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Chemical Communications: Chem Comm

James R Hickson, Samuel J Horsewill, Jake McGuire, Claire Wilson, Stephen Sproules, Joy H Farnaby
Reduction of 1,10-phenanthroline-5,6-dione (pd) with CoCpR2 resulted in the first molecular compounds of the pd˙- semi-quinone radical anion, [CoCpR2]+[pd]˙- (R = H, (1); R = Me4, (2)). Furthermore compounds 1 and 2 were reacted with [Y(hfac)3(thf)2] (hfac = 1,1,1-5,5,5-hexafluoroacetylacetonate) to synthesise the rare earth-transition metal heterometallic compounds, [CoCpR2]+[Y(hfac)3(N,N'-pd)]˙- (R = H, (3); R = Me4, (4)).
September 21, 2018: Chemical Communications: Chem Comm
Xiaojuan Zhu, Zaichun Liu, Qin Liu, Yonglan Luo, Xifeng Shi, Abdullah M Asiri, Yuping Wu, Xuping Sun
NH3 is one of the most important chemicals with a wide range of applications. NH3 is mainly produced via the Haber-Bosch process, which leads to large energy consumption and carbon emission. Electrochemical reduction has emerged as an environmentally-benign and sustainable alternative for artificial N2 fixation under ambient conditions, but needs materials to effectively catalyze the N2 reduction reaction (NRR). In this communication, we report that β-FeOOH nanorods behave as an efficient and durable NRR electrocatalyst...
September 21, 2018: Chemical Communications: Chem Comm
Haishan Qi, Weiwei Zheng, Xiao Zhou, Chen Zhang, Lei Zhang
A mussel-inspired chimeric protein as a multifunctional coating was engineered rationally and applied in antifouling. 3,4-Dihydroxyphenyl-alanine (Dopa) and zwitterionic peptides inspired from molecular chaperones were incorporated into the designed protein. The multifunctional protein coating can anchor onto various substrates surfaces readily and exhibits superior antifouling properties.
September 21, 2018: Chemical Communications: Chem Comm
Shenghong Zhong, Xiulin Yang, Zhen Cao, Xinglong Dong, Sergey M Kozlov, Laura Falivene, Jing-Kai Huang, Xiaofeng Zhou, Mohamed N Hedhili, Zhiping Lai, Kuo-Wei Huang, Yu Han, Luigi Cavallo, Lain-Jong Li
A simple and efficient catalyst, benzimidazole (BIMH)-modified copper foil, is developed to enhance the selective conversion of CO2 to C2/C3 products. The overall faradaic efficiency (FE) for CO2 reduction reaches 92.1% and the undesired hydrogen evolution reaction (HER) is lowered to a FE of 7% at -1.07 VRHE.
September 21, 2018: Chemical Communications: Chem Comm
Shintaro Kawamura, Cassandra J Henderson, Yuma Aoki, Daisuke Sekine, Shū Kobayashi, Mikiko Sodeoka
We developed a practical chlorodifluoromethylation reaction mediated by diacyl peroxide generated in situ from chlorodifluoroacetic anhydride. Allylic and amino-chlorodifluoromethylations of alkenes proceeded well with the combination of this reagent, Cu(ii) catalyst and a pyridine additive. Carbo- and aromatic chlorodifluoromethylations proceeded under metal-free conditions.
September 21, 2018: Chemical Communications: Chem Comm
Chen Qian, Taka-Aki Asoh, Hiroshi Uyama
A novel strategy for fabricating sea cucumber-mimicking hydrogels composed of a bacterial cellulose matrix and a stimuli-responsive polymer is presented. This mechanically adaptive hydrogel shows a unique reversible stiffness change in response to its ionic strength without any significant volume changes.
September 21, 2018: Chemical Communications: Chem Comm
James L Galman, Iustina Slabu, Fabio Parmeggiani, Nicholas J Turner
Heterocycles based on piperidine and pyrrolidine are key moieties in natural products and pharmaceutically active molecules. A novel multi-enzymatic approach based on the combination of a lipase with an α,ω-diamine transaminase is reported, opening up the synthesis, isolation and characterisation of a broad range of 2-substituted N-heterocycle alkaloids.
September 21, 2018: Chemical Communications: Chem Comm
Peng Sun, Zhen Li, Jingyun Wang, Hui Gao, Xi Yang, Sudong Wu, Deqiang Liu, Qixian Chen
A supramolecular catiomer with a metal-organic framework (MOF) motif was developed to manufacture messenger RNA (mRNA) assemblies. In contrast to the linear catiomer, the dendritic MOF catiomer appeared to markedly improve the colloidal stability of the mRNA assemblies, particularly affording substantial protection to the mRNA payloads from enzymatic degradation, eventually conducing to appreciable mRNA transfection activities at the targeted cells.
September 20, 2018: Chemical Communications: Chem Comm
Songjun Xiao, Jeffery T Davis
A G4·K+ hydrogel made from 5'-hydrazinoguanosine and KCl reacts with α,β-unsaturated carbonyls of different electrophilicities (acrolein, methyl vinyl ketone and methyl acrylate) in water and the gas phase to form cyclic adducts. This aza-Michael addition/cyclization domino reaction by the 5'-hydrazino G4·K+ hydrogel has promise for environmental remediation of toxic α,β-unsaturated carbonyls from water and the atmosphere.
September 20, 2018: Chemical Communications: Chem Comm
Jutao Jiang, Guangzhan Shao, Zelong Zhang, Ling Ding, Huiling Zhang, Jianming Liu, Zhaoping Chen, Weidong Xiang, Xiaojuan Liang
A series of CsPbBrxI3-x NC glasses, showing tunable emission (523-693 nm) controlled by different ratios of Br- and I-, were successfully prepared. The CsPbBrxI3-x NC glasses exhibited excellent optical properties and outstanding stability towards ambient conditions, water and heat.
