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1.
ACS Comb Sci ; 22(10): 475-494, 2020 10 12.
Artículo en Inglés | MEDLINE | ID: mdl-32631055

RESUMEN

N-Isocyaniminotriphenylphosphorane (NIITP) is a functionalized isonitrile that has been extensively applied in a variety of organic reactions during the last two decades. This Review summarizes the most important applications in organic synthesis of this versatile reactant, with the focus posed on mechanistic and methodological aspects allowing the generation of molecular diversity. NIITP combines the reactivity of isonitriles with that of phosphoranes to enable chemical transformations employed in the construction of compound libraries. Here, we cover from the initial applications of NIITP in the Nef isocyanide reaction to further derivations that render a variety of heterocyclic scaffolds. The presence of the isonitrile moiety in this singular compound makes possible the double addition of nucleophiles and electrophiles, which followed by inter(intra)molecular aza-Wittig type transformations enable several multicomponent and tandem processes. In particular, we stress the impact of NIITP in oxadiazole chemistry, from the early two-component transformations to recent examples of multicomponent reactions that take place in the presence of suitable electrophiles. In addition, we briefly describe the role of NIITP chemistry in generating skeletal and conformational diversity in cyclic peptides. The reaction of NIITP with alkynes is thoroughly revised, with particular emphasis on silver-catalyzed processes that have been developed in the last years. Biomedicinal applications of some reaction products are also mentioned along with a perspective of future applications of this reactant.


Asunto(s)
Técnicas de Química Sintética/métodos , Fosforanos/química , Alquinos/química , Carbodiimidas/química , Catálisis , Ciclización , Conformación Molecular , Estructura Molecular , Nitrilos/química , Oxadiazoles/química , Plata/química , Bibliotecas de Moléculas Pequeñas/síntesis química
2.
J Enzyme Inhib Med Chem ; 35(1): 639-649, 2020 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-32048531

RESUMEN

Leishmaniasis is a neglected disease caused by the protozoa Leishmania ssp. Environmental differences found by the parasites in the vector and the host are translated into cellular stress, leading to the production of heat shock proteins (Hsp). These are molecular chaperones involved in the folding of nascent proteins as well as in the regulation of gene expression, signalling events and proteostasis. Since Leishmania spp. use Hsp90 to trigger important transitions between their different stages of the life cycle, this protein family becomes a profitable target in anti-parasite drug discovery. In this work, we implemented a multidisciplinary strategy coupling molecular modelling with in vitro assays to identify small molecules able to inhibit Hsp90 from L. braziliensis (LbHsp90). Overall, we identified some compounds able to kill the promastigote form of the L. braziliensis, and to inhibit LbHsp90 ATPase activity.


Asunto(s)
Antiprotozoarios/farmacología , Inhibidores Enzimáticos/farmacología , Proteínas HSP90 de Choque Térmico/antagonistas & inhibidores , Leishmania braziliensis/efectos de los fármacos , Chaperonas Moleculares/farmacología , Bibliotecas de Moléculas Pequeñas/farmacología , Adenosina Trifosfatasas/antagonistas & inhibidores , Adenosina Trifosfatasas/metabolismo , Antiprotozoarios/síntesis química , Antiprotozoarios/química , Relación Dosis-Respuesta a Droga , Descubrimiento de Drogas , Inhibidores Enzimáticos/síntesis química , Inhibidores Enzimáticos/química , Proteínas HSP90 de Choque Térmico/metabolismo , Leishmania braziliensis/química , Modelos Moleculares , Chaperonas Moleculares/síntesis química , Chaperonas Moleculares/química , Estructura Molecular , Pruebas de Sensibilidad Parasitaria , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/química , Relación Estructura-Actividad
3.
Eur J Med Chem ; 182: 111628, 2019 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-31472473

