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Nature Chemistry

Qin Cao, Woo Shik Shin, Henry Chan, Celine K Vuong, Bethany Dubois, Binsen Li, Kevin A Murray, Michael R Sawaya, Juli Feigon, Douglas L Black, David S Eisenberg, Lin Jiang
In the version of this Article originally published online, the upper right panel of Fig. 5a was mistakenly a repeat of the lower right panel. This has now been corrected in all versions of the Article.
November 12, 2018: Nature Chemistry
Michelle J MacLeod, Aaron J Goodman, Hong-Zhou Ye, Hung V-T Nguyen, Troy Van Voorhis, Jeremiah A Johnson
Although N-heterocyclic carbenes (NHCs) have demonstrated outstanding potential for use as surface anchors, synthetic challenges have limited their application to either large planar substrates or very small spherical nanoparticles. The development of a strategy to graft NHCs onto non-spherical nanomaterials, such as gold nanorods, would greatly expand their utility as surface ligands. Here, we use a bidentate thiolate-NHC-gold(I) complex that is easily grafted onto commercial cetyl trimethylammonium bromide-stabilized gold nanorods through ligand exchange...
November 12, 2018: Nature Chemistry
Robert A Tromans, Tom S Carter, Laurent Chabanne, Matthew P Crump, Hongyu Li, Johnathan V Matlock, Michael G Orchard, Anthony P Davis
Specific molecular recognition is routine for biology, but has proved difficult to achieve in synthetic systems. Carbohydrate substrates are especially challenging, because of their diversity and similarity to water, the biological solvent. Here we report a synthetic receptor for glucose, which is biomimetic in both design and capabilities. The core structure is simple and symmetrical, yet provides a cavity which almost perfectly complements the all-equatorial β-pyranoside substrate. The receptor's affinity for glucose, at Ka ~ 18,000 M-1 , compares well with natural receptor systems...
November 12, 2018: Nature Chemistry
Jin-Ling Ma, Fan-Lu Meng, Yue Yu, Da-Peng Liu, Jun-Min Yan, Yu Zhang, Xin-Bo Zhang, Qing Jiang
Rechargeable aprotic alkali metal (Li or Na)-O2 batteries are the subject of great interest because of their high theoretical specific energy. However, the growth of dendrites and cracks at the Li or Na anode, as well as their corrosive oxidation lead to poor cycling stability and safety issues. Understanding the mechanism and improving Li/Na-ion plating and stripping electrochemistry are therefore essential to realizing their technological potential. Here, we report how the use of a Li-Na alloy anode and an electrolyte additive realizes an aprotic bimetal Li-Na alloy-O2 battery with improved cycling stability...
November 12, 2018: Nature Chemistry
Marta Falcone, Luciano Barluzzi, Julie Andrez, Farzaneh Fadaei Tirani, Ivica Zivkovic, Alberto Fabrizio, Clemence Corminboeuf, Kay Severin, Marinella Mazzanti
Cooperativity between metal centres is identified as a crucial step in dinitrogen reduction both for the industrial Haber-Bosch process and for the natural fixation of nitrogen by nitrogenase enzymes, but the mechanism of N2 reduction remains poorly understood. This is in large part because multimetallic complexes that reduce and functionalize dinitrogen in the absence of strong alkali reducing agents are crucial to establish a structure-activity relationship, but remain extremely rare. Recently, we reported a multimetallic nitride-bridged diuranium(III) complex capable of reducing and functionalizing dinitrogen...
November 12, 2018: Nature Chemistry
Jianzhong Liu, Xu Qiu, Xiaoqiang Huang, Xiao Luo, Cheng Zhang, Jialiang Wei, Jun Pan, Yujie Liang, Yuchao Zhu, Qixue Qin, Song Son, Ning Jiao
The version of this Article originally published online did not include a caution statement relating to safety concerns over some of the reagents used. All versions of the Article now have the following text included at the start of the Methods section "Caution: Sodium azide (NaN3 ) is highly toxic and also a potential explosion hazard; it can also react with organohalides to form explosive organic azides. Under acidic conditions, sodium azide can form hydrazoic acid (HN3 ) which is highly toxic. Considering these hazards, appropriate safety precautions should be taken when undertaking the C-C amination reactions reported in this Article...
November 8, 2018: Nature Chemistry
Jun Zhu, Jianchun Wang, Guangbin Dong
Transition metal catalysis has emerged as an important means for C-C activation that allows mild and selective transformations. However, the current scope of C-C bonds that can be activated is primarily restricted to either highly strained systems or more polarized C-C bonds. In contrast, the catalytic activation of non-polar and unstrained C-C moieties remains an unmet challenge. Here we report a general approach for the catalytic activation of the unstrained C(aryl)-C(aryl) bonds in 2,2'-biphenols. The key is to utilize the phenol moiety as a handle to install phosphinites as a recyclable directing group...
