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Chemical Communications: Chem Comm

Shiori Fujimori, Yoshiyuki Mizuhata, Norihiro Tokitoh
Ruthenium complexes having an anionic germabenzenyl ligand, [Cp*Ru{η1,η3-GeC5(t-Bu)H4}]2 (1) and [Cp*Ru{η1-GeC5(t-Bu)H4}{[η1,η5-GeC5(t-Bu)H4]RuCp*}2] (2), have been synthesized by the reaction of germabenzenylpotassium, KGeC5(t-Bu)H4, with [Cp*RuCl]4. Complexes 1 and 2 exhibit both σ- and π-type coordination and can be regarded as the first examples of a transition-metal substituted benzenoid of heavier Group 14 elements. The isolated complexes 1 and 2 have been characterized using NMR and UV-vis spectroscopy, X-ray crystallographic analysis, and theoretical calculations...
May 22, 2018: Chemical Communications: Chem Comm
Tomohiro Meguro, Norikazu Terashima, Harumi Ito, Yuka Koike, Isao Kii, Suguru Yoshida, Takamitsu Hosoya
Efficient formation of water- and air-stable aza-ylides has been achieved using the Staudinger reaction between electron-deficient aromatic azides such as 2,6-dichlorophenyl azide and triarylphosphines. The reaction proceeds rapidly and has been successfully applied to chemical modification of proteins in living cells.
May 22, 2018: Chemical Communications: Chem Comm
Tsuyoshi Sugawa, Koji Yamamoto, Tetsuro Murahashi
We report bimodal coordination behaviour of fused arenes at a Pd3 cluster site. A cyclooctatetraene-supported Pd3 cluster accommodates anthracene and tetracene in an oxidative π-addition manner, whereas triphenylene and fluoranthene are accommodated in a π-coordination manner.
May 22, 2018: Chemical Communications: Chem Comm
Shinichi Sato, Kensuke Hatano, Michihiko Tsushima, Hiroyuki Nakamura
We designed and synthesised peptides conjugated with proline linkers and ruthenium photocatalysts. These peptides were used as substrates to evaluate the photocatalyst-proximity dependences of candidates for tyrosine labelling reagents. The 1-methyl-4-aryl-urazole (MAUra) structure was found to be a novel tyrosyl radical trapping agent to label tyrosine residues effectively under the conditions where the ruthenium photocatalyst and tyrosine were in close proximity. Using a ruthenium photocatalyst conjugated to a carbonic anhydrase ligand, the target protein in a complex protein mixture was labelled with remarkable target selectivity by azide- or desthiobiotin-conjugated MAUra derivatives...
May 22, 2018: Chemical Communications: Chem Comm
Qingqing Wang, Yuye Zhao, Wei Luo, Weizhong Jiang, Jianwei Fan, Lianjun Wang, Wan Jiang, Wei-Xian Zhang, Jianping Yang
A spatially confined reduction strategy for the fabrication of small nanoparticles in a micro-box is reported, where iron nanoparticles with uniform diameter are highly distributed in a carbon matrix and surrounded by a mesoporous silica layer. Due to their unique confined nanostructure, the Fe/C@mSiO2 capsules could effectively remove and recycle Se(iv) from a low concentration solution.
May 22, 2018: Chemical Communications: Chem Comm
Haina Jia, Yuhong Wang, Shoujun Xu
Probing biomolecular motion beyond a single nucleotide is technically challenging but fundamentally significant. We have developed super-resolution force spectroscopy (SURFS) with 0.5 pN force resolution and revealed that the ribosome moves by half a nucleotide upon the formation of the pre-translocation complex, which is beyond the resolution of other techniques.
