Angewandte Chemie International Edition
© WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
The following papers are very important in the opinion of two referees.
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Photocatalytically Renewable Micro-electrochemical Sensor for Real-Time Monitoring of Cells
Jia-Quan Xu, Yan-Ling Liu, Qian Wang, Huan-Huan Duo, Xin-Wei Zhang, Dr. Yu-Tao Li and Prof. Wei-Hua Huang
No electrode fouling: A versatile and efficient strategy based on photocatalytic cleaning is proposed for construction of a renewable electrochemical sensor used for cell analysis. The electrode was composed of TiO2 nanoparticles wrapped by a reduced graphene oxide membrane and decorated by gold nanoparticles. The electrode was successfully used for biosensing at single-cell level.
The HOMO Nodal Arrangement in Polychromophoric Molecules and Assemblies Controls the Interchromophoric Electronic Coupling
Dr. Marat R. Talipov, Dr. Tushar S. Navale and Prof. Rajendra Rathore
Pulling the plug: A visual inspection of the HOMOs enables the ready evaluation of the electronic coupling in cofacially arrayed polychromophoric molecules/assemblies. Both qualitative and quantitative applications of this simple approach can serve as powerful methods for the rational design of next-generation charge-transport materials for photovoltaic applications.
Remote Control of the Planar Chirality in Peptide-Bound Metallomacrocycles and Dynamic-to-Static Planar Chirality Control Triggered by Solvent-Induced 310-to-α-Helix Transitions
Fumihiko Mamiya, Dr. Naoki Ousaka and Prof. Dr. Eiji Yashima
Locked rotation: The dynamic planar chirality in a nickel(II)-salphen-based macrocycle can be remotely controlled by a domino effect through the dynamic helical peptides that are bonded to the macrocycle rims. A solvent-induced conformational transition of the peptide chains from 310- to wider α-helices leads to kinetically trapped, static planar chirality.
CH Oxidation of Ingenanes Enables Potent and Selective Protein Kinase C Isoform Activation
Dr. Yehua Jin, Dr. Chien-Hung Yeh, Dr. Christian A. Kuttruff, Dr. Lars Jørgensen, Dr. Georg Dünstl, Dr. Jakob Felding, Dr. Swaminathan R. Natarajan and Prof. Dr. Phil S. Baran
Ingenious access: Ingenol derivatives with varying degrees of CH oxidation were prepared by two-phase terpene synthesis to give analogues that cannot be prepared by semisynthesis from ingenol. Since interaction with protein kinase C (PKC) was found to be dependent on oxidation level, this enabled PKC isoform selectivity, wherein PKCδ-driven activation of keratinocytes is strongly reduced while PKCβII-driven activation of neutrophils is retained.
Microporous Molecular Materials from Dipeptides Containing Non-proteinogenic Residues
Dr. Vitthal N. Yadav, Prof. Angiolina Comotti, Prof. Piero Sozzani, Dr. Silvia Bracco, Prof. Tore Bonge-Hansen, Dr. Martin Hennum and Prof. Carl Henrik Görbitz
Crystals of dipeptides comprised of a combination of proteinogenic and non-proteinogenic residues show open channels with variable and tunable diameters modulated by the bulk of the latter units. The accessibility of these novel porous materials from the gas phase is demonstrated by the adsorption isotherms of CO2 and CH4. Direct observations of captured CO2 in the 1D and 2D NMR spectra revealed close gas–matrix interaction.
Syntheses and Structures of F6XeNCCH3 and F6Xe(NCCH3)2
Dr. Kazuhiko Matsumoto, M. Sc. Jamie Haner, Dr. Hélène P. A. Mercier and Prof. Gary J. Schrobilgen
XeVIN bonds at last: Two shock-sensitive, highly explosive adducts of the potent oxidant XeF6 and CH3CN have been synthesized and characterized at low temperatures. Crystal structures and Raman spectra confirm that the title compounds represent the first examples of XeVIN bonds and a well-isolated XeF6 (C3v) moiety in the solid state. Calculations were used to assign vibrational frequencies and determine binding energies.
Direct Dual-Template Synthesis of MWW Zeolite Monolayers
Vicente J. Margarit, Marta E. Martínez-Armero, Dr. M. Teresa Navarro, Dr. Cristina Martínez and Prof. Avelino Corma
The direct synthesis of a delaminated MWW zeolite was achieved by using two organic structure-directing agents. The resultant material consists of approximately 70 % single and double layers with well preserved structural integrity and was found to be an excellent catalyst for the liquid-phase alkylation of benzene with propylene.
