The occurrence of carbon monoxide (CO) and nitric oxide (NO) in human physiology and the potential of metal nitrosyl and carbonyl complexes as pharmaceuticals have added new paradigms in modern biology and medicine. In addition to one or more NO or CO as ligands, these metal complexes contain designed organic frames as auxiliary ligand(s). These auxiliary ligands have been carefully tailored so as to promote release of NO or CO from the resulting nitrosyls and carbonyls upon exposure to light of selected wavelengths and with desired efficiencies. Once isolated, the NO and CO releasing molecules (NORMs and CORMs, respectively) have been subjected to a wide range of in vitro and in vivo biological experiments to evaluate the utility of the photoactive NORMS and CORMs as photochemotherapeutics. This chapter focuses on the results from these pursuits by various groups during the past few years.
Chapter 6 Reactive Transition Metal Nitride Complexes Jeremy M. Smith, Jeremy M. Smith Department of Chemistry and Biochemistry, New Mexico State University, Las Cruces, NM 88003Search for more papers by this author Jeremy M. Smith, Jeremy M. Smith Department of Chemistry and Biochemistry, New Mexico State University, Las Cruces, NM 88003Search for more papers by this author Book Editor(s):Kenneth D. Karlin, Kenneth D. Karlin Department of Chemistry Johns Hopkins University Baltimore, MarylandSearch for more papers by this author First published: 04 April 2014 https://doi.org/10.1002/9781118792797.ch06Citations: 72Book Series:Progress in Inorganic Chemistry AboutPDFPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShareShare a linkShare onEmailFacebookTwitterLinkedInRedditWechat Summary This chapter focuses on the chemistry of the terminal metal nitride fragment, MN (i.e., the synthesis and reactivity of the nitride ligand in transition metal complexes). 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During the last few decades, transition metal catalysts, especially those on precious metals have proven to be efficient for a large number of applications. Due to its abundance, inexpensiveness, and environmentally benign nature, use of iron has increased significantly in the last two decades for synthetic transformation both in asymmetric synthesis and reaction methodology. This development encouraged to summarize the use of iron catalysis in organic synthesis, which includes cycloadditions, CC, CN bond formation, redox, and other reactions. Trifluoromethylated cyclopropanes are important compounds in drug delivery, though very few synthetic methods were reported for their preparation. This chapter has been divided into different sections based on the reaction type. It discusses that the iron-catalyzed cross-coupling reaction mechanism is versatile and varies with the nature of the coupling partners and based on the reaction condition. Sulfoxides are an important class of compounds since they were used for various ligand syntheses.
AbstractReview: history and evolution of tris(dithiolene) complexes (arenedithiolate, alkenedihiolate, and dithione complexes); 360 refs.
Chapter 4 MetalMetal Bond-Containing Complexes as Catalysts for CH Functionalization Katherine P. Kornecki, Katherine P. Kornecki Department of Chemistry, University of Wisconsin – Madison, Madison, WI53706Search for more papers by this authorJohn F. Berry, John F. Berry Department of Chemistry, University of Wisconsin – Madison, Madison, WI53706Search for more papers by this authorDavid C. Powers, David C. Powers Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA02138Search for more papers by this authorTobias Ritter, Tobias Ritter Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA02138Search for more papers by this author Katherine P. Kornecki, Katherine P. Kornecki Department of Chemistry, University of Wisconsin – Madison, Madison, WI53706Search for more papers by this authorJohn F. Berry, John F. Berry Department of Chemistry, University of Wisconsin – Madison, Madison, WI53706Search for more papers by this authorDavid C. Powers, David C. Powers Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA02138Search for more papers by this authorTobias Ritter, Tobias Ritter Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA02138Search for more papers by this author Book Editor(s):Kenneth D. Karlin, Kenneth D. Karlin Department of Chemistry Johns Hopkins University Baltimore, MarylandSearch for more papers by this author First published: 04 April 2014 https://doi.org/10.1002/9781118792797.ch04Citations: 33Book Series:Progress in Inorganic Chemistry AboutPDFPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShareShare a linkShare onFacebookTwitterLinked InRedditWechat Summary This chapter explores examples in which binuclear complexes are involved in CH functionalization reactions and explores the effect of MM bonds in catalysis. Functionalization of CH bonds is a field of current interest, and many methodologies for achieving selective CH functionalization continue to appear in the literature. The chapter discusses mixed-valent Ru2(II,III) dimers, having an Ru-Ru bond order of 2.5. Although the topics of Rh2 and Pd2 CH functionalization have been reviewed extensively, this chapter focuses on the relationship between electronic structure and reaction mechanisms. It compares the chemistries of Rh2 and Pd2 complexes and discusses the ways in which the intriguing geometric and electronic structure of these species may facilitate CH functionalization reactions. Citing Literature Progress in Inorganic Chemistry Volume 58 RelatedInformation
This chapter focuses attention on the interactions of four types of organo–NOx (x= 1) compounds with metals. It describes the chemistry of C-nitroso compounds, N-nitroso compounds, S-nitroso compounds, and O-nitroso compounds. Nitrosoalkanes and nitrosoarenes frequently serve as ligands to metal centers, and in many cases simple adduct formation between the pre-formed C-nitroso compounds and metal centers occur with or without the displacement of an existing ligand on the metal. The chapter presents the synthetic routes to metal-nitrosoalkane and metal-nitrosoarene compounds and the binding modes of the C-nitroso ligands that have been established crystallographically. It examines the fundamental coordination chemistry of these organonitroso compounds with metal centers that form the basis for their observed chemical and biochemical reactivity. Adsorption of alkyl nitrites on metal surfaces frequently results in the generation of alkoxy radicals and NO, and can lead to follow-up reactions with other substrates.