September 20, 2018: Chemical Communications: Chem Comm
Xuewei Liang, Yunjun Shen, Kang Zhang, Jiyong Liu, Simon Duttwyler
closo-Boranes and closo-carboranes, clusters with a closed-cage structure, exhibit remarkable inertness and are unique components of products with applications in areas such as medicinal chemistry, fluorescence and materials science. Herein, we report the first transition metal-catalyzed functionalization of the mono-closo-decaborate cluster [1-CB9H10]- by regioselective B-H activation. Using terminal alkenes bearing a wide range of functional groups, dehydrogenative coupling under mild conditions leads to B2/3-dialkenylated products, as verified by X-ray crystallography and NMR studies...
September 20, 2018: Chemical Communications: Chem Comm
Dong-Cheng Liu, Hong-Juan Wang, Jia-Wei Wang, Di-Chang Zhong, Long Jiang, Tong-Bu Lu
Herein, we report a mononuclear Co(ii) cryptate which exhibits highly efficient and selective photocatalytic CO2-to-CO conversion in H2O/CH3CN solution. The TON and selectivity reach as high as 51 392 and 98%, respectively.
September 20, 2018: Chemical Communications: Chem Comm
Yingyi Wang, Qian Su, Xiaoming Yang
Currently, the synthesis of carbon dots (CDs) exhibiting long-wavelength emission is still challenging. Herein, we have synthesized for the first time three types of CD with multicolor emission derived from isomers. Importantly, their particle size, nitrogen-doping amount and band gaps collectively regulate the fluorescence emission of the proposed CDs.
September 20, 2018: Chemical Communications: Chem Comm
Ye Tao, Scott R Gilbertson
The bis(trifluoromethane)sulfonimide (Tf2NH) catalyzed intramolecular hydroamidation of terminal alkynes is reported. The combination of Et3SiH and Tf2NH provides cis-1,3-disubstituted isoindolines and sultams in high yield (up to 98%) and high diastereoselectivity (up to 99 : 1 d.r.).
September 20, 2018: Chemical Communications: Chem Comm
Michael D Dore, Johans J Fakhoury, Aurélie Lacroix, Hanadi F Sleiman
RNA has inherent therapeutic and structural properties that make it an important component of biologically-functional nanoparticles. Using DNA-amphiphiles as synthetic templates, we report the synthesis of two classes of RNA-amphiphiles that self-assemble into spherical nanoparticles in aqueous solution and show gene silencing activity.
September 20, 2018: Chemical Communications: Chem Comm
Yu Shen, Tao Shao, Bin Fang, Wei Du, Mingzhu Zhang, Jiejie Liu, Tianyan Liu, Xiaohe Tian, Qiong Zhang, Aidong Wang, Jiaxiang Yang, Jieying Wu, Yupeng Tian
We present a thiophene-based terpyridine Zn(ii) complex (namely LC) which could specifically target live cell mitochondria via binding with mitochondrial DNA (mtDNA). Due to its high biocompatibility, red emission and photo-stability, mtDNA distribution within mitochondrial cristae and inner matrix in living cells was successfully visualized using stimulated emission depletion (STED) nanoscopy with unprecedented resolution.
September 20, 2018: Chemical Communications: Chem Comm
Huajun Yang, Min Luo, Zhou Wu, Wei Wang, Chaozhuang Xue, Tao Wu
We demonstrated here a novel semiconducting metal-chalcogenide-organic framework (MCOF-89) with an optical bandgap through the unlikely assembly between a metal chalcogenide unit and carboxylic acid. The elusive metal-chalcogenide unit [Mn4(μ4-S)] with square-planar tetra-coordinated sulfur (sptS) is for the first time observed in MOFs.
September 20, 2018: Chemical Communications: Chem Comm
Sam Mathew, Milos Trajkovic, Hemant Kumar, Quoc-Thai Nguyen, Marco W Fraaije
In the past decade it has become clear that many microbes harbor enzymes that employ an unusual flavin cofactor, the F420 deazaflavin cofactor. Herein we show that F420-dependent reductases (FDRs) can successfully perform enantio-, regio- and chemoselective ene-reductions. For the first time, we have demonstrated that F420H2-driven reductases can be used as biocatalysts for the reduction of α,β-unsaturated ketones and aldehydes with good conversions (>99%) and excellent regioselectivities and enantiomeric excesses (>99% ee)...
September 19, 2018: Chemical Communications: Chem Comm
Igor V Kolesnichenko, P Rogelio Escamilla, Jason A Michael, Vincent M Lynch, David A Vanden Bout, Eric V Anslyn
We demonstrate that bisulfite can be used for reduction of a highly electrophilic anthraquinone derivative, N,N'-dimethyl-2,6-diaza-9,10-anthraquinonediium (DAAQ), and subsequent autoxidation generates an equivalent of hydrogen peroxide. The mechanism for DAAQ reduction by bisulfite, DAAQ electrochemistry, and use of a simple test strip assay for H2O2, are described.
September 19, 2018: Chemical Communications: Chem Comm
Mahadev Sharanappa Sherikar, Raja Kapanaiah, Veeranjaneyulu Lanke, Kandikere Ramaiah Prabhu
A Rh(iii)-catalyzed C-H activation of indole at the C4-position leading to novel and switchable functionalization has been reported by employing a weakly co-ordinating COCF3 group as a directing group. An additive plays an important role in switching the selectivity between 1,4-addition products and Heck-type products. An acid additive led to the formation of 1,4-addition products whereas a base additive promotes the formation of Heck-type products. Deuteration studies and control experiments were helpful to propose the mechanism...
September 19, 2018: Chemical Communications: Chem Comm
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