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With Tag: Physical And Theoretical Chemistry

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Anion-induced reconstitution of a self-assembling system to express a chloride-binding Co10L15 pentagonal prism

John D. Thoburn, Jonathan R. Nitschke, Boris Breiner, Maarten M. J. Smulders, Jack K. Clegg, Imogen A. Riddell, Yana R. Hristova
Nature Chemistry | 2012 | 10.1038/nchem.1407

Biochemical systems are adaptable, capable of reconstitution at all levels to achieve the functions associated with life. Synthetic chemical systems are more limited in their ability to reorganize to achieve new functions; they can reconfigure to bind an...

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The effect of isotopic substitution on the chirality of a self-assembled helix

Maarten M. J. Smulders, Seda Cantekin, E. W. Meijer, Anja R. A. Palmans, Diederik W. R. Balkenende
Nature Chemistry | 2011 | 10.1038/nchem.889

N,N′,N″-trialkylbenzene-1,3,5-tricarboxamides (BTAs) self-assemble by means of strong, threefold α-helix-type intermolecular hydrogen bonding into well-defined, helical, one-dimensional columnar aggregates. When a stereogenic centre is introduced into the...

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Redox-responsive molecular helices with highly condensed π-clouds

Atsuko Kosaka, Mikio Yamasaki, Takanori Fukushima, Takuzo Aida, Azusa Muraoka, Koichi Yamashita, Eisuke Ohta, Hiroyasu Sato, Hiroshi Ushiyama, Shinji Ando, Kimiko Hasegawa, Daisuke Hashizume
Nature Chemistry | 2011 | 10.1038/nchem.900

Helices have long attracted the attention of chemists, both for their inherent chiral structure and their potential for applications such as the separation of chiral compounds or the construction of molecular machines. As a result of steric forces, polymeric o...

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A ‘clusters-in-liquid’ method for calculating infrared spectra identifies the proton-transfer mode in acidic aqueous solutions

Waldemar Kulig, Noam Agmon
Nature Chemistry | 2013 | 10.1038/nchem.1503

In liquid water the transfer of an excess proton between two water molecules occurs through the Zundel cation, H 2 O···H + ···OH 2 . The proton-transfer mode is the asymmetric stretch of the central O···H + ···O moiety, but there is no consensus on its...

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Precision design of ethylene- and polar-monomer-based copolymers by organometallic-mediated radical polymerization

Anthony Kermagoret, Antoine Debuigne, Christophe Detrembleur, Christine Jérôme
Nature Chemistry | 2014 | 10.1038/nchem.1850

The copolymerization of ethylene with polar monomers is a major challenge when it comes to the manufacture of materials with potential for a wide range of commercial applications. In the chemical industry, free-radical polymerization is used to make a large...

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The direct anti-Markovnikov addition of mineral acids to styrenes

Dale J. Wilger, Taylor R. Lammert, David A. Nicewicz, Jean-Marc M. Grandjean
Nature Chemistry | 2014 | 10.1038/nchem.2000

The direct anti-Markovnikov addition of strong Brønsted acids to alkenes remains an unsolved problem in synthetic chemistry. Here, we report an efficient organic photoredox catalyst system for the addition of ​HCl, ​HF and also phosphoric and sulfonic acids...

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Self-repairing polymers: Materials that heal themselves

Howard M. Colquhoun
Nature Chemistry | 2012 | 10.1038/nchem.1357

Previous approaches to the development of self-repairing polymeric materials have required either the input of external energy or the use of a healing agent. Now, a new type of elastomer, in which hard/soft phase-separation occurs at the nanoscale, displays...

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The energy barrier in singlet fission can be overcome through coherent coupling and entropic gain

X-Y. Zhu, Manuel Ligges, Wai-Lun Chan
Nature Chemistry | 2012 | 10.1038/nchem.1436

One strategy to improve solar-cell efficiency is to generate two excited electrons from just one photon through singlet fission, which is the conversion of a singlet (S 1 ) into two triplet (T 1 ) excitons. For efficient singlet fission it is believed that...

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Quantitative sequencing of 5-formylcytosine in DNA at single-base resolution

Martin Bachman, Shankar Balasubramanian, Giovanni Marsico, Michael J. Booth, Dario Beraldi
Nature Chemistry | 2014 | 10.1038/nchem.1893

Recently, the cytosine modifications 5-hydroxymethylcytosine (5hmC) and 5-formylcytosine (5fC) were found to exist in the genomic deoxyribonucleic acid (DNA) of a wide range of mammalian cell types. It is now important to understand their role in normal...

