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  • Glucose-responsive insulin by molecular and physical design
    Nat. Chem. (IF 25.87) Pub Date : 
    Naveed A. Bakh, Abel B. Cortinas, Michael A. Weiss, Robert S. Langer, Daniel G. Anderson, Zhen Gu, Sanjoy Dutta, Michael S. Strano

    Glucose-responsive insulin by molecular and physical design Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2857 Glucose-responsive insulin is a therapeutic that modulates its potency, concentration or dosing relative to a patient’s dynamic glucose concentration. This Perspective summarizes some of the recent accomplishments in this field as well as discussing new computational algorithms that may aid in the development of such therapeutics.

    更新日期:2017-09-22
  • The darmstadtium cornerstone
    Nat. Chem. (IF 25.87) Pub Date : 
    Dieter Ackermann

    The darmstadtium cornerstone Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2867 Dieter Ackermann explains why element 110 occupies a significant place in the superheavy corner of the periodic table.

    更新日期:2017-09-22
  • Nucleic acid nanomaterials: Silver-wired DNA
    Nat. Chem. (IF 25.87) Pub Date : 
    Pascal Auffinger, Eric Ennifar

    Nucleic acid nanomaterials: Silver-wired DNA Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2869 DNA double helical structures are supramolecular assemblies that are typically held together by classical Watson–Crick pairing. Now, nucleotide chelation of silver ions supports an extended silver–DNA hybrid duplex featuring an uninterrupted silver array.

    更新日期:2017-09-22
  • Synthesis and the Nobel Prize in Chemistry
    Nat. Chem. (IF 25.87) Pub Date : 
    Jeffrey I. Seeman

    Synthesis and the Nobel Prize in Chemistry Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2864 The question often arises as to who may have deserved a Nobel Prize but was not awarded one. Rarely is this discussion extended to who should have received more than one Nobel Prize, but in the field of organic synthesis there are some compelling candidates.

    更新日期:2017-09-22
  • Water dynamics: Gliding and trudging
    Nat. Chem. (IF 25.87) Pub Date : 
    Yoshimitsu Itoh, Takuzo Aida

    Water dynamics: Gliding and trudging Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2870 Water is increasingly recognized as being of paramount importance in biological processes, yet its exact role remains difficult to elucidate. Now, the motion of water molecules within and around a synthetic peptide-amphiphile nanofibre has been precisely determined, showing significant differences between its core and surface.

    更新日期:2017-09-22
  • Reaction dynamics: The view from a transition state
    Nat. Chem. (IF 25.87) Pub Date : 
    Robert E. Continetti

    Reaction dynamics: The view from a transition state Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2868 Ejecting electrons from negative ions using light can create structures that very closely resemble the transition states of bimolecular reactions. Now, using this technique, trapped quantum states, or 'resonances', have been observed in a seven-atom reaction, and theory has been shown to be up to the task of capturing such complex phenomena.

    更新日期:2017-09-22
  • Glucose-responsive insulin by molecular and physical design
    Nat. Chem. (IF 25.87) Pub Date : 
    Naveed A. Bakh, Abel B. Cortinas, Michael A. Weiss, Robert S. Langer, Daniel G. Anderson, Zhen Gu, Sanjoy Dutta, Michael S. Strano

    Glucose-responsive insulin by molecular and physical design Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2857 Glucose-responsive insulin is a therapeutic that modulates its potency, concentration or dosing relative to a patient’s dynamic glucose concentration. This Perspective summarizes some of the recent accomplishments in this field as well as discussing new computational algorithms that may aid in the development of such therapeutics.

    更新日期:2017-09-22
  • The darmstadtium cornerstone
    Nat. Chem. (IF 25.87) Pub Date : 
    Dieter Ackermann

    The darmstadtium cornerstone Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2867 Dieter Ackermann explains why element 110 occupies a significant place in the superheavy corner of the periodic table.