November 5, 2018: Nature Chemistry
Daniel T Cohen, Chi Zhang, Colin M Fadzen, Alexander J Mijalis, Liana Hie, Kenneth D Johnson, Zachary Shriver, Obadiah Plante, Scott J Miller, Stephen L Buchwald, Bradley L Pentelute
Conjugates between proteins and small molecules enable access to a vast chemical space that is not achievable with either type of molecule alone; however, the paucity of specific reactions capable of functionalizing proteins and natural products presents a formidable challenge for preparing conjugates. Here we report a strategy for conjugating electron-rich (hetero)arenes to polypeptides and proteins. Our bioconjugation technique exploits the electrophilic reactivity of an oxidized selenocysteine residue in polypeptides and proteins, and the electron-rich character of certain small molecules to provide bioconjugates in excellent yields under mild conditions...
November 5, 2018: Nature Chemistry
Gareth T Whiting, Nikolaos Nikolopoulos, Ioannis Nikolopoulos, Abhishek Dutta Chowdhury, Bert M Weckhuysen
The performances of porous materials are closely related to the accessibility and interconnectivity of their porous domains. Visualizing pore architecture and its role on functionality-for example, mass transport-has been a challenge so far, and traditional bulk and often non-visual pore measurements have to suffice in most cases. Here, we present an integrated, facile fluorescence microscopy approach to visualize the pore accessibility and interconnectivity of industrial-grade catalyst bodies, and link it unequivocally with their catalytic performance...
November 5, 2018: Nature Chemistry
Wei Wang
No abstract text is available yet for this article.
November 5, 2018: Nature Chemistry
Xiaohong Liu, Fuying Kang, Cheng Hu, Li Wang, Zhen Xu, Dandan Zheng, Weimin Gong, Yi Lu, Yanhe Ma, Jiangyun Wang
Photosensitizers, which harness light energy to upgrade weak reductants to strong reductants, are pivotal components of the natural and artificial photosynthesis machineries. However, it has proved difficult to enhance and expand their functions through genetic engineering. Here we report a genetically encoded, 27 kDa photosensitizer protein (PSP), which facilitates the rational design of miniature photocatalytic CO2 -reducing enzymes. Visible light drives PSP efficiently into a long-lived triplet excited state (PSP*), which reacts rapidly with reduced nicotinamide adenine dinucleotide to generate a super-reducing radical (PSP• ), which is strong enough to reduce many CO2 -reducing catalysts...
November 5, 2018: Nature Chemistry
Stefan Knecht, Hans Jørgen Aa Jensen, Trond Saue
Understanding the bonding, reactivity and electronic structure of actinides is lagging behind that of the rest of the periodic table. This can be partly explained by the challenges that one faces in experimental studies of such radioactive compounds and also by the need to properly account for relativistic effects in theoretical studies. A further challenge is the very complicated electronic structures encountered in actinide chemistry, as vividly illustrated by the naked diuranium molecule U2 . Here we report a computational study of this emblematic molecule using state-of-the-art relativistic quantum chemical methods...
October 29, 2018: Nature Chemistry
Jianzhong Liu, Xu Qiu, Xiaoqiang Huang, Xiao Luo, Cheng Zhang, Jialiang Wei, Jun Pan, Yujie Liang, Yuchao Zhu, Qixue Qin, Song Song, Ning Jiao
Anilines are fundamental motifs in various chemical contexts, and are widely used in the industrial production of fine chemicals, polymers, agrochemicals and pharmaceuticals. A recent development for the synthesis of anilines uses the primary amination of C-H bonds in electron-rich arenes. However, there are limitations to this strategy: the amination of electron-deficient arenes remains a challenging task and the amination of electron-rich arenes has a limited control over regioselectivity-the formation of meta-aminated products is especially difficult...
October 29, 2018: Nature Chemistry
Eun-Ang Raiber, Guillem Portella, Sergio Martínez Cuesta, Robyn Hardisty, Pierre Murat, Zhe Li, Mario Iurlaro, Wendy Dean, Julia Spindel, Dario Beraldi, Zheng Liu, Mark A Dawson, Wolf Reik, Shankar Balasubramanian
Nucleosomes are the basic unit of chromatin that help the packaging of genetic material while controlling access to the genetic information. The underlying DNA sequence, together with transcription-associated proteins and chromatin remodelling complexes, are important factors that influence the organization of nucleosomes. Here, we show that the naturally occurring DNA modification, 5-formylcytosine (5fC) is linked to tissue-specific nucleosome organization. Our study reveals that 5fC is associated with increased nucleosome occupancy in vitro and in vivo...
