A5072262316- X-ray Diffraction in Crystallography
- Crystallization and Solubility Studies
- Organometallic Complex Synthesis and Catalysis
- Magnetism in coordination complexes
- Metal-Catalyzed Oxygenation Mechanisms
- Inorganic Fluorides and Related Compounds
- Metalloenzymes and iron-sulfur proteins
- Inorganic Chemistry and Materials
- Crystallography and molecular interactions
- Metal complexes synthesis and properties
- Metal-Organic Frameworks: Synthesis and Applications
- Research on Leishmaniasis Studies
- Synthesis and Biological Evaluation
- Chemical Thermodynamics and Molecular Structure
- X-ray Spectroscopy and Fluorescence Analysis
- Trypanosoma species research and implications
Harvard University
2019-2025
Chagas disease is caused by the intracellular protozoan parasite Trypanosomal cruzi, and current drugs are lacking in terms of desired safety efficacy profiles. Following on a recently reported high-throughput screening campaign, we have explored initial structure–activity relationships around class imidazole-based compounds. This profiling has uncovered compounds 4c (NEU321) 4j (NEU704), which potent against vitro cultures T. cruzi greater than 160-fold selective over host cells. We report...
Metal atom lability from a well-defined bimetallic cluster was canvassed as function of ligand substitution, redox chemistry, and group transfer processes.
We analyze the effect of integrated resolution, data scaling, structural refinement, and crystal symmetry on extracted scattering perturbations their uncertainties for anomalous (resonant) X-ray diffraction mixed-metal molecular clusters. probe metal constituency, substitutional homogeneity, positional disorder both biased unbiased ligand environments. Anomalous studies were conducted (FtbsL)Zn2Ni(py) (1), [K(C222)][(FtbsL)Zn2Ni] (2), [K(THF)3][(FtbsL)Zn2Ni(NAd)] (3). Analysis collected at...
In polynuclear biological active sites, multiple electrons are needed for turnover, and the distribution of these among metal sites is affected by structure site. However, study interplay between redox difficult not only in systems but also synthetic clusters since most changes produce one thermodynamically stable product. Here, unusual chemistry a sterically hindered trichromium complex allowed us to probe relationship structural isomerism. Two structurally isomeric imides were isolated:...
In this report we examine a family of trinuclear iron complexes by multiple-wavelength, anomalous diffraction (MAD) to explore the redox load distribution within cluster materials free refinement atomic scattering factors. Several effects were explored that can impact factors clusters, including 1) metal atom primary coordination sphere, 2) M−M bonding, and 3) delocalization in formally mixed-valent species. Complexes investigated which vary from highly symmetric fully asymmetric 57 Fe...
Abstract The trichromium cluster ( tbs L)Cr 3 (thf) ([ L] 6− =[1,3,5‐C 6 H 9 (NC 4 ‐ o ‐NSi t BuMe 2 ) ] exhibits steric‐ and solvation‐controlled reactivity with organic azides to form three distinct products: reaction of benzyl azide forms a symmetrized bridging imido complex μ ‐NBn); mesityl in benzene affords terminally bound 1 ‐NMes); whereas the THF leads terminal N‐atom excision from yield nitride ‐N). this demonstrates ability cluster‐templating ligand produce well‐defined...
Anomalous X-ray diffraction (AXD) and neutron can be used to crystallographically distinguish between metals of similar electron density. Despite the use AXD for structural characterization in mixed metal clusters, there are no benchmark studies evaluating accuracy toward assessing elemental occupancy molecules with comparisons what is determined via diffraction. We collected resonant data on several homo heterometallic clusters refined their anomalous scattering components determine site...
Metalation of the polynucleating ligand F,tbs LH6 (1,3,5-C6 H9 (NC6 H3 -4-F-2-NSiMe2t Bu)3 ) with two equivalents Zn(N(SiMe3 )2 affords dinuclear product (F,tbs LH2 )Zn2 (1), which can be further deprotonated to yield L)Zn2 Li2 (OEt2 )4 (2). Transmetalation 2 NiCl2 (py)2 yields heterometallic, trinuclear cluster Ni(py) (3). Reduction 3 KC8 [KC222 ][(F,tbs Ni] (4) features a monovalent Ni centre. Addition 1-adamantyl azide 4 generates bridging μ3 -nitrenoid adduct [K(THF)3 Ni(μ3 -NAd)] (5)....
Abstract Metalation of the polynucleating ligand F,tbs LH 6 (1,3,5‐C H 9 (NC 3 −4‐F−2‐NSiMe 2 t Bu) ) with two equivalents Zn(N(SiMe affords dinuclear product ( )Zn 1 ), which can be further deprotonated to yield L)Zn Li (OEt 4 ). Transmetalation NiCl (py) yields heterometallic, trinuclear cluster Ni(py) Reduction KC 8 [KC 222 ][( Ni] features a monovalent Ni centre. Addition 1‐adamantyl azide generates bridging μ ‐nitrenoid adduct [K(THF) Ni(μ ‐NAd)] 5 EPR spectroscopy reveals that anionic...
Abstract The trichromium cluster ( tbs L)Cr 3 (thf) ([ L] 6− =[1,3,5‐C 6 H 9 (NC 4 ‐ o ‐NSi t BuMe 2 ) ] exhibits steric‐ and solvation‐controlled reactivity with organic azides to form three distinct products: reaction of benzyl azide forms a symmetrized bridging imido complex μ ‐NBn); mesityl in benzene affords terminally bound 1 ‐NMes); whereas the THF leads terminal N‐atom excision from yield nitride ‐N). this demonstrates ability cluster‐templating ligand produce well‐defined...