    更新日期:2017-09-22
  • Nucleic acid nanomaterials: Silver-wired DNA
    Nat. Chem. (IF 25.87) Pub Date : 
    Pascal Auffinger, Eric Ennifar

    Nucleic acid nanomaterials: Silver-wired DNA Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2869 DNA double helical structures are supramolecular assemblies that are typically held together by classical Watson–Crick pairing. Now, nucleotide chelation of silver ions supports an extended silver–DNA hybrid duplex featuring an uninterrupted silver array.

    更新日期:2017-09-22
  • Synthesis and the Nobel Prize in Chemistry
    Nat. Chem. (IF 25.87) Pub Date : 
    Jeffrey I. Seeman

    Synthesis and the Nobel Prize in Chemistry Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2864 The question often arises as to who may have deserved a Nobel Prize but was not awarded one. Rarely is this discussion extended to who should have received more than one Nobel Prize, but in the field of organic synthesis there are some compelling candidates.

    更新日期:2017-09-22
  • Water dynamics: Gliding and trudging
    Nat. Chem. (IF 25.87) Pub Date : 
    Yoshimitsu Itoh, Takuzo Aida

    Water dynamics: Gliding and trudging Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2870 Water is increasingly recognized as being of paramount importance in biological processes, yet its exact role remains difficult to elucidate. Now, the motion of water molecules within and around a synthetic peptide-amphiphile nanofibre has been precisely determined, showing significant differences between its core and surface.

    更新日期:2017-09-22
  • Reaction dynamics: The view from a transition state
    Nat. Chem. (IF 25.87) Pub Date : 
    Robert E. Continetti

    Reaction dynamics: The view from a transition state Nature Chemistry, Published online: 22 September 2017; doi:10.1038/nchem.2868 Ejecting electrons from negative ions using light can create structures that very closely resemble the transition states of bimolecular reactions. Now, using this technique, trapped quantum states, or 'resonances', have been observed in a seven-atom reaction, and theory has been shown to be up to the task of capturing such complex phenomena.

    更新日期:2017-09-22
  • Bioinspired chemical synthesis of monomeric and dimeric stephacidin A congeners
    Nat. Chem. (IF 25.87) Pub Date : 
    Ken Mukai, Danilo Pereira de Sant'Ana, Yasuo Hirooka, Eduardo V. Mercado-Marin, David E. Stephens, Kevin G. M. Kou, Sven C. Richter, Naomi Kelley, Richmond Sarpong

    Stephacidin A and its congeners are a collection of secondary metabolites that possess intriguing structural motifs. They stem from unusual biosynthetic sequences that lead to the incorporation of a prenyl or reverse-prenyl group into a bicyclo[2.2.2]diazaoctane framework, a chromene unit or the vestige thereof. To complement biosynthetic studies, which normally play a significant role in unveiling the biosynthetic pathways of natural products, here we demonstrate that chemical synthesis can provide important insights into biosynthesis. We identify a short total synthesis of congeners in the reverse-prenylated indole alkaloid family related to stephacidin A by taking advantage of a direct indole C6 halogenation of the related ketopremalbrancheamide. This novel strategic approach has now made possible the syntheses of several natural products, including malbrancheamides B and C, notoamides F, I and R, aspergamide B, and waikialoid A, which is a heterodimer of avrainvillamide and aspergamide B. Our approach to the preparation of these prenylated and reverse-prenylated indole alkaloids is bioinspired, and may also inform the as-yet undetermined biosynthesis of several congeners.