RESUMEN

Dengue fever is a mosquito-borne viral disease that has become a major public health concern worldwide. This disease presents with a wide range of clinical manifestations, from a mild cold-like illness to the more serious hemorrhagic dengue fever and dengue shock syndrome. Currently, neither an approved drug nor an effective vaccine for the treatment are available to fight the disease. The envelope protein (E) is a major component of the virion surface. This protein plays a key role during the viral entry process, constituting an attractive target for the development of antiviral drugs. The crystal structure of the E protein reveals the existence of a hydrophobic pocket occupied by the detergent n-octyl-ß-d-glucoside (ß-OG). This pocket lies at the hinge region between domains I and II and is important for the low pH-triggered conformational rearrangement required for the fusion of the virion with the host's cell. Aiming at the design of novel molecules which bind to E and act as virus entry inhibitors, we undertook a de novo design approach by "growing" molecules inside the hydrophobic site (ß-OG). From more than 240000 small-molecules generated, the 2,4 pyrimidine scaffold was selected as the best candidate, from which one synthesized compound displayed micromolar activity. Molecular dynamics-based optimization was performed on this hit, and thirty derivatives were designed in silico, synthesized and evaluated on their capacity to inhibit dengue virus entry into the host cell. Four compounds were found to be potent antiviral compounds in the low-micromolar range. The assessment of drug-like physicochemical and in vitro pharmacokinetic properties revealed that compounds 3e and 3h presented acceptable solubility values and were stable in mouse plasma, simulated gastric fluid, simulated intestinal fluid, and phosphate buffered saline solution.


Asunto(s)
Antivirales/farmacología , Virus del Dengue/efectos de los fármacos , Diseño de Fármacos , Bibliotecas de Moléculas Pequeñas/farmacología , Proteínas del Envoltorio Viral/antagonistas & inhibidores , Células A549 , Animales , Antivirales/síntesis química , Antivirales/química , Línea Celular , Supervivencia Celular/efectos de los fármacos , Virus del Dengue/metabolismo , Relación Dosis-Respuesta a Droga , Humanos , Ratones , Pruebas de Sensibilidad Microbiana , Modelos Moleculares , Estructura Molecular , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/química , Solubilidad , Relación Estructura-Actividad , Proteínas del Envoltorio Viral/metabolismo
4.
Drug Dev Res ; 80(5): 666-679, 2019 08.
Artículo en Inglés | MEDLINE | ID: mdl-31112325

RESUMEN

Inflammation is the response of the body to noxious stimuli such as infections, trauma, or injury. Experimental studies have shown that vanillic acid has anti-inflammatory effects. The objective of this study was to investigate the anti-inflammatory and antipyretic properties of the derivative of vanillic acid, isopropyl vanillate (ISP-VT), in mice. The results of this study indicated that ISP-VT reduced paw edema induced by carrageenan, dextran sulfate (DEX), compound 48/80, serotonin, bradykinin (BK), histamine (HIST), and prostaglandin E2 (PGE2). Furthermore, ISP-VT reduced recruitment of leukocytes and neutrophils and reduced its adhesion and rolling, and decreased myeloperoxidase enzyme activity (MPO), cytokine levels (tumor necrosis factor-α and interleukin-6), and vascular permeability. ISP-VT also significantly reduced the expression of cyclooxygenase-2 (COX-2) in subplantar tissue of mice. ISP-VT inhibited COX-2 selectively compared to the standard drug. Our results showed that although ISP-VT binds to COX-1, it is less toxic than indomethacin, as evidenced by MPO analysis of gastric tissue. Treatment with the ISP-VT significantly reduced rectal temperature in yeast-induced hyperthermia in mice. Our results showed that the main mechanism ISP-VT-induced anti-inflammatory activity is by inhibition of COX-2. In conclusion, our results indicate that ISP-VT has potential as an anti-inflammatory and antipyretic therapeutic compound.


Asunto(s)
Antiinflamatorios/administración & dosificación , Carragenina/efectos adversos , Inhibidores de la Ciclooxigenasa/administración & dosificación , Inflamación/tratamiento farmacológico , Fenoles/efectos adversos , Ácido Vanílico/química , Animales , Antiinflamatorios/síntesis química , Antiinflamatorios/química , Antiinflamatorios/farmacología , Anticuerpos Monoclonales/efectos de los fármacos , Inhibidores de la Ciclooxigenasa/síntesis química , Inhibidores de la Ciclooxigenasa/química , Inhibidores de la Ciclooxigenasa/farmacología , Modelos Animales de Enfermedad , Femenino , Inflamación/inducido químicamente , Inflamación/metabolismo , Inyecciones Intraperitoneales , Masculino , Ratones , Modelos Moleculares , Fenoles/síntesis química , Fenoles/química , Fenoles/farmacología , Bibliotecas de Moléculas Pequeñas/administración & dosificación , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/química , Bibliotecas de Moléculas Pequeñas/farmacología
5.
J Enzyme Inhib Med Chem ; 34(1): 310-321, 2019 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-30734604

RESUMEN

Loxosceles spiders' venoms consist of a mixture of proteins, including the sphingomyelinases D (SMases D), which are the main toxic components responsible for local and systemic effects in human envenomation. Herein, based on the structural information of SMase D from Loxosceles laeta spider venom and virtual docking-based screening approach, three benzene sulphonate compounds (named 1, 5 and 6) were identified as potential Loxosceles SMase D inhibitors. All compounds inhibited the hydrolysis of the sphingomyelin substrate by both recombinant and native SMases D. Compounds 5 and 6 acted as SMases D uncompetitive inhibitors with Ki values of 0.49 µM and 0.59 µM, respectively. Compound 1 is a mixed type inhibitor, and presented a Ki value of 0.54 µM. In addition, the three compounds inhibited the binding of SMases D to human erythrocytes and the removal of glycophorin C from the cell surface, which are important events in the complement-dependent haemolysis induced by Loxosceles venom. Moreover, compounds 5 and 6 reduced the binding of SMases to human keratinocytes membrane and the venom induced cell death. Importantly, compounds 5 and 6 also controlled the development of the necrotic lesion in an in vivo model of loxoscelism. Together, our findings indicate that the novel SMase D inhibitors presented here are able to suppress both local and systemic reactions induced by Loxosceles venoms. Since the number of Loxosceles envenomation accidents is currently growing worldwide, our results indicate that both inhibitors are promising scaffolds for the rational design of new drugs targeting SMases D from these spiders.


Asunto(s)
Inhibidores de Fosfodiesterasa/farmacología , Hidrolasas Diéster Fosfóricas/metabolismo , Enfermedades de la Piel/tratamiento farmacológico , Bibliotecas de Moléculas Pequeñas/farmacología , Picaduras de Arañas/tratamiento farmacológico , Animales , Eritrocitos/efectos de los fármacos , Eritrocitos/metabolismo , Humanos , Estructura Molecular , Inhibidores de Fosfodiesterasa/síntesis química , Inhibidores de Fosfodiesterasa/química , Conejos , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/química , Arañas
6.
ChemMedChem ; 13(16): 1732-1740, 2018 08 20.
Artículo en Inglés | MEDLINE | ID: mdl-29931741

RESUMEN

Over the last decades, much effort has been devoted to the design of the "ideal" library for screening, the most promising strategies being those which draw inspiration from biogenic compounds, as the aim is to add biological relevance to such libraries. On the other hand, there is a growing understanding of the role that molecular complexity plays in the discovery of new bioactive small molecules. Nevertheless, the introduction of molecular complexity must be balanced with synthetic accessibility. In this work, we show that both concepts can be efficiently merged-in a minimalist way-by using very simple guidelines during the design process along with the application of multicomponent reactions as key steps in the synthetic process. Natural phenanthrenoids, a class of plant aromatic metabolites, served as inspiration for the synthesis of a library in which complexity-enhancing features were introduced in few steps using multicomponent reactions. These resulting chemical entities were not only more complex than the parent natural products, but also interrogated an alternative region of the chemical space, which led to an outstanding hit rate in an antiproliferative assay: four out of twenty-six compounds showed in vitro activity, one of them being more potent than the clinically useful drug 5-fluorouracil.