May 22, 2018: Chemical Communications: Chem Comm
Weixin Huang, Subha Sadhu, Pitambar Sapkota, Sylwia Ptasinska
The optical and structural properties of hybrid perovskites can be tuned by the post-synthetic introduction of new cations. To advance the development of this approach, knowledge of the reaction mechanism is essential, but has not yet been elucidated. Here, the effect of n-octylamine on three-dimensional (3D) methylammonium lead bromide (MAPbBr3) was investigated by in situ X-ray photoelectron spectroscopy. Spectroscopic analysis indicated equimolar substitutions between octylammonium (OcA+) and methylammonium (MA+) cations that cause the formation of two-dimensional (2D) octylammonium lead bromide ((OcA)2PbBr4)...
May 22, 2018: Chemical Communications: Chem Comm
Alex I Wixtrom, Zeeshan A Parvez, Miles D Savage, Elaine A Qian, Dahee Jung, Saeed I Khan, Arnold L Rheingold, Alexander M Spokoyny
We report a new class of redox-active vertex-differentiated dodecaborate clusters featuring pentafluoroaryl groups. These [B12(OR)11NO2] clusters share several unique photophysical properties with their [B12(OR)12] analogues, while exhibiting significantly higher (+0.5 V) redox potentials. This work describes the synthesis, characterization, and isolation of [B12(O-CH2C6F5)11NO2] clusters in all 3 oxidation states (dianion, radical, and neutral). Reactivity to post-functionalization with thiol species via SNAr on the pentafluoroaryl groups is also demonstrated...
May 22, 2018: Chemical Communications: Chem Comm
Tomoki Tateishi, Shumpei Kai, Yuya Sasaki, Tatsuo Kojima, Satoshi Takahashi, Shuichi Hiraoka
An NMR-based quantitative analysis of self-assembly process (QASAP) for the self-assembly of a Pd3L6 double-walled triangle (DWT) from PdPy*4(BF4)2 (Py* indicates 3-chloropyridine) and V-shaped ditopic ligands (L) revealed that DWT was assembled through trinuclear single-walled chains, in which the intramolecular macrocyclization and the formation of double-walls took place leading to the final assembly.
May 21, 2018: Chemical Communications: Chem Comm
Sumanta Banerjee, Ankur, Alex Andrews, Ajay Venugopal
The ability of the β-CH functionality in a butylmagnesium cation [Me6TREN-Mg-n-Bu]+ to quantitatively reduce benzophenone has been demonstrated. The hydridic nature of the β-CH functionality is highlighted by its abstraction using B(C6F5)3. β-CH abstraction over alkylation in [Me6TREN-Mg-n-Bu]+ is dependent on the nature of the incoming electrophile and the polarity of the solvent.
May 21, 2018: Chemical Communications: Chem Comm
B A Trofimov, K V Belyaeva, L P Nikitina, A G Mal'kina, A V Afonin, I A Ushakov, A V Vashchenko
Transition metal-free one-pot reaction of quinolines with acylarylacetylenes and water proceeds in the presence of KOH (55-60 °C, MeCN, 48 h) to afford 2-aryl-3-acylquinolines in up to 66% yield. Here, a formal replacement of the acetylene moiety by the aryl and acyl substituents in the quinoline scaffold takes place. In fact, it has been proved experimentally that the reaction involves the ring cleavage, accompanied by the rearrangement and insertion of the electron-deficient acetylene moiety to form a dihydroquinoline intermediate with an aldehyde functional group in position 4...
May 21, 2018: Chemical Communications: Chem Comm
Duo Zhang, Han Wang, Carsten Bolm
Reacting N-Br sulfoximines with ammonium thiocyanate leads to unprecedented sulfur reagents, which add to vinyl arenes under photocatalysis via N-centered sulfoximidoyl radicals. As a result, 1,2-difunctionalised products are obtained, which can subsequently be derivatised taking advantage of the unique properties of the thiocyanate group.
May 21, 2018: Chemical Communications: Chem Comm
Chunqing Ma, Ming-Fai Lo, Chun-Sing Lee
Stabilization of two-dimensional (2D) PEA2PbI4 (PEA is phenethylammonium) perovskite nanocrystals (PNCs) in water is achieved. By inhibiting the desorption process, the PNCs show exceptional stability for more than 2 months in PEA+ aqueous solutions. Stabilized PNCs are successfully applied for probing Cu2+ in aqueous solution.
