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Chemical Communications: Chem Comm

Sijie Liu, Zhihua Sun, Chengmin Ji, Lina Li, Sangen Zhao, Junhua Luo
We report a new solid-state nonlinear optical switch based on a one-dimensional channel compound NH4[(CH3)4N]SO4·H2O. It shows an exceptional bi-step switching of second harmonic generation (SHG) effects, corresponding to its SHG-Off, SHG-Low and SHG-High states, which originate from two-step structural transitions with unique centrosymmetric-polar-chiral symmetry transformations.
June 23, 2017: Chemical Communications: Chem Comm
Gesi Wen, Daoyuan Chen, Wenjing Qin, Binhua Zhou, Youqiao Wang, Ziyi Liu, Jun Du, Qiang Zhou, Junmin Quan, Xianzhang Bu
Elimination of amyloid-β (Aβ) oligomers remains challenging. We describe here a novel strategy to prevent and eliminate the Aβ oligomers from either the early aggregation or the fibril dissolution pathway by targeting the flexible N-terminus, but not the widely investigated hydrophobic segment, with a rationally designed cyclopeptide.
June 23, 2017: Chemical Communications: Chem Comm
Shao-Xia Lin, Gui-Jun Sun, Qiang Kang
We report an efficient enantioselective conjugate addition of photogenerated α-amino radicals to Michael acceptors catalyzed by a newly prepared chiral-at-metal rhodium complex. This protocol shows that a single Rh(iii) complex can serve not only as a Lewis acid but also as a photoredox catalyst to control the stereoselectivity during the bond formation.
June 23, 2017: Chemical Communications: Chem Comm
Georges Mouchaham, Brian Abeykoon, Mónica Giménez-Marqués, Sergio Navalon, Andrea Santiago-Portillo, Maame Affram, Nathalie Guillou, Charlotte Martineau, Hermenegildo Garcia, Alexandra Fateeva, Thomas Devic
The use of a 5,10,15,20-tetrakis(3,4,5-trihydroxyphenyl)porphyrin has yielded a new MOF based on M-1,2,3-trioxobenzene chains that can be made of M = Zr(iv) or RE(iii) (RE = rare earth), showing a very high and limited chemical stability, respectively. The robust metallated Zr-analogue, Co-MIL-173(Zr), has proven to be a heme-like heterogeneous catalyst suitable for aerobic oxidation of hydrocarbons.
June 23, 2017: Chemical Communications: Chem Comm
Adam D Piascik, Peter J Hill, Andrew D Crawford, Laurence R Doyle, Jennifer C Green, Andrew E Ashley
The first cationic Fe silyldiazenido complexes, [Fe(PP)2(NN-SiMe3)](+)[BAr(F)4](-) (PP = dmpe/depe), have been synthesised and thoroughly characterised. Computational studies show the compounds to be useful structural and electronic surrogates for the more elusive [Fe(PP)2(NN-H)](+), which are postulated intermediates in the H(+)/e(-) mediated fixation of N2 by Fe(PP)2(N2) species.
June 23, 2017: Chemical Communications: Chem Comm
Xiang Zhu, Shunmin Ding, Carter W Abney, Katie L Browning, Robert L Sacci, Gabriel M Veith, Chengcheng Tian, Sheng Dai
A superacid-promoted "knitting" strategy has been developed for the generation of a novel family of hypercrosslinked nanoporous polycarbazoles for efficient CO2 capture. Using trifluoromethanesulfonic acid, a Brønsted superacid, we demonstrate the facile and rapid synthesis of highly porous polycarbazoles with BET surface areas as high as 1688 m(2) g(-1), and capable of adsorbing 3.5 mmol g(-1) of CO2 at 298 K and 1 bar. This impressive result bestows the material with the highest CO2 uptake capacity for all nanoporous carbazolic polymers and ranks among the best by known porous organic polymers under this condition...
