Angewandte Chemie International Edition

Cover image for Vol. 54 Issue 5

Editor: Peter Gölitz, Deputy Editors: Neville Compton, Haymo Ross

Online ISSN: 1521-3773

Associated Title(s): Angewandte Chemie, