Gelation-driven component selection in the generation of constitutional dynamic hydrogels based on guanine-quartet formation.

Abstract:

:The guanosine hydrazide 1 yields a stable supramolecular hydrogel based on the formation of a guanine quartet (G-quartet) in presence of metal cations. The effect of various parameters (concentration, nature of metal ion, and temperature) on the properties of this gel has been studied. Proton NMR spectroscopy is shown to allow a molecular characterization of the gelation process. Hydrazide 1 and its assemblies can be reversibly decorated by acylhydrazone formation with various aldehydes, resulting in formation of highly viscous dynamic hydrogels. When a mixture of aldehydes is used, the dynamic system selects the aldehyde that leads to the most stable gel. Mixing hydrazides 1, 9 and aldehydes 6, 8 in 1:1:1:1 ratio generated a constitutional dynamic library containing the four acylhydrazone derivatives A, B, C, and D. The library constitution displayed preferential formation of the acylhydrazone B that yields the strongest gel. Thus, gelation redirects the acylhydrazone distribution in the dynamic library as guanosine hydrazide 1 scavenges preferentially aldehyde 8, under the pressure of gelation because of the collective interactions in the assemblies of G-quartets B, despite the strong preference of the competing hydrazide 9 for 8. Gel formation and component selection are thermoreversible. The process amounts to gelation-driven self-organization with component selection and amplification in constitutional dynamic hydrogels based on G-quartet formation and reversible covalent connections. The observed self-organization and component selection occur by means of a multilevel self-assembly involving three dynamic processes, two of supramolecular and one of reversible covalent nature. They extend constitutional dynamic chemistry to phase-organization and phase-transition events.

authors

Sreenivasachary N,Lehn JM

doi

10.1073/pnas.0501663102

keywords:

subject

Has Abstract

pub_date

2005-04-26 00:00:00

pages

5938-43

issue

17

eissn

0027-8424

issn

1091-6490

pii

0501663102

journal_volume

102

pub_type

杂志文章
  • mRNAs encoding ribulose-1,5-bisphosphate carboxylase remain bound to polysomes but are not translated in amaranth seedlings transferred to darkness.

    abstract::When light-grown seedlings of amaranth are transferred to total darkness, synthesis of the large subunit (LS) and small subunit (SS) of ribulose-1,5-bisphosphate carboxylase [RbuP(2)Case; 3-phospho-D-glycerate carboxylase (dimerizing), EC 4.1.1.39] is rapidly depressed. This reduction in RbuP(2)Case synthesis occurs i...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.85.12.4190

    authors: Berry JO,Carr JP,Klessig DF

    更新日期:1988-06-01 00:00:00

  • Insulin-like growth factors 1 and 2 induce lymphangiogenesis in vivo.

    abstract::Lymphangiogenesis is an important process that contributes to the spread of cancer. Here we show that insulin-like growth factors 1 (IGF-1) and 2 (IGF-2) induce lymphangiogenesis in vivo. In a mouse cornea assay, IGF-1 and IGF-2 induce lymphangiogenesis as detected with LYVE-1, a specific marker for lymphatic endothel...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0507865102

    authors: Björndahl M,Cao R,Nissen LJ,Clasper S,Johnson LA,Xue Y,Zhou Z,Jackson D,Hansen AJ,Cao Y

    更新日期:2005-10-25 00:00:00

  • Transposon tagging of tobacco mosaic virus resistance gene N: its possible role in the TMV-N-mediated signal transduction pathway.

    abstract::Plants can recognize and resist invading pathogens by signaling the induction of rapid defense responses. Often these responses are mediated by single dominant resistance genes (R genes). The products of R genes have been postulated to recognize the pathogen and trigger rapid host defense responses. Here we describe i...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.92.10.4175

    authors: Dinesh-Kumar SP,Whitham S,Choi D,Hehl R,Corr C,Baker B

    更新日期:1995-05-09 00:00:00

  • Evidence for intron capture: an unusual path for the evolution of proteins.

    abstract::Most new genes are thought to evolve from preexisting genes but duplications of entire genes or shuffling of preexisting exons provides only a limited repertoire of new sequences that can be presented to a cell. Only pieces that previously existed can be used in the construction and any further divergence depends on t...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.91.16.7506

    authors: Golding GB,Tsao N,Pearlman RE

    更新日期:1994-08-02 00:00:00

  • Vortices and turbulence in trapped atomic condensates.

    abstract::After more than a decade of experiments generating and studying the physics of quantized vortices in atomic gas Bose-Einstein condensates, research is beginning to focus on the roles of vortices in quantum turbulence, as well as other measures of quantum turbulence in atomic condensates. Such research directions have ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1312737110

    authors: White AC,Anderson BP,Bagnato VS

    更新日期:2014-03-25 00:00:00

  • Xenopus oocyte germinal-vesicle breakdown induced by [Val12]Ras is inhibited by a cytosol-localized Ras mutant.