June 23, 2017: Chemical Communications: Chem Comm
Jiwoong Kwon, Doyk Hwang, Jong Woo Lee, Inhae Zoh, Jooyoun Kang, Seong Keun Kim
We report a serendipitous discovery of light-induced generation of a circular microstructure on a glass surface. The microstructure has a ring shape with notable photophysical properties such as highly bright luminescence and strong resistance to photobleaching. We investigated the formation process as well as the luminescence properties of the micro ring to understand the origin of this peculiar phenomenon.
June 23, 2017: Chemical Communications: Chem Comm
Huanfeng Jiang, Wei Huang, Yue Yu, Songjian Yi, Jiawei Li, Wanqing Wu
We have developed a transition-metal free trifluoromethylation protocol between enamines and CF3SO2Na. A wide range of β-trifluoromethyl substituted enamines were delivered in moderate to high yields with only E-configurations.
June 23, 2017: Chemical Communications: Chem Comm
Daily Rodriguez-Padrón, Alain R Puente-Santiago, Alina M Balu, Antonio A Romero, Rafael Luque
A solventless mechanochemical approach was employed to obtain a bioconjugate (BSA-DA-Fe2O3) based on bovine serum albumin (BSA) and dopamine (DA) coated iron oxide magnetic nanoparticles. UV-vis measurements of the obtained material showed a distinctive peak at 280 nm which, together with the presence of N on the surface of the nanomaterial (a band at 400 eV in the XPS spectrum) and zeta potential measurements, confirmed the successful immobilization of the protein. Additionally, the presence of two bands at 1652 and 1545 cm(-1) in the FT-IR spectra of both BSA and BSA-DA-Fe2O3 and steady-state fluorescence analysis validated that the protein preserved its native-like structure after the mechanochemical milling process...
June 23, 2017: Chemical Communications: Chem Comm
Feng Xu, Qin Lu, Lin Ye, S C Edman Tsang
Using physical mixtures of Pd/SWNTs (Pd nanoparticles on single-walled carbon nanotubes) and Pt/SWNTs, the composites show electro-catalytic properties comparable to the corresponding alloys: electron exchange readily occurs between the two metal nanoparticles via SWNT support at long ranges without direct atomic contact, which is responsible for the tunable alloy-like properties.
June 23, 2017: Chemical Communications: Chem Comm
Jing Fang, Zhong-Kui Wang, Shu-Wei Wu, Wei-Guo Shen, Gui-Zhen Ao, Feng Liu
A mild and transition-metal-free protocol is herein presented for chloro-, bromo- and trifluoromethylthiotrifluoromethylation of unactivated alkenes. The easy-handling Langlois reagent, as well as N-halophthalimide and N-trifluoromethylthiosaccharin, is used in this method. In the presence of an organic photoredox catalyst N-methyl-9-mesityl acridinium, a broad range of desired products were afforded in satisfactory yields upon visible-light irradiation via a radical process.
June 23, 2017: Chemical Communications: Chem Comm
Shu-Mei Yang, Ganapuram Madhusudhan Reddy, Tzu-Ping Wang, Yu-Sheng Yeh, Min Wang, Wenwei Lin
A highly enantioselective cascade reaction for the generation of five quaternary stereocenters in one-pot operation is reported for the first time in the history of organic synthesis. Cinchona-alkaloid derived hydrogen-bonding catalyst furnished structurally complex cascade products from simple substrates in excellent yields and stereoselectivities.
June 23, 2017: Chemical Communications: Chem Comm
A Liu, L Yang, C H-H Traulsen, J J L M Cornelissen
A functional microfluidic reactor is constructed by the immobilization of gold containing virus-based protein cages that catalyze the reduction of nitro-arenes with high efficiency.
June 22, 2017: Chemical Communications: Chem Comm
M T Soper-Hopper, A S Petrov, J N Howard, S-S Yu, J G Forsythe, M A Grover, F M Fernández
Traditional methods for deriving computationally-generated collision cross sections for comparisons with ion mobility-mass spectrometry data require 3-dimensional energy-minimized structures and are often time consuming, preventing high throughput implementation. Here, we introduce a method to predict ion mobility collision cross sections of lipids and peptide analogs important in prebiotic chemistry and other fields. Using less than 100 2-D molecular descriptors this approach resulted in prediction errors of less than 2%...