October 22, 2018: Nature Chemistry
Ryo Nakano, Rodolphe Jazzar, Guy Bertrand
By flanking a carbene carbon with two substituents, it is possible to synthesize persistent triplet carbenes and isolable singlet carbenes. Isolable singlet carbenes are among the most powerful tools in chemistry, and they have even found medicinal and materials science applications. Between the rich chemistry of disubstituted carbenes and the transient parent carbene are the monosubstituted carbenes that, so far, have only been observed in matrices at very low temperatures of just a few K. Herein, we describe the synthesis of a crystalline monosubstituted carbene...
October 15, 2018: Nature Chemistry
Sean D S Gordon, Juan J Omiste, Junwen Zou, Silvia Tanteri, Paul Brumer, Andreas Osterwalder
A prerequisite to gain a complete understanding of the most basic aspects of chemical reactions is the ability to perform experiments with complete control over the reactant degrees of freedom. By controlling these, details of a reaction mechanism can be investigated and ultimately manipulated. Here, we present a study of chemi-ionization-a fundamental energy-transfer reaction-under completely controlled conditions. The collision energy of the reagents was tuned from 0.02 K to 1,000 K, with the orientation of the excited Ne atom relative to Ar fully specified by an external magnetic field...
October 8, 2018: Nature Chemistry
Suhang He, Frank Biedermann, Nina Vankova, Lyuben Zhechkov, Thomas Heine, Roy E Hoffman, Alfonso De Simone, Timothy T Duignan, Werner M Nau
The accurate dissection of binding energies into their microscopic components is challenging, especially in solution. Here we study the binding of noble gases (He-Xe) with the macrocyclic receptor cucurbit[5]uril in water by displacement of methane and ethane as 1 H NMR probes. We dissect the hydration free energies of the noble gases into an attractive dispersive component and a repulsive one for formation of a cavity in water. This allows us to identify the contributions to host-guest binding and to conclude that the binding process is driven by differential cavitation energies rather than dispersion interactions...
October 8, 2018: Nature Chemistry
Annabelle Hoegl, Matthew B Nodwell, Volker C Kirsch, Nina C Bach, Martin Pfanzelt, Matthias Stahl, Sabine Schneider, Stephan A Sieber
Pyridoxal phosphate (PLP) is an enzyme cofactor required for the chemical transformation of biological amines in many central cellular processes. PLP-dependent enzymes (PLP-DEs) are ubiquitous and evolutionarily diverse, making their classification based on sequence homology challenging. Here we present a chemical proteomic method for reporting on PLP-DEs using functionalized cofactor probes. We synthesized pyridoxal analogues modified at the 2'-position, which are taken up by cells and metabolized in situ...
October 8, 2018: Nature Chemistry
Xiang Sun, Junting Chen, Tobias Ritter
Alkenes are among the most versatile building blocks and are widely used for the production of polymers, detergents and synthetic lubricants. Currently, alkenes are sourced from petroleum feedstocks such as naphtha. In light of the necessity to invent sustainable production methods, multiple approaches to making alkenes from abundant fatty acids have been evaluated. However, all attempts so far have required at least one stoichiometric additive, which is an obstruction for applications at larger scales. Here, we report an approach to making olefins from carboxylic acids, in which every additional reaction constituent can be used as a catalyst...
October 8, 2018: Nature Chemistry
Qin Cao, Woo Shik Shin, Henry Chan, Celine K Vuong, Bethany Dubois, Binsen Li, Kevin A Murray, Michael R Sawaya, Juli Feigon, Douglas L Black, David S Eisenberg, Lin Jiang
Inhibiting the interaction between amyloid-β (Aβ) and a neuronal cell surface receptor, LilrB2, has been suggested as a potential route for treating Alzheimer's disease. Supporting this approach, Alzheimer's-like symptoms are reduced in mouse models following genetic depletion of the LilrB2 homologue. In its pathogenic, oligomeric state, Aβ binds to LilrB2, triggering a pathway to synaptic loss. Here we identify the LilrB2 binding moieties of Aβ (16 KLVFFA21 ) and identify its binding site on LilrB2 from a crystal structure of LilrB2 immunoglobulin domains D1D2 complexed to small molecules that mimic phenylalanine residues...
October 8, 2018: Nature Chemistry
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