    更新日期:2017-09-20
  • Bioinspired chemical synthesis of monomeric and dimeric stephacidin A congeners
    Nat. Chem. (IF 25.87) Pub Date : 2017-09-18
    Ken Mukai, Danilo Pereira de Sant'Ana, Yasuo Hirooka, Eduardo V. Mercado-Marin, David E. Stephens, Kevin G. M. Kou, Sven C. Richter, Naomi Kelley, Richmond Sarpong
    更新日期:2017-09-20
  • Late-stage chemoselective functional-group manipulation of bioactive natural products with super-electrophilic silylium ions
    Nat. Chem. (IF 25.87) Pub Date : 2017-09-18
    Trandon A. Bender, Philippa R. Payne, Michel R. Gagné
    更新日期:2017-09-18
  • Designing cooperatively folded abiotic uni- and multimolecular helix bundles
    Nat. Chem. (IF 25.87) Pub Date : 2017-09-18
    Soumen De, Bo Chi, Thierry Granier, Ting Qi, Victor Maurizot, Ivan Huc
    更新日期:2017-09-18
  • Late-stage chemoselective functional-group manipulation of bioactive natural products with super-electrophilic silylium ions
    Nat. Chem. (IF 25.87) Pub Date : 
    Trandon A. Bender, Philippa R. Payne, Michel R. Gagné

    Late-stage chemoselective functional-group manipulation of bioactive natural products with super-electrophilic silylium ions Nature Chemistry, Published online: 18 September 2017; doi:10.1038/nchem.2863 Determining the structure­–activity relationships for complex structures can be quite challenging, but it is often the method in which many natural products can be used as drugs. Now, the combination of a fluoroaryl borane catalyst, a phosphine additive and a silane reducing agent enables the late-stage selective modification of complex bioactive natural products.

    更新日期:2017-09-18
  • Designing cooperatively folded abiotic uni- and multimolecular helix bundles
    Nat. Chem. (IF 25.87) Pub Date : 
    Soumen De, Bo Chi, Thierry Granier, Ting Qi, Victor Maurizot, Ivan Huc

    Designing cooperatively folded abiotic uni- and multimolecular helix bundles Nature Chemistry, Published online: 18 September 2017; doi:10.1038/nchem.2854 Rationally designed arrays of hydrogen bonds between aromatic oligoamide segments have now been shown to generate abiotic helix-turn-helix and unexpected dimeric and trimeric helix bundle motifs. These structures show kinetic and thermodynamic stability, and cooperative folding in nonpolar solvents.

    更新日期:2017-09-18
  • Chromophore twisting in the excited state of a photoswitchable fluorescent protein captured by time-resolved serial femtosecond crystallography
    Nat. Chem. (IF 25.87) Pub Date : 
    Nicolas Coquelle, Michel Sliwa, Joyce Woodhouse, Giorgio Schirò, Virgile Adam, Andrew Aquila, Thomas R. M. Barends, Sébastien Boutet, Martin Byrdin, Sergio Carbajo, Eugenio De la Mora, R. Bruce Doak, Mikolaj Feliks, Franck Fieschi, Lutz Foucar, Virginia Guillon, Mario Hilpert, Mark S. Hunter, Stefan Jakobs, Jason E. Koglin, Gabriela Kovacsova, Thomas J. Lane, Bernard Lévy, Mengning Liang, Karol Nass, Jacqueline Ridard, Joseph S. Robinson, Christopher M. Roome, Cyril Ruckebusch, Matthew Seaberg, Michel Thepaut, Marco Cammarata, Isabelle Demachy, Martin Field, Robert L. Shoeman, Dominique Bourgeois, Jacques-Philippe Colletier, Ilme Schlichting, Martin Weik

    Chromophores absorb light in photosensitive proteins and thereby initiate fundamental biological processes such as photosynthesis, vision and biofluorescence. An important goal in their understanding is the provision of detailed structural descriptions of the ultrafast photochemical events that they undergo, in particular of the excited states that connect chemistry to biological function. Here we report on the structures of two excited states in the reversibly photoswitchable fluorescent protein rsEGFP2. We populated the states through femtosecond illumination of rsEGFP2 in its non-fluorescent off state and observed their build-up (within less than one picosecond) and decay (on the several picosecond timescale). Using an X-ray free-electron laser, we performed picosecond time-resolved crystallography and show that the hydroxybenzylidene imidazolinone chromophore in one of the excited states assumes a near-canonical twisted configuration halfway between the trans and cis isomers. This is in line with excited-state quantum mechanics/molecular mechanics and classical molecular dynamics simulations. Our new understanding of the structure around the twisted chromophore enabled the design of a mutant that displays a twofold increase in its off-to-on photoswitching quantum yield.