    abstract::The GTPase-activating protein (GAP) has been postulated to function either as a negative regulator or as a possible target protein of Ras in mammalian cells and Xenopus oocytes. Ras must be localized in the plasma membrane of vertebrate cells to function, but GAP is localized in the cytosol. To test whether Ras functi...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.86.17.6630

    authors: Gibbs JB,Schaber MD,Schofield TL,Scolnick EM,Sigal IS

    更新日期:1989-09-01 00:00:00

  • Reciprocal effects of an inhibitory factor on catalytic activity and noncatalytic cGMP binding sites of rod phosphodiesterase.

    abstract::In illuminated rod outer segment membranes, GTP and guanosine 5'-[beta, gamma-imido]triphosphate (p[NH]ppG) have reciprocal effects on cGMP phosphodiesterase (PDEase; 3':5'-cyclic-nucleotide 5'-nucleotidohydrolase, EC 3.1.4.17) activity and cGMP binding to noncatalytic sites on that enzyme. Two micromolar p[NH]ppG inc...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.79.12.3702

    authors: Yamazaki A,Bartucca F,Ting A,Bitensky MW

    更新日期:1982-06-01 00:00:00

  • Functional cavitands: chemical reactivity in structured environments.

    abstract::Container-shaped molecules provide structured environments that impart geometric bounds on the motions and conformations of smaller molecular occupants. Moreover, they provide "solvation" that is constrained in time and space. When inwardly directed functional groups are present, they can interact chemically with the ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章,评审

    doi:10.1073/pnas.0501731102

    authors: Purse BW,Rebek J Jr

    更新日期:2005-08-02 00:00:00

  • Picosecond primary structural transition of the heme is retarded after nitric oxide binding to heme proteins.

    abstract::We investigated the ultrafast structural transitions of the heme induced by nitric oxide (NO) binding for several heme proteins by subpicosecond time-resolved resonance Raman and femtosecond transient absorption spectroscopy. We probed the heme iron motion by the evolution of the iron-histidine Raman band intensity af...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0912938107

    authors: Kruglik SG,Yoo BK,Franzen S,Vos MH,Martin JL,Negrerie M

    更新日期:2010-08-03 00:00:00

  • Quantitative MS-based enzymology of caspases reveals distinct protein substrate specificities, hierarchies, and cellular roles.

    abstract::Proteases constitute the largest enzyme family, yet their biological roles are obscured by our rudimentary understanding of their cellular substrates. There are 12 human caspases that play crucial roles in inflammation and cell differentiation and drive the terminal stages of cell death. Recent N-terminomics technolog...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1524900113

    authors: Julien O,Zhuang M,Wiita AP,O'Donoghue AJ,Knudsen GM,Craik CS,Wells JA

    更新日期:2016-04-05 00:00:00

  • The neural origins of shell structure and pattern in aquatic mollusks.

    abstract::We present a model to explain how the neurosecretory system of aquatic mollusks generates their diversity of shell structures and pigmentation patterns. The anatomical and physiological basis of this model sets it apart from other models used to explain shape and pattern. The model reproduces most known shell shapes a...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0810311106

    authors: Boettiger A,Ermentrout B,Oster G

    更新日期:2009-04-21 00:00:00

  • A systematic study of low-resolution recognition in protein--protein complexes.

    abstract::A comprehensive nonredundant database of 475 cocrystallized protein-protein complexes was used to study low-resolution recognition, which was reported in earlier docking experiments with a small number of proteins. The docking program GRAMM was used to delete the atom-size structural details and systematically dock th...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.96.15.8477

    authors: Vakser IA,Matar OG,Lam CF

    更新日期:1999-07-20 00:00:00

  • Unveiling functional protein motions with picosecond x-ray crystallography and molecular dynamics simulations.

    abstract::A joint analysis of all-atom molecular dynamics (MD) calculations and picosecond time-resolved x-ray structures was performed to gain single-molecule insights into mechanisms of protein function. Ensemble-averaged MD simulations of the L29F mutant of myoglobin after ligand dissociation reproduce the direction, amplitu...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0405295101

    authors: Hummer G,Schotte F,Anfinrud PA

    更新日期:2004-10-26 00:00:00

  • Immunostimulatory oligodeoxynucleotides containing the CpG motif are effective as immune adjuvants in tumor antigen immunization.

