper left-hand corner and continuing from left to right in equal sections with small overlaps. Each original is also photographed in one exposure and is included in reduced form at the back of the book. Photographs included in the original manuscript have been reproduced xerographically in this copy. Higher quality 6" x 9" black and white photographic prints are available for any photographs or illustrations appearing in this copy for an additional charge. Contact UMI directly to order. University Microfilms International A Ben & Howe'i Information Company 300 North ZeeO Road Ann ArOo> Ml 48106-1346 USA 313 761-4700 800 521-0600 Order Number 910522S The bonding and electronic structure of tris(cyclopentadienyl) actinide compounds and related transition metal systems Strittmatter, Richard Joseph, Ph.D. The Ohio State University, 1990 UMI 300 N. Zceb RA Ann Arbor, MI 48106 THE BONDING AND ELECTRONIC STRUCTURE OF TRIS(CYCLOPENTADIENYL) ACTINIDE COMPOUNDS AND RELATED TRANSITION-METAL SYSTEMS DISSERTATION Presented in Partial Fulfillment of the Requirements for the Degree Doctor of Philosophy in the Graduate School of the Ohio State University By Richard Joseph Strittmatter, B.S. ***** The Ohio State University 1990 Dissertation Committee: Approved by Dr. Bruce E . Bursten Dr. Sheldon G. Shore — Bruce E. Bursten, Dr. James A. Cowan Department of Chemistry With Love, To My Mother and to My Father and To Carol ii ACKNOWLEDGMENTS Many people have helped to make my graduate career a truly rewarding experience. I would like to first thank Professor Bruce Bursten for his guidance and encouragement in the development of my scientific career. Bruce is not only an advisor and teacher, but a friend who continually provides his students with excellent opportunities, and 1 consider myself fortunate to have worked with him. I would also like to thank all members of the Bursten group, past and present, for providing an enjoyable and challenging working environment. Larry Rhodes, whose constant encouragement (or was that nagging?) served as a springboard for my experimental work, and Bill Schneider, who (probably to his chagrin) was a constant source of theoretical expertise, deserve special recognition. I am indebted to Dr. A1 Sattelberger for providing me the wonderful opportunity of working at Los Alamos National Laboratory, and to all my friends and colleagues at INC-4 who made my time in New Mexico an unforgettable experience. I must thank Dave Morris for his help with the electrochemical studies, Robin Rogers for his crystallographic work, and Adam Brldgeman and Dr. Jennifer Green for the photoelectron spectroscopic data. I wish to thank all of those people who have made my time in Columbus a happy and memorable period of my life; Bob, Sheila, Phil, Chris, Toshi, Laurie, Pete, the Degenerate HOMO'S (we almost made it to iii New Orleans), the Uave, and everyone else - thank you. I also would like to thank ray parents and my family for their encouragement, support, and love. Finally, I would like to thank my loving and caring wife, Carol. Without your boundless patience and understanding, I would not have made it. You make life worth living. iv VITA November 20, 1963 ......................Bom, Washington, D.C. May, 1985 .............................. B.S., Wake Forest University, Winston-Salem, North Carolina, Chemistry, Mathematics (Minor) Sept., 1985 - Aug., 1988............... Teaching Assistant, Department of Chemistry, The Ohio State University, Sept., 1988 - Dec., 1988............... Amoco Industrial Fellow, Department of Chemistry, The Ohio State University Jan., 1989 - June, 1989 ................Graduate Research Assistant, Los Alamos National Laboratory Los Alamos, New Mexico July, 1989 - March, 1990............... Presidential Fellow, Department of Chemistry, The Ohio State University April, 1990 - July, 1990............... Research Associate, Department of Chemistry, The Ohio State University PUBLICATIONS nf-0rbital to Carbonyl 2»r Back-bonding: The Electronic Structures of (r^-CjHjJjUCO and (rj5-C5Hj)3U0C", B. E, Bursten and R. J. Strittmatter, J. Am. Chem. Soc. 1987, 1££, 6606-6608. "The Bonding in Tris(tj3-cyclopentadienyl) Actinide Complexes. 2. On the Ground Electronic Configurations of "Base-Free" Cp3An Complexes (An - Th, Pa, U, Np, Pu)", B. E. Bursten, L. F. Rhodes, and R. J. Strittmatter, J. Am. Chem Soc. 1989, 111. 