Chapter 5 Monomeric Dinitrosyl Iron Complexes: Synthesis and Reactivity Camly T. Tran, Camly T. Tran Department of Chemistry, Brown University, Providence, RISearch for more papers by this authorKelsey M. Skodje, Kelsey M. Skodje Department of Chemistry, Brown University, Providence, RISearch for more papers by this authorEunsuk Kim, Eunsuk Kim Department of Chemistry, Brown University, Providence, RISearch for more papers by this author Camly T. Tran, Camly T. Tran Department of Chemistry, Brown University, Providence, RISearch for more papers by this authorKelsey M. Skodje, Kelsey M. Skodje Department of Chemistry, Brown University, Providence, RISearch for more papers by this authorEunsuk Kim, Eunsuk Kim Department of Chemistry, Brown University, Providence, RISearch for more papers by this author Book Editor(s):Kenneth D. Karlin, Kenneth D. Karlin Department of Chemistry, Johns Hopkins University, Baltimore, MarylandSearch for more papers by this author First published: 25 July 2014 https://doi.org/10.1002/9781118869994.ch05Citations: 14Book Series:Progress in Inorganic Chemistry AboutPDFPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShareShare a linkShare onFacebookTwitterLinked InRedditWechat Summary This chapter focuses on the synthesis, physical properties, and chemical reactivity of the synthetic analogues of such dinitrosyl iron species. Though monomeric dinitrosyl iron complexes (DNICs) have gained interest due to their biological relevance, there are various types of iron nitrosyls that have historical or chemical significance. The aim of the chapter is to highlight the synthesis, structure, and reactivity of various known discrete DNICs currently in the literature, which can complement the existing reviews of their biological roles. Dinitrosyl iron complexes may also play roles outside of NO storage and transfer, as is suggested by the ability of neutral {Fe(NO)2}10 complexes to promote phenol nitration in the presence of dioxygen. Examining the trends in electronic and geometric structure in these complexes and how that contributes to their reactivity is vital in forming an understanding of how they behave in a biological setting. Citing Literature Progress in Inorganic Chemistry: Volume 59 RelatedInformation
Chapter 2 A New Paradigm for Photodynamic Therapy Drug Design: Multifunctional, Supramolecular DNA Photomodification Agents Featuring Ru(II)/Os(II) Light Absorbers Coupled to Pt(II) or Rh(III) Bioactive Sites Jessica D. Knoll, Jessica D. Knoll Department of Chemistry, Virginia Tech, Blacksburg, VASearch for more papers by this authorKaren J. Brewer, Karen J. Brewer Department of Chemistry, Virginia Tech, Blacksburg, VASearch for more papers by this author Jessica D. Knoll, Jessica D. Knoll Department of Chemistry, Virginia Tech, Blacksburg, VASearch for more papers by this authorKaren J. Brewer, Karen J. Brewer Department of Chemistry, Virginia Tech, Blacksburg, VASearch for more papers by this author Book Editor(s):Kenneth D. Karlin, Kenneth D. Karlin Department of Chemistry, Johns Hopkins University, Baltimore, MarylandSearch for more papers by this author First published: 25 July 2014 https://doi.org/10.1002/9781118869994.ch02Citations: 1Book Series:Progress in Inorganic Chemistry AboutPDFPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShareShare a linkShare onFacebookTwitterLinked InRedditWechat Summary This chapter focuses on Ru(II) or Os(II) light absorbers coupled to Pt(II) or Rh(III) bioactive sites. These bioactive sites interact with deoxyribonucleic acid (DNA) through thermal and/or photoinduced binding and photocleavage via oxygen dependent or independent mechanisms designed as a new paradigm for photodynamic therapy drug design. A brief introduction into targeting DNA in cancer therapy research, photodynamic therapy (PDT), cisplatin and related platinum-based chemotherapy drugs, and Rh(III)–polyazine and Rh2(II,II)– DNA modification agents is given to set the stage for the discussion of supramolecular complexes containing PDT active light absorbing units coupled to Pt(II) or Rh(III) centers. Incorporation of Os(II) in place of Ru(II) in other previously reported supramolecular complexes may also result in interesting interactions with DNA in the PDT window. This result provides a promising direction for mixed-metal DNA photomodification agents. Citing Literature Progress in Inorganic Chemistry: Volume 59 RelatedInformation
Nowhere is creative scientific talent busier than in the world of inorganic chemistry experimentation. Progress in Inorganic Chemistry continues in its tradition of being the most respected avenue for exchanging innovative research. This series provides inorganic chemists and materials scientists with a forum for critical, authoritative evaluations of advances in every area of the discipline. With contributions from internationally renowned chemists, this latest volume offers an in-depth, far-ranging examination of the changing face of the field, providing a tantalizing glimpse of the emerging state of the science.