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Binary fluorous tagging enables the synthesis and separation of a 16-stereoisomer library of macrosphelides

Jesse J. Sabatini, Dennis P. Curran, Kai Zhang, Mantosh K. Sinha, Dae-Hyun Cho
Nature Chemistry | 2012 | 10.1038/nchem.1233

Fluorous mixture synthesis minimizes the effort to synthesize small-molecule libraries by labelling the molecules rather than the reaction vessels. Reactants are labelled with fluorinated tags and products can later be demixed based on the fluorine content. A...

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Atmospheric photochemistry: Roaming in the dark

Simon W. North
Nature Chemistry | 2011 | 10.1038/nchem.1079

The mechanism of NO and O 2 production through the photolysis of the nitrate radical has long proved elusive. Now, theoretical studies help to explain previous experiments, suggesting that two distinct pathways are responsible that both involve 'roaming...

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Conditionally fluorescent molecular probes for detecting single base changes in double-stranded DNA

David Yu Zhang, Georg Seelig, Sherry Xi Chen
Nature Chemistry | 2013 | 10.1038/nchem.1713

Small variations in nucleic acid sequences can have far-reaching phenotypic consequences. Reliably distinguishing closely related sequences is therefore important for research and clinical applications. Here, we demonstrate that conditionally fluorescent DNA...

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An iron complex with pendent amines as a molecular electrocatalyst for oxidation of hydrogen

Tianbiao Liu, R. Morris Bullock, Daniel L. DuBois
Nature Chemistry | 2013 | 10.1038/nchem.1571

The increasing energy needs of society have led to a search for technologies that can tap carbon-neutral and sustainable energy sources, such as solar and wind. Using properly designed catalysts, such sources can also be used to create fuels such as hydrogen;...

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Electrically induced bonding of DNA to gold

Matthias Erdmann, Ralf David, Ann R. Fornof, Hermann E. Gaub
Nature Chemistry | 2010 | 10.1038/nchem.722

The development of single-molecule techniques has afforded many new methods for the observation and assembly of supramolecular structures and biomolecular networks. We previously reported a method, known as the single-molecule cut-and-paste approach, to pick...

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Macroscopic self-assembly through molecular recognition

Ryosuke Kobayashi, Hiroyasu Yamaguchi, Yoshinori Takashima, Akira Harada, Akihito Hashidzume
Nature Chemistry | 2011 | 10.1038/nchem.893

Molecular recognition plays an important role in nature, with perhaps the best known example being the complementarity exhibited by pairs of nucleobases in DNA. Studies of self-assembling and self-organizing systems based on molecular recognition are often...

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Chemical bonding: Rethinking carbon

C. Adam Dyker, Guy Bertrand
Nature Chemistry | 2009 | 10.1038/nchem.265

The covalent bonding behaviour of carbon is the mainstay of organic chemistry, but in some compounds carbon seems to behave more like a metal.

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A microdroplet dilutor for high-throughput screening

Joshua B. Edel, Fabrice Gielen, Andrew J. DeMello, Xize Niu
Nature Chemistry | 2011 | 10.1038/nchem.1046

Pipetting and dilution are universal processes used in chemical and biological laboratories to assay and experiment. In microfluidics such operations are equally in demand, but difficult to implement. Recently, droplet-based microfluidics has emerged as an...

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Dinitrogen cleavage: Breaking bonds

Gavin Armstrong
Nature Chemistry | 2008 | 10.1038/nchem.68

The catalytic synthesis of ammonia has huge biological and industrial significance. The method, whether it is nitrogen fixation through enzymes or the Haber–Bosch process, must cleave the immensely strong N|[equiv]|N bond and usually relies on cooperation...

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The oxidative inactivation of FeFe hydrogenase reveals the flexibility of the H-cluster

Maurizio Bruschi, Pierre Ezanno, Philippe Soucaille, Vincent Fourmond, Marco Montefiori, Isabelle Meynial-Salles, Po-Hung Wang, Hervé Bottin, Luca De Gioia, Christophe Léger, Carole Baffert, Kateryna Sybirna, Claudio Greco, Jochen Blumberger
Nature Chemistry | 2014 | 10.1038/nchem.1892

Nature is a valuable source of inspiration in the design of catalysts, and various approaches are used to elucidate the mechanism of hydrogenases, the enzymes that oxidize or produce H 2 . In FeFe hydrogenases, H 2 oxidation occurs at the H-cluster, and...

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Reconstitution of a fungal meroterpenoid biosynthesis reveals the involvement of a novel family of terpene cyclases

Yutaka Ebizuka, Tetsuo Kushiro, Kinya Tokunaga, Isao Fujii, Takayuki Itoh, Yudai Matsuda, Ikuro Abe
Nature Chemistry | 2010 | 10.1038/nchem.764

Meroterpenoids are hybrid natural products of both terpenoid and polyketide origin. We identified a biosynthetic gene cluster that is responsible for the production of the meroterpenoid pyripyropene in the fungus Aspergillus fumigatus through reconstituted...

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