Asunto(s)
Antineoplásicos/farmacología , Fenantrenos/farmacología , Bibliotecas de Moléculas Pequeñas/farmacología , Antineoplásicos/síntesis química , Antineoplásicos/química , Apoptosis/efectos de los fármacos , Línea Celular Tumoral , Diseño de Fármacos , Humanos , Estructura Molecular , Fenantrenos/síntesis química , Fenantrenos/química , Prueba de Estudio Conceptual , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/química
7.
Molecules ; 23(5)2018 May 16.
Artículo en Inglés | MEDLINE | ID: mdl-29772720

RESUMEN

The application of the reagent-based diversification strategy for generation of libraries of biologically promising ß-lactam derivatives is described. Key features are the versatility of the linker used and the cross-metathesis functionalization at the cleavage step. From an immobilized primary library, diversity was expanded by applying different cleavage conditions, leading to a series of cholesterol absorption inhibitor analogues together with interesting hybrid compounds through incorporation of a chalcone moiety.


Asunto(s)
Alquenos/química , Bibliotecas de Moléculas Pequeñas/síntesis química , beta-Lactamas/síntesis química , Anticolesterolemiantes/síntesis química , Anticolesterolemiantes/química , Catálisis , Estructura Molecular , Bibliotecas de Moléculas Pequeñas/química , Extracción en Fase Sólida , beta-Lactamas/química
8.
ChemMedChem ; 13(7): 648-661, 2018 04 06.
Artículo en Inglés | MEDLINE | ID: mdl-29160016

RESUMEN

Glycosaminoglycans (GAGs) are extracellular matrix and/or cell-surface sulfated glycans crucial to the regulation of various signaling proteins, the functions of which are essential in many pathophysiological systems. Because structural heterogeneity is high in GAG chains and purification is difficult, the use of structurally defined GAG oligosaccharides from natural sources as molecular models in both biophysical and pharmacological assays is limited. To overcome this obstacle, GAG-like oligosaccharides of well-defined structures are currently being synthesized by chemical and/or enzymatic means in many research groups around the world. These synthetic GAG oligosaccharides serve as useful molecular tools in studies of GAG-protein interactions. In this review, besides discussing the commonest routes used for the synthesis of GAG oligosaccharides, we also survey some libraries of these synthetic models currently available for research and discuss their activities in interaction studies with functional proteins, especially through the microarray approach.


Asunto(s)
Glicómica/métodos , Glicosaminoglicanos/metabolismo , Oligosacáridos/metabolismo , Proteínas/metabolismo , Proteómica/métodos , Bibliotecas de Moléculas Pequeñas/metabolismo , Secuencia de Carbohidratos , Humanos , Análisis por Micromatrices/métodos , Oligosacáridos/síntesis química , Unión Proteica , Bibliotecas de Moléculas Pequeñas/síntesis química
9.
Bioorg Med Chem Lett ; 27(16): 3851-3855, 2017 08 15.
Artículo en Inglés | MEDLINE | ID: mdl-28668194

RESUMEN

Dengue is a mosquito-borne virus that has become a major public health concern worldwide in recent years. However, the current treatment for dengue disease is only supportive therapy, and no specific antivirals are available to control the infections. Therefore, the need for safe and effective antiviral drugs against this virus is of utmost importance. Entry of the dengue virus (DENV) into a host cell is mediated by its major envelope protein, E. The crystal structure of the E protein reveals a hydrophobic pocket occupied by the detergent n-octyl-ß-d-glucoside (ß-OG) lying at a hinge region between domains I and II, which is important for the low-pH-triggered conformational rearrangement required for fusion. Thus, the E protein is an attractive target for the development of antiviral agents. In this work, we performed prospective docking-based virtual screening to identify small molecules that likely bind to the ß-OG binding site. Twenty-three structurally different compounds were identified and two of them had an EC50 value in the low micromolar range. In particular, compound 2 (EC50=3.1µM) showed marked antiviral activity with a good therapeutic index. Molecular dynamics simulations were used in an attempt to characterize the interaction of 2 with protein E, thus paving the way for future ligand optimization endeavors. These studies highlight the possibility of using a new class of DENV inhibitors against dengue.


