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Nature Chemistry

Jonathan Rittle, Mackenzie J Field, Michael T Green, F Akif Tezcan
The bottom-up design and construction of functional metalloproteins remains a formidable task in biomolecular design. Although numerous strategies have been used to create new metalloproteins, pre-existing knowledge of the tertiary and quaternary protein structure is often required to generate suitable platforms for robust metal coordination and activity. Here we report an alternative and easily implemented approach (metal active sites by covalent tethering or MASCoT) in which folded protein building blocks are linked by a single disulfide bond to create diverse metal coordination environments within evolutionarily naive protein-protein interfaces...
February 18, 2019: Nature Chemistry
Alessandro Ianiro, Hanglong Wu, Mark M J van Rijt, M Paula Vena, Arthur D A Keizer, A Catarina C Esteves, Remco Tuinier, Heiner Friedrich, Nico A J M Sommerdijk, Joseph P Patterson
The self-assembly of amphiphilic molecules in solution is a ubiquitous process in both natural and synthetic systems. The ability to effectively control the structure and properties of these systems is essential for tuning the quality of their functionality, yet the underlying mechanisms governing the transition from molecules to assemblies have not been fully resolved. Here we describe how amphiphilic self-assembly can be preceded by liquid-liquid phase separation. The assembly of a model block co-polymer system into vesicular structures was probed through a combination of liquid-phase electron microscopy, self-consistent field computations and Gibbs free energy calculations...
February 18, 2019: Nature Chemistry
Luis Bañares
In the version of this News & Views originally published, Fig. 1b incorrectly displayed the chemical formula "CH3 NHCH3 ". This has been corrected to "CH3 NHCH2 ".
February 7, 2019: Nature Chemistry
Wenmao Huang, Xin Wu, Xiang Gao, Yifei Yu, Hai Lei, Zhenshu Zhu, Yi Shi, Yulan Chen, Meng Qin, Wei Wang, Yi Cao
Maleimide-thiol reactions are widely used to produce protein-polymer conjugates for therapeutics. However, maleimide-thiol adducts are unstable in vivo or in the presence of thiol-containing compounds because of the elimination of the thiosuccinimide linkage through a retro-Michael reaction or thiol exchange. Here, using single-molecule force spectroscopy, we show that applying an appropriate stretching force to the thiosuccinimide linkage can considerably stabilize the maleimide-thiol adducts, in effect using conventional mechanochemistry of force-accelerated bond dissociation to unconventionally stabilize an adjacent bond...
February 4, 2019: Nature Chemistry
Genfeng Feng, Mingxing Zhang, Dong Shao, Xinyi Wang, Shuao Wang, Laurent Maron, Congqing Zhu
Heterometallic clusters are important in catalysis and small-molecule activation because of the multimetallic synergistic effects from different metals. However, multimetallic species that contain uranium-metal bonds remain very scarce due to the difficulties in their synthesis. Here we present a straightforward strategy to construct a series of heterometallic clusters with multiple uranium-metal bonds. These complexes were created by facile reactions of a uranium precursor with Ni(COD)2 (COD, cyclooctadiene)...
January 28, 2019: Nature Chemistry
Zhenjie Ni, Hanlin Wang, Huanli Dong, Yanfeng Dang, Qiang Zhao, Xiaotao Zhang, Wenping Hu
Conjugated polymers are attractive components for plastic electronics, but their structural defects, low solubility and batch-to-batch variation-mainly in terms of molecular weight and dispersity-hinder practical applications. Here, we demonstrate that these issues can be circumvented by using conjugated mesopolymers, which have the advantages of both oligomers and polymers. A diketopyrrolopyrrole monomer and a benzothiadiazole derivative react through direct arylation polycondensation, promoted by sterically hindered adamantyl ligand coordinated palladium catalysts, to form mesopolymers...
January 28, 2019: Nature Chemistry
Zackaria Nairoukh, Marco Wollenburg, Christoph Schlepphorst, Klaus Bergander, Frank Glorius
Piperidines and fluorine substituents are both independently indispensable components in pharmaceuticals, agrochemicals and materials. Logically, the incorporation of fluorine atoms into piperidine scaffolds is therefore an area of tremendous potential. However, synthetic approaches towards the formation of these architectures are often impractical. The diastereoselective synthesis of substituted monofluorinated piperidines often requires substrates with pre-defined stereochemistry. That of multifluorinated piperidines is even more challenging, and often needs to be carried out in multistep syntheses...