    abstract::Recent advances in our understanding of the immune response are allowing for the logical design of new approaches to cancer immunization. One area of interest is the development of new immune adjuvants. Immunostimulatory oligodeoxynucleotides containing the CpG motif (CpG ODN) can induce production of a wide variety o...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.94.20.10833

    authors: Weiner GJ,Liu HM,Wooldridge JE,Dahle CE,Krieg AM

    更新日期:1997-09-30 00:00:00

  • Photoincorporation of puromycin and N-(ethyl-2-diazomalonyl)puromycin into Escherichia coli ribosomes.

    abstract::[3H]Puromycin and N-(ethyl-2-diazomalonyl)[3H]puromycin are incorporated into E. coli ribosomes on irradiation at 253.7 nm. Both compounds incorporate into both protein and nucleic acid. Two-dimensional gel electrophoresis of ribosomal protein shows that L23 is the major protein labeled by puromycin. Although incorpor...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.72.8.2974

    authors: Cooperman BS,Jaynes EN,Brunswick DJ,Luddy MA

    更新日期:1975-08-01 00:00:00

  • Building more accurate decision trees with the additive tree.

    abstract::The expansion of machine learning to high-stakes application domains such as medicine, finance, and criminal justice, where making informed decisions requires clear understanding of the model, has increased the interest in interpretable machine learning. The widely used Classification and Regression Trees (CART) have ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1816748116

    authors: Luna JM,Gennatas ED,Ungar LH,Eaton E,Diffenderfer ES,Jensen ST,Simone CB 2nd,Friedman JH,Solberg TD,Valdes G

    更新日期:2019-10-01 00:00:00

  • Evolution of sociality in a primitively eusocial lineage of bees.

    abstract::Eusociality is a major evolutionary innovation involving alterations in life history, morphology, and behavior. Advanced eusocial insects, such as ants, termites, and corbiculate bees, cannot provide insights into the earliest stages of eusocial evolution because eusociality in these taxa evolved long ago (in the Cret...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.012387999

    authors: Danforth BN

    更新日期:2002-01-08 00:00:00

  • Label-free Raman observation of cytochrome c dynamics during apoptosis.

    abstract::We performed label-free observation of molecular dynamics in apoptotic cells by Raman microscopy. Dynamic changes in cytochrome c distribution at the Raman band of 750 cm(-1) were observed after adding an apoptosis inducer to the cells. The comparison of mitochondria fluorescence images and Raman images of cytochrome ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1107524108

    authors: Okada M,Smith NI,Palonpon AF,Endo H,Kawata S,Sodeoka M,Fujita K

    更新日期:2012-01-03 00:00:00

  • Postsynaptic alpha-adrenergic receptors potentiate the beta-adrenergic stimulation of pineal serotonin N-acetyltransferase.

    abstract::The role played by postsynaptic alpha-adrenergic receptors in the stimulation of pineal N-acetyltransferase (EC 2.3.1.5) and [3H]melatonin production was investigated in the rat. In vivo studies indicated that phenylephrine, an alpha-adrenergic agonist, potentiated and prolonged the effects of isoproterenol, a beta-ad...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.80.2.599

    authors: Klein DC,Sugden D,Weller JL

    更新日期:1983-01-01 00:00:00

  • Protein folding under confinement: a role for solvent.

    abstract::Although most experimental and theoretical studies of protein folding involve proteins in vitro, the effects of spatial confinement may complicate protein folding in vivo. In this study, we examine the folding dynamics of villin (a small fast folding protein) with explicit solvent confined to an inert nanopore. We hav...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0608256104

    authors: Lucent D,Vishal V,Pande VS

    更新日期:2007-06-19 00:00:00

  • Chromosome 14 transfer and functional studies identify a candidate tumor suppressor gene, mirror image polydactyly 1, in nasopharyngeal carcinoma.

    abstract::Chromosome 14 allelic loss is common in nasopharyngeal carcinoma (NPC) and may reflect essential tumor suppressor gene loss in tumorigenesis. An intact chromosome 14 was transferred to an NPC cell line using a microcell-mediated chromosome transfer approach. Microcell hybrids (MCHs) containing intact exogenously trans...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0900198106

    authors: Cheung AK,Lung HL,Ko JM,Cheng Y,Stanbridge EJ,Zabarovsky ER,Nicholls JM,Chua D,Tsao SW,Guan XY,Lung ML

    更新日期:2009-08-25 00:00:00

  • Involvement of wild-type p53 in pre-B-cell differentiation in vitro.

    abstract::Wild-type p53 protein is a growth modulator whose inactivation has been found to be a key event in malignant transformation. Reconstitution of wild-type p53 in the p53-nonproducer, Abelson murine leukemia virus-transformed pre-B-cell line L12 gave rise to stably growing clones. Wild-type p53-producer derived cell line...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.88.20.8982

    authors: Shaulsky G,Goldfinger N,Peled A,Rotter V

    更新日期:1991-10-15 00:00:00

  • Silencing of tryptamine biosynthesis for production of nonnatural alkaloids in plant culture.