(18)O-isotope-labeling studies have led to the conclusion that there exist two major pathways for water oxidation catalyzed by dimeric ruthenium ions of the general type cis, cis-[L2Ru(III)(OH2)]2O(4+). We have proposed that both pathways involve concerted addition of H and OH fragments derived from H 2O to the complexes in their four-electron-oxidized states, i.e., [L2Ru(V)(O)]2O(4+), ultimately generating bound peroxy intermediates that decay with the evolution of O2. The pathways differ primarily in the site of addition of the OH fragment, which is either a ruthenyl O atom or a bipyridine ligand. In the former case, water addition is thought to give rise to a critical intermediate whose structure is L2Ru(IV)(OH)ORu(IV)(OOH)L2(4+); the structures of intermediates involved in the other pathway are less well defined but may involve bipyridine OH adducts of the type L2Ru(V)(O)ORu(IV)(OH)(L(*)OH)L(4+), which could react further to generate unstable dioxetanes or similar endoperoxides. Published experimental and theoretical support for these pathways is reviewed within the broader context of water oxidation catalysis and related reactions reported for other diruthenium and group 8 monomeric diimine-based catalysts. New experiments that are designed to probe the issue of bipyridine ligand "noninnocence" in catalysis are described. Specifically, the relative contributions of the two pathways have been shown to correlate with substituent effects in 4,4'- and 5,5'-substituted bipyridine complexes in a manner consistent with the formation of a reactive OH-adduct intermediate in one of the pathways, and the formation of OH-bipyridine adducts during catalytic turnover has been directly confirmed by optical spectroscopy. Finally, a photosensitized system for catalyzed water oxidation has been developed that allows assessment of the catalytic efficiencies of the complex ions under neutral and alkaline conditions; these studies show that the ions are far better catalysts than had previously been assumed based upon reported catalytic parameters obtained with strong oxidants in acidic media.
This chapter contains sections titled: Introduction Early Studies with Nonbiological Metal Ions Studies of the Cleavage of Phosphate Diesters Promoted by Metal Ion Complexes in Alcohol Fast Metal Ion Promoted Hydrolysis in Wet Alcohol: 20:Zn2 II:(RO−) Promoted Hydrolysis of a DNA Model (21b) in Ethanol Conclusions Acknowledgments Abbreviations References
Chapter 6 DNA Based Metal Catalysis Jens Oelerich, Jens Oelerich Stratingh Institute for Chemistry, University of Groningen, The NetherlandsSearch for more papers by this authorGerard Roelfes, Gerard Roelfes Stratingh Institute for Chemistry, University of Groningen, The NetherlandsSearch for more papers by this author Jens Oelerich, Jens Oelerich Stratingh Institute for Chemistry, University of Groningen, The NetherlandsSearch for more papers by this authorGerard Roelfes, Gerard Roelfes Stratingh Institute for Chemistry, University of Groningen, The NetherlandsSearch for more papers by this author Book Editor(s):Kenneth D. Karlin, Kenneth D. Karlin Department of Chemistry, Johns Hopkins University, Baltimore, Maryland, USASearch for more papers by this author First published: 16 November 2011 https://doi.org/10.1002/9781118148235.ch6Citations: 2Book Series:Progress in Inorganic Chemistry AboutPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShare Give accessShare full text accessShare full-text accessPlease review our Terms and Conditions of Use and check box below to share full-text version of article.I have read and accept the Wiley Online Library Terms and Conditions of UseShareable LinkUse the link below to share a full-text version of this article with your friends and colleagues. Learn more.Copy URL Share a linkShare onFacebookTwitterLinked InRedditWechat Summary This chapter contains sections titled: Introduction DNA Templated Metal Catalysis Asymmetric DNA Based Metal Catalysis Mechanistic Investigations into DNA Based Catalysis Conclusion and Perspective Abbreviations References Citing Literature Progress in Inorganic Chemistry, Volume 57 RelatedInformation