June 22, 2017: Chemical Communications: Chem Comm
Synøve Ø Scottwell, Jonathan E Barnsley, C John McAdam, Keith C Gordon, James D Crowley
A 2,2'-bipyridine-appended bis(ferrocene) three tiered molecular folding ruler, can be switched from a folded conformation to an extended conformation by the addition of [Cu(CH3CN)4](PF6) and 6,6'-dimesityl-2,2'-bipyridine. This extension and contraction process could be triggered either chemically or electrochemically and was reversible.
June 22, 2017: Chemical Communications: Chem Comm
Shigetaka Nakamura, Hayato Kawabata, Kenzo Fujimoto
In the creation of double duplex formation with genomic DNA, the probe must be able to invade and hybridize to the duplex DNA. We designed new photoresponsive probes containing (CNV)K and (CN)U; these probes have a high double-duplex invasion capability upon photoirradiation.
June 22, 2017: Chemical Communications: Chem Comm
Yuriy V Zatsikha, Natalia O Didukh, Dion Nemez, Adrien C Schlachter, Paul-Ludovic Karsenti, Yuriy P Kovtun, Pierre D Harvey, Victor N Nemykin
Ferrocene-BODIPYmerocyanine dyads 5 and 6 were prepared and characterized by a variety of spectroscopic, electrochemical, and theoretical methods. Experimental and theoretical data on these NIR absorbing compounds are suggestive of unusual susceptibility (for BODIPY chromophores) of the delocalized π-system in 5 and 6 to protonation and low-potential oxidation of their π-systems.
June 22, 2017: Chemical Communications: Chem Comm
A Beneduci, G A Corrente, E Fabiano, V Maltese, S Cospito, G Ciccarella, G Chidichimo, G Gigli, A-L Capodilupo
Herein we present organic mixed-valence compounds with an innovative H-shape design, where four redox centres are bridged "vertically" via a dibenzofulvene backbone and "horizontally" via a bis-(dibenzofulvene)-thiophene bridge. These compounds are easily oxidized to stable highly charged radical species which show intense intervalence charge transfer transitions in the near infrared region. Interestingly, depending on the position of the arylamine substituents on the bridge, both vertical and horizontal electron transfer pathways can be optically induced...
June 22, 2017: Chemical Communications: Chem Comm
Xiaoqiang Huang, Jing Xue, Yushan Zhu
Computational enzyme design exhibits excellent performance for identifying potential scaffolds from structural databases and creating new enzymatic catalysts from naught. Using the active site-matching algorithm ProdaMatch, we identified a new scaffold cocaine esterase from Rhodococcus sp. that showed modest activity (kcat/Km = 0.018 M(-1) s(-1)) towards the hydrolysis of β-lactam antibiotic cephradine. The identified cocaine esterase scaffold afforded low sequence identity (<30%) with the known β-lactam synthases, such as penicillin G acylase or α-amino acid ester hydrolase, and was able to catalyze the condensation reaction between d-dihydrophenylglycine methyl ester and 7-aminodesacetoxycephalosporanic acid to produce cephradine via a kinetically controlled synthesis...
June 22, 2017: Chemical Communications: Chem Comm
K Liang, K Marcus, L Guo, Z Li, L Zhou, Y Li, S T De Oliveira, N Orlovskaya, Y-H Sohn, Yang Yang
An ultrathin, freestanding NiSx nanoporous thin-film was developed by facile electrochemical deposition, etching, anodization and chemical vapor treatments. The NiSx nanoporous thin-film shows excellent reversible insertion/extraction of Mg ions and long-term cycling performance, which is an ideal energy storage device for small/micro-size electronic and medical devices.
June 22, 2017: Chemical Communications: Chem Comm
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