    更新日期:2017-09-12
  • Assembly of a biocompatible triazole-linked gene by one-pot click-DNA ligation
    Nat. Chem. (IF 25.87) Pub Date : 
    Mikiembo Kukwikila, Nittaya Gale, Afaf H. El-Sagheer, Tom Brown, Ali Tavassoli

    The chemical synthesis of oligonucleotides and their enzyme-mediated assembly into genes and genomes has significantly advanced multiple scientific disciplines. However, these approaches are not without their shortcomings; enzymatic amplification and ligation of oligonucleotides into genes and genomes makes automation challenging, and site-specific incorporation of epigenetic information and/or modified bases into large constructs is not feasible. Here we present a fully chemical one-pot method for the assembly of oligonucleotides into a gene by click-DNA ligation. We synthesize the 335 base-pair gene that encodes the green fluorescent protein iLOV from ten functionalized oligonucleotides that contain 5ʹ-azide and 3ʹ-alkyne units. The resulting click-linked iLOV gene contains eight triazoles at the sites of chemical ligation, and yet is fully biocompatible; it is replicated by DNA polymerases in vitro and encodes a functional iLOV protein in Escherichia coli. We demonstrate the power and potential of our one-pot gene-assembly method by preparing an epigenetically modified variant of the iLOV gene.

    更新日期:2017-09-12
  • Direct mapping of the angle-dependent barrier to reaction for Cl + CHD3 using polarized scattering data
    Nat. Chem. (IF 25.87) Pub Date : 
    Huilin Pan, Fengyan Wang, Gábor Czakó, Kopin Liu

    The transition state, which gates and modulates reactive flux, serves as the central concept in our understanding of activated reactions. The barrier height of the transition state can be estimated from the activation energy taken from thermal kinetics data or from the energetic threshold in the measured excitation function (the dependence of reaction cross-sections on initial collision energies). However, another critical and equally important property, the angle-dependent barrier to reaction, has not yet been amenable to experimental determination until now. Here, using the benchmark reaction of Cl + CHD3(v1 = 1) as an example, we show how to map this anisotropic property of the transition state as a function of collision energy from the preferred reactant bond alignment of the backward-scattered products—the imprints of small impact-parameter collisions. The deduced bend potential at the transition state agrees with ab initio calculations. We expect that the method should be applicable to many other direct reactions with a collinear barrier.

    更新日期:2017-09-12
  • Vibronically coherent ultrafast triplet-pair formation and subsequent thermally activated dissociation control efficient endothermic singlet fission
    Nat. Chem. (IF 25.87) Pub Date : 
    Hannah L. Stern, Alexandre Cheminal, Shane R. Yost, Katharina Broch, Sam L. Bayliss, Kai Chen, Maxim Tabachnyk, Karl Thorley, Neil Greenham, Justin M. Hodgkiss, John Anthony, Martin Head-Gordon, Andrew J. Musser, Akshay Rao, Richard H. Friend

    Singlet exciton fission (SF), the conversion of one spin-singlet exciton (S1) into two spin-triplet excitons (T1), could provide a means to overcome the Shockley–Queisser limit in photovoltaics. SF as measured by the decay of S1 has been shown to occur efficiently and independently of temperature, even when the energy of S1 is as much as 200 meV less than that of 2T1. Here we study films of triisopropylsilyltetracene using transient optical spectroscopy and show that the triplet pair state (TT), which has been proposed to mediate singlet fission, forms on ultrafast timescales (in 300 fs) and that its formation is mediated by the strong coupling of electronic and vibrational degrees of freedom. This is followed by a slower loss of singlet character as the excitation evolves to become only TT. We observe the TT to be thermally dissociated on 10–100 ns timescales to form free triplets. This provides a model for ‘temperature-independent’ efficient TT formation and thermally activated TT separation.