January 21, 2019: Nature Chemistry
Jiqing Jiao, Rui Lin, Shoujie Liu, Weng-Chon Cheong, Chao Zhang, Zheng Chen, Yuan Pan, Jianguo Tang, Konglin Wu, Sung-Fu Hung, Hao Ming Chen, Lirong Zheng, Qi Lu, Xuan Yang, Bingjun Xu, Hai Xiao, Jun Li, Dingsheng Wang, Qing Peng, Chen Chen, Yadong Li
The electrochemical reduction of CO2 could play an important role in addressing climate-change issues and global energy demands as part of a carbon-neutral energy cycle. Single-atom catalysts can display outstanding electrocatalytic performance; however, given their single-site nature they are usually only amenable to reactions that involve single molecules. For processes that involve multiple molecules, improved catalytic properties could be achieved through the development of atomically dispersed catalysts with higher complexities...
January 21, 2019: Nature Chemistry
Lifei Zheng, Hui Zhao, Yanxiao Han, Haibin Qian, Lela Vukovic, Jasmin Mecinović, Petr Král, Wilhelm T S Huck
Transport at the molecular scale is a prerequisite for the development of future molecular factories. Here, we have designed oligoanionic molecular sliders on polycationic tracks that exploit Brownian motion and diffusive binding to transport cargo without using a chemical fuel. The presence of the polymer tracks increases the rate of bimolecular reactions between modified sliders by over two orders of magnitude. Molecular dynamics simulations showed that the sliders not only diffuse, but also jump and hop surprisingly efficiently along polymer tracks...
January 21, 2019: Nature Chemistry
Dingchang Lin, Yayuan Liu, Yanbin Li, Yuzhang Li, Allen Pei, Jin Xie, William Huang, Yi Cui
Developing a viable metallic lithium anode is a prerequisite for next-generation batteries. However, the low redox potential of lithium metal renders it prone to corrosion, which must be thoroughly understood for it to be used in practical energy-storage devices. Here we report a previously overlooked mechanism by which lithium deposits can corrode on a copper surface. Voids are observed in the corroded deposits and a Kirkendall-type mechanism is validated through electrochemical analysis. Although it is a long-held view that lithium corrosion in electrolytes involves direct charge-transfer through the lithium-electrolyte interphase, the corrosion observed here is found to be governed by a galvanic process between lithium and the copper substrate-a pathway largely neglected by previous battery corrosion studies...
January 21, 2019: Nature Chemistry
Jamie Hicks, Akseli Mansikkamäki, Petra Vasko, Jose M Goicoechea, Simon Aldridge
Solid-state auride salts featuring the negatively charged Au- ion are known to be stable in the presence of alkali metal counterions. While such electron-rich species might be expected to be nucleophilic (in the same manner as I- , for example), their instability in solution means that this has not been verified experimentally. Here we report a two-coordinate gold complex (NON)AlAuPt Bu3 (where NON is the chelating tridentate ligand 4,5-bis(2,6-diisopropylanilido)-2,7-di-tert-butyl-9,9-dimethylxanthene) that features a strongly polarized bond, Auδ- -Alδ+ ...
January 21, 2019: Nature Chemistry
Anna J Simon, Yi Zhou, Vyas Ramasubramani, Jens Glaser, Arti Pothukuchy, Jimmy Gollihar, Jillian C Gerberich, Janelle C Leggere, Barrett R Morrow, Cheulhee Jung, Sharon C Glotzer, David W Taylor, Andrew D Ellington
Symmetrical protein oligomers are ubiquitous in biological systems and perform key structural and regulatory functions. However, there are few methods for constructing such oligomers. Here we have engineered completely synthetic, symmetrical oligomers by combining pairs of oppositely supercharged variants of a normally monomeric model protein through a strategy we term 'supercharged protein assembly' (SuPrA). We show that supercharged variants of green fluorescent protein can assemble into a variety of architectures including a well-defined symmetrical 16-mer structure that we solved using cryo-electron microscopy at 3...
January 14, 2019: Nature Chemistry
Brett F Thornton, Shawn C Burdette
In the version of this Comment originally published, the image was incorrectly credited to Chelsea Anne Bar; it should have been to Brett F. Thornton. This has now been corrected.
January 10, 2019: Nature Chemistry
Michelle Francl
In the version of this Comment originally published, the name of the author of ref. 10 was incorrectly given as "Chapman, J."; this has now been corrected to "Chapman, K.".