Asunto(s)
Antivirales/farmacología , Virus del Dengue/efectos de los fármacos , Descubrimiento de Drogas , Bibliotecas de Moléculas Pequeñas/farmacología , Internalización del Virus/efectos de los fármacos , Antivirales/síntesis química , Antivirales/química , Células CACO-2 , Relación Dosis-Respuesta a Droga , Humanos , Pruebas de Sensibilidad Microbiana , Simulación de Dinámica Molecular , Estructura Molecular , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/química , Relación Estructura-Actividad
10.
Curr Top Med Chem ; 17(20): 2260-2270, 2017.
Artículo en Inglés | MEDLINE | ID: mdl-28240184

RESUMEN

Fragment-based drug discovery (FBDD) is a broadly used strategy in structure-guided ligand design, whereby low-molecular weight hits move from lead-like to drug-like compounds. Over the past 15 years, an increasingly important role of the integration of these strategies into industrial and academic research platforms has been successfully established, allowing outstanding contributions to drug discovery. One important factor for the current prominence of FBDD is the better coverage of the chemical space provided by fragment-like libraries. The development of the field relies on two features: (i) the growing number of structurally characterized drug targets and (ii) the enormous chemical diversity available for experimental and virtual screenings. Indeed, fragment-based campaigns have contributed to address major challenges in lead optimization, such as the appropriate physicochemical profile of clinical candidates. This perspective paper outlines the usefulness and applications of FBDD approaches in medicinal chemistry and drug design.


Asunto(s)
Química Farmacéutica , Descubrimiento de Drogas , Bibliotecas de Moléculas Pequeñas/química , Bibliotecas de Moléculas Pequeñas/farmacología , Estructura Molecular , Proteínas/antagonistas & inhibidores , Proteínas/química , Bibliotecas de Moléculas Pequeñas/síntesis química
11.
ACS Comb Sci ; 18(5): 225-9, 2016 05 09.
Artículo en Inglés | MEDLINE | ID: mdl-27073985

RESUMEN

A versatile palladium-catalyzed tandem synthetic sequence to afford E-stilbenes libraries has been developed. Excellent regio- and stereocontrol have been achieved by means of the sequence of Hiyama and Heck cross-couplings. Undesirable homocoupling byproducts were avoided employing immobilized substrates.


Asunto(s)
Paladio/química , Bibliotecas de Moléculas Pequeñas/síntesis química , Estilbenos/síntesis química , Catálisis
12.
Bioorg Med Chem Lett ; 24(4): 1052-6, 2014 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-24484899

RESUMEN

Several molecules have been discovered that interfere with formation of bacterial biofilms, opening a new strategy for the development of more efficient treatments in case of antibiotic resistant bacteria. Amongst the most active compounds are some natural brominated furanones from marine algae Delisea pulchra that have proven to be able to control pathogenic biofilms. We have recently reported that some rubrolide analogues are able to inhibit biofilm formation of Enterococcus faecalis. In the present Letter we describe results of the biological evaluation of a small library of 28 compounds including brominated furanones and the corresponding lactams against biofilm formation of Staphylococcus aureus, Pseudomonas aeruginosa, Staphylococcus epidermidis and Streptococcus mutans. Our results showed that in general these compounds were more active against biofilms of S. epidermidis and P. aeruginosa, with little or no inhibition of planktonic bacterial growth. In some cases they were able to prevent biofilm formation of P. aeruginosa at concentrations as low as 0.6 µg/mL (1.3 µM, compound 3d) and 0.7 µg/mL (1.3 µM, 3f). Results also indicate that, in general, lactams are more active against biofilms than their precursors, thus designating this class of molecules as good candidates for the development of a new generation of antimicrobial drugs targeted to biofilm inhibition.


Asunto(s)
Antibacterianos/farmacología , Biopelículas/efectos de los fármacos , Furanos/farmacología , Lactonas/farmacología , Bibliotecas de Moléculas Pequeñas/farmacología , Antibacterianos/síntesis química , Antibacterianos/química , Relación Dosis-Respuesta a Droga , Furanos/síntesis química , Furanos/química , Lactonas/síntesis química , Lactonas/química , Pruebas de Sensibilidad Microbiana , Estructura Molecular , Pseudomonas aeruginosa/efectos de los fármacos , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/química , Staphylococcus aureus/efectos de los fármacos , Staphylococcus epidermidis/efectos de los fármacos , Streptococcus mutans/efectos de los fármacos , Relación Estructura-Actividad
13.
Mol Divers ; 18(1): 1-12, 2014 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-24136658