2756-2758. v "The Bonding in Tris (fj5-cyclopentadienyl) Actinide Complexes. 3. The Interaction of w-Neutral, *-Acidic, and x-Basic Ligands with (»?!- CsH5)3U", B. E. Bursten, L. F. Rhodes, and R. J. Strittmatter, J . Am. Chem. Soc. 1989, 111, 2758-2766. "The Bonding in Tris(ij3-cyclopentadienyl) Actinide Complexes. 4. Electronic Structural Effects in AnCl3 and (fjs-C5H5)3An (An — Th through Cf) Complexes", B . E. Bursten, L. F. Rhodes, and R. J . Strittmatter, J . Less-Common Met. 1989, 142, 207-211. "Relativistic DV-Xa Studies of Three-Coordinate Actinide Complexes", W. F. Schneider, R. J. Strittmatter, B. E. Bursten, and D. E. Ellis, in Density Functional Approaches to Chemistry. J. K. Labanowski and J. W. Andzelm, eds., Springer-Verlag, New York, 1990. FIELDS OF STUDY Major Field: Chemistry Inorganic Chemistry, Organometallic Chemistry, and Theoretical Chemistry. The Ohio State University; Professor Bruce E. Bursten, Adviser. vi TABLE OF CONTENTS DEDICATION........................................................... il ACKNOWLEDGMENTS.................................................... iii VITA............................................ v LIST OF TABLES........................................................ x LIST OF FIGURES.................................................... xii CHAPTER PAGE I THE ELECTRONIC STRUCTURE OF ACTINIDE ORGANOMETALLICS: AN HISTORICAL PERSPECTIVE .................................... I INTRODUCTION .............................................. 2 ORGANOACTINIDE COMPOUNDS WITH n-BONDED LIGANDS ............ 5 8-Annulene (Cyclooctatetraene) Complexes ............ 5 Electronic states of the actinocenes ................ 6 Photoelectron Spectroscopy and Molecular Orbital Studies of Actinocenes ........................ 11 Cyclopentadienyl Complexes .......................... 19 Tetrakis(cyclopentadienyl) Complexes ................ 20 Tris(cyclopentadienyl) Complexes .................... 25 Bis(cyclopentadienyl)actinide Complexes .............. 28 ORGANOACTINIDE COMPOUNDS WITH a -BONDED LIGANDS ............ 32 Tris(cyclopentadienyl)actinide Complexes ............ 33 Bis(cyclopentadienyl)actinide Complexes .............. 39 Mono(cyclopentadienyl) Actinide Compounds ............ 51 ORGANOACTINIDES CONTAINING METAL-METAL BONDS .............. 51 II COMPUTATIONAL INVESTIGATIONS OF THE BONDING AND ELECTRONIC STRUCTURE OF "BASE-FREE" TRIS(CYCLOPENTADIENYL) ACTINIDE COMPLEXES.................................................. 55 INTRODUCTION .............................................. 56 vii QUALITATIVE BONDING PICTURE OF Cp3An COMPOUNDS ............ 60 Assumed structures of Cp3An compounds................ 60 Symmetry considerations of the Cp33' ligand field . 61 GROUND ELECTRON CONFIGURATIONS OF Cp3An COMPOUNDS WHERE An - Th THROUGH P u ........................................ 67 Xa-SW results........................................ 70 Comparison of Xa-SW with DV-Xa results .............. 74 Nonrelativistic vs. relativistlc.......... 80 THE BONDING IN Cp3An COMPOUNDS WHERE An - U THROUGH Cf AND A COMPARISON TO Cp3Ln COMPOUNDS AND A TRANSITION-METAL ANALOGUE ............................................ 80 Cp3An compounds...................................... 80 CpaLn compounds........................................ 100 Comparison with a transition-metal analogue............. 108 Conclusions............................................ Ill COMPUTATIONAL DETAILS ...................................... 113 III COMPUTATIONAL INVESTIGATIONS 01 THE BINDING OF A FOURTH LIGAND BY Cp3U .............................................. 116 Cp3U AS A F R A G M E N T .......................................... 116 Planar vs. pyramidal Cp3U .............................. 116 The frontier orbitals of Cp3U .......................... 119 U(III) vs. U(IV) compounds .......................... 126 a -BONDING INTERACTIONS OF Cp3U WITH A FOURTH LIGAND ..... 128 Cp3UH, the cr*only case ................................ 128 Cp3UNH3 and Cp3UCH3, examples of observed compounds . 133 Cp3U as a Q-donor? .....................................136 THE INTERACTION OF Cp3U WITH ir-ACIDIC L I G A N D S................. 139 Cp3UC0, an example of a classical ir-acid compound . 139 Isocyanlde, nitrosyl, and dinltrogen complexesof
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