Influence of Arrestin on the Photodecay of Bovine Rhodopsin
Deep Chatterjee, Carl Elias Eckert, Dr. Chavdar Slavov, Dr. Krishna Saxena, Dr. Boris Fürtig, Prof. Dr. Charles R. Sanders, Prof. Dr. Vsevolod V. Gurevich, Prof. Dr. Josef Wachtveitl and Prof. Dr. Harald Schwalbe
In the twilight: The influence of arrestin (arr) on the photokinetics of the mammalian visual dim-light photoreceptor rhodopsin is studied by time-resolved liquid-state NMR spectroscopy and flash photolysis spectroscopy. The data reveal the important role of arrestin in the retinal regeneration processes in the rod outer segments: Arrestin stabilizes the metarhodopsin III state and thus induces a twofold slower retinal release.
Gold Nanoparticles Supported on a Layered Double Hydroxide as Efficient Catalysts for the One-Pot Synthesis of Flavones
Takafumi Yatabe, Dr. Xiongjie Jin, Dr. Kazuya Yamaguchi and Prof. Dr. Noritaka Mizuno
Go for gold: In the presence of gold nanoparticles supported on a Mg-Al layered double hydroxide (Au/LDH), various flavones were obtained from the corresponding 2′-hydroxyacetophenones and benzaldehydes (or benzyl alcohols). All three (four) steps of this one-pot process are catalyzed by Au/LDH in a truly heterogeneous fashion.
Energy Migration Upconversion in Manganese(II)-Doped Nanoparticles
Dr. Xiyan Li, Xiaowang Liu, Daniel M. Chevrier, Dr. Xian Qin, Dr. Xiaoji Xie, Dr. Shuyan Song, Prof. Hongjie Zhang, Prof. Peng Zhang and Prof. Xiaogang Liu
On the up: The upconversion emission of Mn2+ ions can be realized in NaGdF4:Yb/Tm@NaGdF4:Mn core–shell nanoparticles by utilizing energy migration through the gadolinium sublattice (see figure). The multiphoton upconversion process can be further enhanced under pulsed laser excitation at high power densities. The ability of the Mn2+-doped nanoparticles to easily undergo oxidization makes them attractive for use in hydrogen peroxide detection.
A Fluorescent Molecular Probe for the Detection of Hydrogen Based on Oxidative Addition Reactions with Crabtree-Type Hydrogenation Catalysts
M. Sc. Pavlo Kos and Prof. Dr. Herbert Plenio
A green light for hydrogen: The oxidative addition of H2 to a fluorophore-tagged IrI Crabtree-type complex leads to brightly fluorescent IrIII dihydride species. This fluorogenic reaction is useful for sensing hydrogen and for uncovering mechanistic details in hydrogenation reactions.
Regulating Molecular Recognition with C-Shaped Strips Attained by Chirality-Assisted Synthesis
Dr. Xiaoxi Liu, Zackariah J. Weinert, Mona Sharafi, Dr. Chenyi Liao, Prof. Jianing Li and Prof. Severin T. Schneebeli
Hosts turn into guests in the presence of preorganized, C-shaped molecular strips. Such structures can now be readily built by chirality-assisted synthesis. They embrace pillararene macrocycles in a specific binding mode that is driven by π–π stacking and solvophobic interactions. This action in turn regulates the affinity of the macrocycles for binding electron-deficient guests in a cooperative fashion.
Rapid, On-Command Debonding of Stimuli-Responsive Cross-Linked Adhesives by Continuous, Sequential Quinone Methide Elimination Reactions
Dr. Hyungwoo Kim, Dr. Hemakesh Mohapatra and Prof. Scott T. Phillips
The depolymerization of <1 mol % of a macro-cross-linker gives rise to an amplified response in stimuli-responsive cross-linked adhesives. This amplified response enables rapid and sensitive debonding in response to specific stimuli, as well as pre-programmed debonding of layers in composite materials. The use of depolymerizable macro-cross-linkers transforms an inexpensive monomer into a highly stimuli-responsive adhesive.
Synthesis and Stereochemical Assignment of Crypto-Optically Active 2H6-Neopentane
Dr. Ahmad Masarwa, Dr. Dennis Gerbig, Liron Oskar, Prof. Dr. Aharon Loewenstein, Dr. Hans Peter Reisenauer, Prof. Dr. Philippe Lesot, Prof. Dr. Peter R. Schreiner and Prof. Dr. Ilan Marek
The spectroscopic limits for chiral discrimination with NMR spectroscopy in chiral aligned media and with vibrational circular dichroism spectroscopy have been studied with sixfold-deuterated chiral neopentane. Since the stereogenicity of this compound is only due to small mass differences, the determination of its structure is particularly difficult.