RESUMEN

In this study, we report a strategy using dynamic combinatorial chemistry for targeting the thioredoxin (Trx)-reductase catalytic site on Trx glutathione reductase (TGR), a pyridine nucleotide thiol-disulfide oxido-reductase. We chose Echinococcus granulosus TGR since it is a bottleneck enzyme of platyhelminth parasites and a validated pharmacological target. A dynamic combinatorial library (DCL) was constructed based on thiol-disulfide reversible exchange. We demonstrate the use of 5-thio-2-nitrobenzoic acid (TNB) as a non-covalent anchor fragment in a DCL templated by E. granulosus TGR. The heterodimer of TNB and bisthiazolidine (2af) was identified, upon library analysis by HPLC (IC50 = 24 µM). Furthermore, 14 analogs were synthetically prepared and evaluated against TGR. This allowed the study of a structure-activity relationship and the identification of a disulfide TNB-tricyclic bisthiazolidine (2aj) as the best enzyme inhibitor in these series, with an IC50 = 24 µM. Thus, our results validate the use of DCL for targeting thiol-disulfide oxido-reductases.


Asunto(s)
Dominio Catalítico , Técnicas Químicas Combinatorias , Descubrimiento de Drogas , Echinococcus granulosus/enzimología , Inhibidores Enzimáticos/farmacología , Complejos Multienzimáticos/antagonistas & inhibidores , NADH NADPH Oxidorreductasas/antagonistas & inhibidores , Animales , Dimerización , Inhibidores Enzimáticos/síntesis química , Inhibidores Enzimáticos/química , Concentración 50 Inhibidora , Complejos Multienzimáticos/química , NADH NADPH Oxidorreductasas/química , Nitrobenzoatos/química , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/química , Bibliotecas de Moléculas Pequeñas/farmacología , Relación Estructura-Actividad , Compuestos de Sulfhidrilo/química , Tiazolidinas/síntesis química , Tiazolidinas/química , Tiazolidinas/farmacología
14.
Bioorg Med Chem ; 21(14): 4225-32, 2013 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-23721916

RESUMEN

A small library of compounds was prepared by a combination of toluene dioxygenase (TDO)-catalyzed enzymatic dihydroxylation and copper(I)-catalyzed Hüisgen cycloaddition. Some compounds were obtained by coupling an alkyne and a conduritol derivative, while more complex structures were obtained by a double Hüisgen reaction of a dialkyne and two molecules of the cyclitol. The compounds were fully characterized and subjected to preliminary biological screening.


Asunto(s)
Ciclitoles/síntesis química , Ciclitoles/farmacología , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/farmacología , Animales , Antifúngicos/síntesis química , Antifúngicos/química , Antifúngicos/farmacología , Proliferación Celular/efectos de los fármacos , Células Cultivadas , Ciclitoles/química , Reacción de Cicloadición , Inmunosupresores/síntesis química , Inmunosupresores/química , Inmunosupresores/farmacología , Masculino , Ratones , Ratones Endogámicos C57BL , Estructura Molecular , Bibliotecas de Moléculas Pequeñas/química , Triazoles/síntesis química , Triazoles/química , Triazoles/farmacología
15.
ACS Comb Sci ; 15(6): 320-30, 2013 Jun 10.
Artículo en Inglés | MEDLINE | ID: mdl-23573787

RESUMEN

The diversity-oriented synthesis of novel bis-spirostanic conjugates utilizing two different Ugi four-component reactions (Ugi-4CR) is described. Spirostanic steroids were functionalized with Ugi-reactive groups, that is, amines, isocyanides, and carboxylic acids, and next were subjected to multicomponent ligation approaches leading to bis-steroidal conjugates featuring pseudo-peptidic and heterocyclic linkage moieties. Both the classic Ugi-4CR and its hydrazoic acid variant were implemented, proving good efficiency for the ligation of isocyanosteroids to spirostanic acids and equatorial amines. Axially oriented amines showed poorer results, although model studies proved that chemical efficiency could be significantly improved while increasing reaction times. Overall, the method comprises the rapid generation of molecular diversity at the bis-steroid linkage moiety and, consequently, shows promise toward the production of combinatorial libraries of bis-spirostanes for biological screening.