    更新日期:2017-09-12
  • Chromophore twisting in the excited state of a photoswitchable fluorescent protein captured by time-resolved serial femtosecond crystallography
    Nat. Chem. (IF 25.87) Pub Date : 
    Nicolas Coquelle, Michel Sliwa, Joyce Woodhouse, Giorgio Schirò, Virgile Adam, Andrew Aquila, Thomas R. M. Barends, Sébastien Boutet, Martin Byrdin, Sergio Carbajo, Eugenio De la Mora, R. Bruce Doak, Mikolaj Feliks, Franck Fieschi, Lutz Foucar, Virginia Guillon, Mario Hilpert, Mark S. Hunter, Stefan Jakobs, Jason E. Koglin, Gabriela Kovacsova, Thomas J. Lane, Bernard Lévy, Mengning Liang, Karol Nass, Jacqueline Ridard, Joseph S. Robinson, Christopher M. Roome, Cyril Ruckebusch, Matthew Seaberg, Michel Thepaut, Marco Cammarata, Isabelle Demachy, Martin Field, Robert L. Shoeman, Dominique Bourgeois, Jacques-Philippe Colletier, Ilme Schlichting, Martin Weik
    更新日期:2017-09-12
  • Assembly of a biocompatible triazole-linked gene by one-pot click-DNA ligation
    Nat. Chem. (IF 25.87) Pub Date : 
    Mikiembo Kukwikila, Nittaya Gale, Afaf H. El-Sagheer, Tom Brown, Ali Tavassoli
    更新日期:2017-09-12
  • Vibronically coherent ultrafast triplet-pair formation and subsequent thermally activated dissociation control efficient endothermic singlet fission
    Nat. Chem. (IF 25.87) Pub Date : 
    Hannah L. Stern, Alexandre Cheminal, Shane R. Yost, Katharina Broch, Sam L. Bayliss, Kai Chen, Maxim Tabachnyk, Karl Thorley, Neil Greenham, Justin M. Hodgkiss, John Anthony, Martin Head-Gordon, Andrew J. Musser, Akshay Rao, Richard H. Friend
    更新日期:2017-09-12
  • Direct mapping of the angle-dependent barrier to reaction for Cl + CHD3 using polarized scattering data
    Nat. Chem. (IF 25.87) Pub Date : 
    Huilin Pan, Fengyan Wang, Gábor Czakó, Kopin Liu
    更新日期:2017-09-12
  • Atomic resolution of structural changes in elastic crystals of copper(II) acetylacetonate
    Nat. Chem. (IF 25.87) Pub Date : 2017-08-28
    Anna Worthy, Arnaud Grosjean, Michael C. Pfrunder, Yanan Xu, Cheng Yan, Grant Edwards, Jack K. Clegg, John C. McMurtrie
    更新日期:2017-09-07
  • The bottom line
    Nat. Chem. (IF 25.87) Pub Date : 

    The bottom line Nature Chemistry, Published online: 24 August 2017; doi:10.1038/nchem.2860 Our understanding of actinide chemistry lags behind that of the rest of the periodic table. A collection of articles in this issue highlights recent progress featuring uranium(VI) dianions bearing four U–N multiple bonds, berkelium(IV) stabilized in solution and delocalization of 5f electrons in a plutonium material.