Rhodium(II) Proximity-Labeling Identifies a Novel Target Site on STAT3 for Inhibitors with Potent Anti-Leukemia Activity
Matthew B. Minus, Dr. Wei Liu, Farrukh Vohidov, Prof. Moses M. Kasembeli, Dr. Xin Long, Michael J. Krueger, Prof. Alexandra Stevens, Mikhail I. Kolosov, Prof. David J. Tweardy, Prof. Edward Allan R. Sison, Prof. Michele S. Redell and Prof. Zachary T. Ball
Touching from a distance: Small molecules block STAT3 SH2 phosphotyrosine recognition by binding to the distal coiled-coil domain (CCD). Inhibition of this new CCD target site, which was identified by catalytic rhodium labeling, blocks tumor progression in a leukemia mouse model.
Nanoscale Surface Modification of Lithium-Rich Layered-Oxide Composite Cathodes for Suppressing Voltage Fade
Fenghua Zheng, Prof. Chenghao Yang, Dr. Xunhui Xiong, Jiawen Xiong, Prof. Renzong Hu, Dr. Yu Chen and Prof. Meilin Liu
Lithium-rich layered oxides, Li1.2Mn0.54Ni0.13Co0.13O2 (LLMO), were modified with a nanoscale LiFePO4 (LFP) surface according to a facile sol–gel method. This surface modification combines the advantages of bulk doping and surface coating as the LLMO crystal structure is stabilized by cationic doping and the LLMO cathode is protected from corrosion processes induced by organic electrolytes.
Ligand-Controlled Regiodivergent Copper-Catalyzed Alkylboration of Alkenes
Wei Su, Dr. Tian-Jun Gong, Xi Lu, Meng-Yu Xu, Chu-Guo Yu, Zheng-Yang Xu, Prof. Hai-Zhu Yu, Prof. Bin Xiao and Prof. Yao Fu
One way or another: The copper-catalyzed regiodivergent alkylboration of alkenes with bis(pinacolato)diboron and alkyl halides is described. The regioselectivity of the carboboration can be controlled by fine-tuning the ligand structure.
Al2O3 Nanosheets Rich in Pentacoordinate Al3+ Ions Stabilize Pt-Sn Clusters for Propane Dehydrogenation
Dr. Lei Shi, Gao-Ming Deng, Prof. Wen-Cui Li, Dr. Shu Miao, Qing-Nan Wang, Prof. Wei-Ping Zhang and Prof. An-Hui Lu
Stable and selective: γ-Al2O3 nanosheets rich in pentacoordinate Al3+ ions can well disperse and stabilize raft-like Pt-Sn clusters, which results in an increase of the electron density of the Pt sites. This material catalyzes the conversion of propane into propylene with >99 % selectivity, and minimizes coke formation and sintering processes.
Formation of Ruthenium Carbenes by gem-Hydrogen Transfer to Internal Alkynes: Implications for Alkyne trans-Hydrogenation
M. Sc. Markus Leutzsch, Dr. Larry M. Wolf, Puneet Gupta, Dr. Michael Fuchs, Prof. Walter Thiel, Dr. Christophe Farès and Prof. Alois Fürstner
Let′s stay together: Certain ruthenium complexes are able to catalyze the stereochemically highly unusual trans-hydrogenation of internal alkynes, but can also effect a geminal hydrogenation, during which both H atoms of a single H2 precursor are delivered to the very same alkyne C atom whilst the neighboring C atom is converted into a metal carbene. The significance of this finding is analyzed by PHIP NMR spectroscopy (PHIP=para-hydrogen-induced polarization transfer) and density functional calculations.
Conductive Elastomers with Autonomic Self-Healing Properties
Kun Guo, Da-Li Zhang, Xiao-Mei Zhang, Prof. Dr. Jian Zhang, Prof. Dr. Li-Sheng Ding, Prof. Dr. Bang-Jing Li and Prof. Dr. Sheng Zhang
Candidates for smart robotics: Self-healing conductive composites were prepared by connecting single-walled carbon nanotubes (SWCNTs) to a polymer network through host–guest interactions (see picture). The poly(2-hydroxyethyl methacrylate)–SWCNT composite combines bulk electrical conductivity, proximity sensitivity, humidity sensitivity, and autonomic self-healing properties.