May 21, 2018: Chemical Communications: Chem Comm
Katherine A Gentry, Meng Zhang, Sang-Choul Im, Lucy Waskell, Ayyalusamy Ramamoorthy
Investigating the interplay between cytochrome-P450 and its redox partners (CPR and cytochrome-b5) is vital for understanding the metabolism of most hydrophobic drugs. Dynamic structural interactions with the ternary complex, with and without substrates, captured by NMR reveal a gating mechanism for redox partners to promote P450 function.
May 21, 2018: Chemical Communications: Chem Comm
Xuehua Dong, Ling Huang, Qingyu Liu, Hongmei Zeng, Zhien Lin, Dingguo Xu, Guohong Zou
A promising UV nonlinear optical material, beryllium-free nitrate Ba2NO3(OH)3, has been synthesized via modified high-temperature solid state reactions in a self-made high-pressure apparatus which exhibits a perfect balance of a large second harmonic generation coefficient, an appropriate birefringence for phase matching, a short UV absorption cutoff edge and physicochemical stabilities.
May 21, 2018: Chemical Communications: Chem Comm
Qi Li, Adam J Zaczek, Timothy M Korter, J Axel Zeitler, Michael T Ruggiero
In ZIF-8 and its cobalt analogue ZIF-67, the imidazolate methyl-groups, which point directly into the void space, have been shown to freely rotate - even down to cryogenic temperatures. Using a combination of experimental terahertz time-domain spectroscopy, low-frequency Raman spectroscopy, and state-of-the-art ab initio simulations, the methyl-rotor dynamics in ZIF-8 and ZIF-67 are fully characterized within the context of a quantum-mechanical hindered-rotor model. The results lend insight into the fundamental origins of the experimentally observed methyl-rotor dynamics, and provide valuable insight into the nature of the weak interactions present within this important class of materials...
May 21, 2018: Chemical Communications: Chem Comm
Zhongcheng Yuan, Sai Bai, Zhibo Yan, Jun-Ming Liu, Feng Gao
We investigate the effect of commonly used solution-processed TiOx, SnO2 and ZnO interlayers on the perovskite film crystallization process. We find that the ZnO/perovskite interface can efficiently catalyze the perovskite crystallization even without thermal annealing.
May 21, 2018: Chemical Communications: Chem Comm
Youhei Takeda, Takahito Kaihara, Masato Okazaki, Heather Higginbotham, Przemyslaw Data, Norimitsu Tohnai, Satoshi Minakata
A novel twisted donor-acceptor-donor (D-A-D) π-conjugated compound that contains flexible and moderately-electron-donating units has been designed and synthesized. It exhibited not only multi-color-changing mechanochromic luminescence and thermally activated delayed fluorescence, but also, unexpectedly, room-temperature phosphorescence in a host layer.
May 21, 2018: Chemical Communications: Chem Comm
Hae-Geun Jeon, Hyun Kyung Lee, Seungwon Lee, Kyu-Sung Jeong
A new double-stranded dinuclear helicate that displays conformational switching in response to temperature was prepared by self-assembly of an aromatic helical foldamer and dichloropalladium(ii). The relative populations of the two helicate conformers, syn-anti and syn-syn, were demonstrated to be reversibly modulated through temperature control.
May 21, 2018: Chemical Communications: Chem Comm
Tongyang Hu, Jun He, Shaomin Zhang, Xuan Mei, Weiku Zhang, Ruizheng Liang, Min Wei, David G Evans, Xue Duan
An ultrathin photosensitizer was prepared by immobilization of chlorin e6 (Ce6) and carbon dots (CDs) onto layered double hydroxide (LDH) nanosheets, which exhibited excellent fluorescence imaging and photodynamic therapy performance toward cancer theranostics.
May 21, 2018: Chemical Communications: Chem Comm
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