    更新日期:2017-09-07
  • Peaceful berkelium
    Nat. Chem. (IF 25.87) Pub Date : 
    Andreas Trabesinger

    Peaceful berkelium Nature Chemistry, Published online: 24 August 2017; doi:10.1038/nchem.2845 The first new element produced after the Second World War has led a rather peaceful life since entering the period table — until it became the target of those producing superheavy elements, as Andreas Trabesinger describes.

    更新日期:2017-09-07
  • Organometallic mechanisms: Measuring up with the early metals
    Nat. Chem. (IF 25.87) Pub Date : 
    Ian A. Tonks

    Organometallic mechanisms: Measuring up with the early metals Nature Chemistry, Published online: 24 August 2017; doi:10.1038/nchem.2851 Mathematically modelling metal–ligand bonding in late transition-metal complexes has been an important tool in catalyst development — although lacking for early transition metals such as Cr and Ti. Now, a simple method for measuring ligand donor properties promises to elevate high-valent early transition metal catalysis to the same level.

    更新日期:2017-09-07
  • Supported liquid metal catalysts: Popping up to the surface
    Nat. Chem. (IF 25.87) Pub Date : 
    Günther Rupprechter

    Supported liquid metal catalysts: Popping up to the surface Nature Chemistry, Published online: 24 August 2017; doi:10.1038/nchem.2849 Merging the advantages of homogeneous and heterogeneous catalysts is a useful strategy for creating improved catalytic systems. Now, a concept has been developed that uses single Pd atoms — supported within liquid alloy droplets — that emerge from the droplet subsurface and interior to react with molecules approaching from the gas phase.

    更新日期:2017-09-07
  • Bonding with actinides
    Nat. Chem. (IF 25.87) Pub Date : 
    Anne Pichon

    Bonding with actinides Nature Chemistry, Published online: 24 August 2017; doi:10.1038/nchem.2855 Suzanne Bart from Purdue University talks to Nature Chemistry about her investigations into the chemistry of actinides, and why she finds them both challenging and rewarding.

    更新日期:2017-09-07
  • Signal transduction in a covalent post-assembly modification cascade
    Nat. Chem. (IF 25.87) Pub Date : 2017-08-21
    Ben S. Pilgrim, Derrick A. Roberts, Thorsten G. Lohr, Tanya K. Ronson, Jonathan R. Nitschke
    更新日期:2017-09-07
  • Dynamic covalent chemistry enables formation of antimicrobial peptide quaternary assemblies in a completely abiotic manner
    Nat. Chem. (IF 25.87) Pub Date : 2017-08-21
    James F. Reuther, Justine L. Dees, Igor V. Kolesnichenko, Erik T. Hernandez, Dmitri V. Ukraintsev, Rusheel Guduru, Marvin Whiteley, Eric V. Anslyn
    更新日期:2017-09-07
  • Atomic resolution of structural changes in elastic crystals of copper(II) acetylacetonate
    Nat. Chem. (IF 25.87) Pub Date : 
    Anna Worthy, Arnaud Grosjean, Michael C. Pfrunder, Yanan Xu, Cheng Yan, Grant Edwards, Jack K. Clegg, John C. McMurtrie

    Single crystals are typically brittle, inelastic materials. Such mechanical responses limit their use in practical applications, particularly in flexible electronics and optical devices. Here we describe single crystals of a well-known coordination compound—copper(II) acetylacetonate—that are flexible enough to be reversibly tied into a knot. Mechanical measurements indicate that the crystals exhibit an elasticity similar to that of soft materials such as nylon, and thus display properties normally associated with both hard and soft matter. Using microfocused synchrotron radiation, we mapped the changes in crystal structure that occur on bending, and determined the mechanism that allows this flexibility with atomic precision. We show that, under strain, the molecules in the crystal reversibly rotate, and thus reorganize to allow the mechanical compression and expansion required for elasticity and still maintain the integrity of the crystal structure.