    abstract::Natural products have long served as both a source and inspiration for pharmaceuticals. Modifying the structure of a natural product often improves the biological activity of the compound. Metabolic engineering strategies to ferment "unnatural" products have been enormously successful in microbial organisms. However, ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0903393106

    authors: Runguphan W,Maresh JJ,O'Connor SE

    更新日期:2009-08-18 00:00:00

  • Modified recombination and transmission of mitochondrial genetic markers in rho minus mutants of Saccharomyces cerevisiae.

    abstract::A large number of primary petite (rho-) clones were isolated after ethidium bromide mutagenesis of various grande (rho+) strains of S. cerevisiae that contained the mitochondrial genetic markers, CR, ER, OIR (or OIIR), and PR. From the frequency of coretention of markers in the petites, we have deduced a probable circ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.73.12.4608

    authors: Boltin-Fukuhara M,Fukuhara H

    更新日期:1976-12-01 00:00:00

  • Sumoylation of heterogeneous nuclear ribonucleoproteins, zinc finger proteins, and nuclear pore complex proteins: a proteomic analysis.

    abstract::SUMO, a small ubiquitin-related modifier, is known to covalently attach to a number of nuclear regulatory proteins such as p53, IkappaB, promyelocytic leukemia protein and c-Jun. The sumoylation reaction is catalyzed by the SUMO protease, which exposes the C-terminal active glycine residue of the nascent SUMO, the het...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0402889101

    authors: Li T,Evdokimov E,Shen RF,Chao CC,Tekle E,Wang T,Stadtman ER,Yang DC,Chock PB

    更新日期:2004-06-08 00:00:00

  • Regulated expression of endonuclease EcoRI in Saccharomyces cerevisiae: nuclear entry and biological consequences.

    abstract::In an investigation to determine how proteins are localized within the nucleus of a cell, we demonstrate that the restriction endonuclease EcoRI is able to enter and function within the nucleus of Saccharomyces cerevisiae when this prokaryotic protein is synthesized in vivo. The EcoRI endonuclease was produced in yeas...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.82.5.1354

    authors: Barnes G,Rine J

    更新日期:1985-03-01 00:00:00

  • Neonicotinoid insecticides induce salicylate-associated plant defense responses.

    abstract::Neonicotinoid insecticides control crop pests based on their action as agonists at the insect nicotinic acetylcholine receptor, which accepts chloropyridinyl- and chlorothiazolyl-analogs almost equally well. In some cases, these compounds have also been reported to enhance plant vigor and (a)biotic stress tolerance, i...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1013020107

    authors: Ford KA,Casida JE,Chandran D,Gulevich AG,Okrent RA,Durkin KA,Sarpong R,Bunnelle EM,Wildermuth MC

    更新日期:2010-10-12 00:00:00

  • Phylogenomics reveals rapid, simultaneous diversification of three major clades of Gondwanan frogs at the Cretaceous-Paleogene boundary.

    abstract::Frogs (Anura) are one of the most diverse groups of vertebrates and comprise nearly 90% of living amphibian species. Their worldwide distribution and diverse biology make them well-suited for assessing fundamental questions in evolution, ecology, and conservation. However, despite their scientific importance, the evol...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1704632114

    authors: Feng YJ,Blackburn DC,Liang D,Hillis DM,Wake DB,Cannatella DC,Zhang P

    更新日期:2017-07-18 00:00:00

  • Structural insight on the recognition of surface-bound opsonins by the integrin I domain of complement receptor 3.

    abstract::Complement receptors (CRs), expressed notably on myeloid and lymphoid cells, play an essential function in the elimination of complement-opsonized pathogens and apoptotic/necrotic cells. In addition, these receptors are crucial for the cross-talk between the innate and adaptive branches of the immune system. CR3 (also...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1311261110

    authors: Bajic G,Yatime L,Sim RB,Vorup-Jensen T,Andersen GR

    更新日期:2013-10-08 00:00:00

  • Structural bases for F plasmid conjugation and F pilus biogenesis in Escherichia coli.

    abstract::Bacterial conjugation systems are members of the large type IV secretion system (T4SS) superfamily. Conjugative transfer of F plasmids residing in the Enterobacteriaceae was first reported in the 1940s, yet the architecture of F plasmid-encoded transfer channel and its physical relationship with the F pilus remain unk...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1904428116

    authors: Hu B,Khara P,Christie PJ

    更新日期:2019-07-09 00:00:00