Asunto(s)
Técnicas Químicas Combinatorias/métodos , Bibliotecas de Moléculas Pequeñas/síntesis química , Espirostanos/síntesis química , Química Farmacéutica , Estructura Molecular , Bibliotecas de Moléculas Pequeñas/química , Espirostanos/química , Estereoisomerismo
16.
Bioorg Med Chem Lett ; 22(4): 1712-5, 2012 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-22248858

RESUMEN

A series of 25 N,N'-substituted diamines were prepared by controlled reductive amination of free aliphatic diamines with different substituted benzaldehydes. The library was screened in vitro for antiparasitic activity on the causative agents of human African trypanosomiasis, Chagas' disease and visceral leishmaniasis. The most potent compounds were derived from a subset of diamines that contained a 4-OBn substitution, having a 50% parasite growth inhibition in the submicromolar (against Trypanosoma cruzi) or nanomolar (against Trypanosoma brucei and Leishmania donovani) range. We conclude that members of this series of N,N'-substituted diamines provide new lead structures that have potential to treat trypanosomal and leishmanial infections.


Asunto(s)
Antiprotozoarios/síntesis química , Antiprotozoarios/farmacología , Diaminas/síntesis química , Diaminas/farmacología , Kinetoplastida/efectos de los fármacos , Animales , Enfermedad de Chagas/tratamiento farmacológico , Diaminas/química , Humanos , Concentración 50 Inhibidora , Leishmaniasis Visceral/tratamiento farmacológico , Estructura Molecular , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/química , Bibliotecas de Moléculas Pequeñas/farmacología , Tripanosomiasis Africana/tratamiento farmacológico
17.
Mol Divers ; 15(4): 1017-24, 2011 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-21633789

RESUMEN

Looking for new active molecules against Mycobacterium tuberculosis, a small focused library of 1,2,3-triazoles was efficiently prepared by click chemistry. Compounds were subsequently tested against different pathogenic and opportunistic mycobacteria including M. avium and M. tuberculosis. Two of them showed MIC at lower µg/mL concentration for M. avium and even below that for M. tuberculosis, being more potent that control drugs.


Asunto(s)
Mycobacterium avium/efectos de los fármacos , Mycobacterium tuberculosis/efectos de los fármacos , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/farmacología , Triazoles/síntesis química , Triazoles/farmacología , Química Clic , Pruebas de Sensibilidad Microbiana , Bibliotecas de Moléculas Pequeñas/química , Triazoles/química
18.
Eur J Med Chem ; 45(12): 5767-72, 2010 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-20889239

RESUMEN

Triosephosphate isomerase from Trypanosoma cruzi (TcTIM), an enzyme in the glycolytic pathway that exhibits high catalytic rates of glyceraldehyde-3-phosphate- and dihydroxyacetone-phosphate-isomerization only in its dimeric form, was screened against an in-house chemical library containing nearly 230 compounds belonging to different chemotypes. After secondary screening, twenty-six compounds from eight different chemotypes were identified as screening positives. Four compounds displayed selectivity for TcTIM over TIM from Homo sapiens and, concomitantly, in vitro activity against T. cruzi.


Asunto(s)
Inhibidores Enzimáticos/farmacología , Bibliotecas de Moléculas Pequeñas/farmacología , Triosa-Fosfato Isomerasa/antagonistas & inhibidores , Tripanocidas/farmacología , Trypanosoma cruzi/efectos de los fármacos , Dimerización , Inhibidores Enzimáticos/síntesis química , Inhibidores Enzimáticos/química , Modelos Moleculares , Estructura Molecular , Pruebas de Sensibilidad Parasitaria , Bibliotecas de Moléculas Pequeñas/síntesis química , Bibliotecas de Moléculas Pequeñas/química , Estereoisomerismo , Relación Estructura-Actividad , Tripanocidas/síntesis química , Tripanocidas/química , Trypanosoma cruzi/enzimología
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