    更新日期:2017-09-07
  • The bottom line
    Nat. Chem. (IF 25.87) Pub Date : 2017-08-24

    The bottom line Nature Chemistry, Published online: 24 August 2017; doi:10.1038/nchem.2860 Our understanding of actinide chemistry lags behind that of the rest of the periodic table. A collection of articles in this issue highlights recent progress featuring uranium(VI) dianions bearing four U–N multiple bonds, berkelium(IV) stabilized in solution and delocalization of 5f electrons in a plutonium material.

    更新日期:2017-09-07
  • Peaceful berkelium
    Nat. Chem. (IF 25.87) Pub Date : 2017-08-24
    Andreas Trabesinger

    Peaceful berkelium Nature Chemistry, Published online: 24 August 2017; doi:10.1038/nchem.2845 The first new element produced after the Second World War has led a rather peaceful life since entering the period table — until it became the target of those producing superheavy elements, as Andreas Trabesinger describes.

    更新日期:2017-09-07
  • Organometallic mechanisms: Measuring up with the early metals
    Nat. Chem. (IF 25.87) Pub Date : 2017-08-24
    Ian A. Tonks

    Organometallic mechanisms: Measuring up with the early metals Nature Chemistry, Published online: 24 August 2017; doi:10.1038/nchem.2851 Mathematically modelling metal–ligand bonding in late transition-metal complexes has been an important tool in catalyst development — although lacking for early transition metals such as Cr and Ti. Now, a simple method for measuring ligand donor properties promises to elevate high-valent early transition metal catalysis to the same level.

    更新日期:2017-09-07
  • Supported liquid metal catalysts: Popping up to the surface
    Nat. Chem. (IF 25.87) Pub Date : 2017-08-24
    Günther Rupprechter

    Supported liquid metal catalysts: Popping up to the surface Nature Chemistry, Published online: 24 August 2017; doi:10.1038/nchem.2849 Merging the advantages of homogeneous and heterogeneous catalysts is a useful strategy for creating improved catalytic systems. Now, a concept has been developed that uses single Pd atoms — supported within liquid alloy droplets — that emerge from the droplet subsurface and interior to react with molecules approaching from the gas phase.

    更新日期:2017-09-07
  • Bonding with actinides
    Nat. Chem. (IF 25.87) Pub Date : 2017-08-24
    Anne Pichon

    Bonding with actinides Nature Chemistry, Published online: 24 August 2017; doi:10.1038/nchem.2855 Suzanne Bart from Purdue University talks to Nature Chemistry about her investigations into the chemistry of actinides, and why she finds them both challenging and rewarding.

    更新日期:2017-09-07
  • Signal transduction in a covalent post-assembly modification cascade
    Nat. Chem. (IF 25.87) Pub Date : 
    Ben S. Pilgrim, Derrick A. Roberts, Thorsten G. Lohr, Tanya K. Ronson, Jonathan R. Nitschke

    Natural reaction cascades control the movement of biomolecules between cellular compartments. Inspired by these systems, we report a synthetic reaction cascade employing post-assembly modification reactions to direct the partitioning of supramolecular complexes between phases. The system is composed of a self-assembled tetrazine-edged FeII8L12 cube and a maleimide-functionalized FeII4L6 tetrahedron. Norbornadiene (NBD) functions as the stimulus that triggers the cascade, beginning with the inverse-electron-demand Diels–Alder reaction of NBD with the tetrazine moieties of the cube. This reaction generates cyclopentadiene as a transient by-product, acting as a relay signal that subsequently undergoes a Diels–Alder reaction with the maleimide-functionalized tetrahedron. Cyclooctyne can selectively inhibit the cascade by outcompeting NBD as the initial trigger. Initiating the cascade with 2-octadecyl NBD leads to selective alkylation of the tetrahedron upon cascade completion. The increased lipophilicity of the C18-tagged tetrahedron drives this complex into a non-polar phase, allowing its isolation from the initially inseparable mixture of complexes.