January 8, 2019: Nature Chemistry
Ruijiao Dong, Ruiyi Liu, Piers R J Gaffney, Marc Schaepertoens, Patrizia Marchetti, Christopher M Williams, Rongjun Chen, Andrew G Livingston
In the version of this Article originally published, the authors inadvertently cited ref. 10 in two places in the first paragraph. They would like to clarify that it should not have been cited in the sentence that starts "Polymer chemists have employed strategies such as single monomer insertion..." as it mistakenly implied that the IEG+ method described in ref. 10 could not produce unimolecular polymers; it can do so, as was demonstrated in ref. 10. The authors would also like to clarify that ref...
January 8, 2019: Nature Chemistry
Jinpeng Zhao, Takeshi Nanjo, Emilio C de Lucca, M Christina White
Despite significant progress in the development of site-selective aliphatic C-H oxidations over the past decade, the ability to oxidize strong methylene C-H bonds in the presence of more oxidatively labile aromatic functionalities remains a major unsolved problem. Such chemoselective reactivity is highly desirable for enabling late-stage oxidative derivatizations of pharmaceuticals and medicinally important natural products that often contain such functionality. Here, we report a simple manganese small-molecule catalyst Mn(CF3 -PDP) system that achieves such chemoselectivity via an unexpected synergy of catalyst design and acid additive...
December 17, 2018: Nature Chemistry
Alexandru Grozavu, Hamish B Hepburn, Philip J Smith, Harish K Potukuchi, Peter J Lindsay-Scott, Timothy J Donohoe
Aromatic rings are ubiquitous in organic chemistry and form the basis of many commercial products. Despite the numerous routes available for the preparation of aromatic compounds, there remain few methods that allow their conversion into synthetically useful partially saturated derivatives and even fewer that allow new C-C bonds to be formed at the same time. Here we set out to address this problem and uncover a unique catalytic partial reduction reaction that forms partially saturated azaheterocycles from aromatic precursors...
December 17, 2018: Nature Chemistry
Hongwei Li, Alexander Kamasah, Spiridoula Matsika, Arthur G Suits
Intersystem crossing plays an important role in photochemistry. It is understood to be efficient when heavy atoms are present due to strong spin-orbit coupling, or when strongly bound long-lived complexes are formed that increase the chance of finding the singlet-triplet intersection seam. Here we present evidence for a different intersystem crossing mechanism in the bimolecular reaction of O(3 P) with alkylamines. In crossed-beam experiments, product velocity-flux maps are measured for aminoalkyl radicals produced from H abstraction from the methyl group, which also gives OH radicals as co-fragments...
December 10, 2018: Nature Chemistry
Zufeng Guo, Sam Y Hong, Jingxin Wang, Shahid Rehan, Wukun Liu, Hanjing Peng, Manisha Das, Wei Li, Shridhar Bhat, Brandon Peiffer, Brett R Ullman, Chung-Ming Tse, Zlatina Tarmakova, Cordelia Schiene-Fischer, Gunter Fischer, Imogen Coe, Ville O Paavilainen, Zhaoli Sun, Jun O Liu
Rapamycin and FK506 are macrocyclic natural products with an extraordinary mode of action, in which they form binary complexes with FK506-binding protein (FKBP) through a shared FKBP-binding domain before forming ternary complexes with their respective targets, mechanistic target of rapamycin (mTOR) and calcineurin, respectively. Inspired by this, we sought to build a rapamycin-like macromolecule library to target new cellular proteins by replacing the effector domain of rapamycin with a combinatorial library of oligopeptides...
December 10, 2018: Nature Chemistry
Lin Liu, Anthony R Prudden, Chantelle J Capicciotti, Gerlof P Bosman, Jeong-Yeh Yang, Digantkumar G Chapla, Kelley W Moremen, Geert-Jan Boons
Contemporary chemoenzymatic approaches can provide highly complex multi-antennary N-linked glycans. These procedures are, however, very demanding and typically involve as many as 100 chemical steps to prepare advanced intermediates that can be diversified by glycosyltransferases in a branch-selective manner to give asymmetrical structures commonly found in nature. Only highly specialized laboratories can perform such syntheses, which greatly hampers progress in glycoscience. Here we describe a biomimetic approach in which a readily available bi-antennary glycopeptide can be converted in ten or fewer chemical and enzymatic steps into multi-antennary N-glycans that at each arm can be uniquely extended by glycosyltransferases to give access to highly complex asymmetrically branched N-glycans...
December 10, 2018: Nature Chemistry
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