    更新日期:2017-09-07
  • Dynamic covalent chemistry enables formation of antimicrobial peptide quaternary assemblies in a completely abiotic manner
    Nat. Chem. (IF 25.87) Pub Date : 
    James F. Reuther, Justine L. Dees, Igor V. Kolesnichenko, Erik T. Hernandez, Dmitri V. Ukraintsev, Rusheel Guduru, Marvin Whiteley, Eric V. Anslyn

    Naturally occurring peptides and proteins often use dynamic disulfide bonds to impart defined tertiary/quaternary structures for the formation of binding pockets with uniform size and function. Although peptide synthesis and modification are well established, controlling quaternary structure formation remains a significant challenge. Here, we report the facile incorporation of aryl aldehyde and acyl hydrazide functionalities into peptide oligomers via solid-phase copper-catalysed azide–alkyne cycloaddition (SP-CuAAC) click reactions. When mixed, these complementary functional groups rapidly react in aqueous media at neutral pH to form peptide–peptide intermolecular macrocycles with highly tunable ring sizes. Moreover, sequence-specific figure-of-eight, dumbbell-shaped, zipper-like and multi-loop quaternary structures were formed selectively. Controlling the proportions of reacting peptides with mismatched numbers of complementary reactive groups results in the formation of higher-molecular-weight sequence-defined ladder polymers. This also amplified antimicrobial effectiveness in select cases. This strategy represents a general approach to the creation of complex abiotic peptide quaternary structures.

    更新日期:2017-09-07
  • Quantifying ligand effects in high-oxidation-state metal catalysis
    Nat. Chem. (IF 25.87) Pub Date : 2017-08-07
    Brennan S. Billow, Tanner J. McDaniel, Aaron L. Odom
    更新日期:2017-08-24
  • Chelation and stabilization of berkelium in oxidation state +IV
    Nat. Chem. (IF 25.87) Pub Date : 2017-04-10
    Gauthier J.-P. Deblonde, Manuel Sturzbecher-Hoehne, Peter B. Rupert, Dahlia D. An, Marie-Claire Illy, Corie Y. Ralston, Jiri Brabec, Wibe A. de Jong, Roland K. Strong, Rebecca J. Abergel
    更新日期:2017-08-24
  • Elucidating bonding preferences in tetrakis(imido)uranate(VI) dianions
    Nat. Chem. (IF 25.87) Pub Date : 2017-04-24
    Nickolas H. Anderson, Jing Xie, Debmalya Ray, Matthias Zeller, Laura Gagliardi, Suzanne C. Bart
    更新日期:2017-08-24
  • Incipient class II mixed valency in a plutonium solid-state compound
    Nat. Chem. (IF 25.87) Pub Date : 2017-05-08
    Samantha K. Cary, Shane S. Galley, Matthew L. Marsh, David L. Hobart, Ryan E. Baumbach, Justin N. Cross, Jared T. Stritzinger, Matthew J. Polinski, Laurent Maron, Thomas E. Albrecht-Schmitt
    更新日期:2017-08-24
  • Gallium-rich Pd–Ga phases as supported liquid metal catalysts
    Nat. Chem. (IF 25.87) Pub Date : 2017-07-24
    N. Taccardi, M. Grabau, J. Debuschewitz, M. Distaso, M. Brandl, R. Hock, F. Maier, C. Papp, J. Erhard, C. Neiss, W. Peukert, A. Görling, H.-P. Steinrück, P. Wasserscheid
    更新日期:2017-08-24
  • Visible-light excitation of iminium ions enables the enantioselective catalytic β-alkylation of enals
    Nat. Chem. (IF 25.87) Pub Date : 2017-03-20
    Mattia Silvi, Charlie Verrier, Yannick P. Rey, Luca Buzzetti, Paolo Melchiorre
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Some contents have been Reproduced with permission of the American Chemical Society.
Some contents have been Reproduced by permission of The Royal Society of Chemistry.
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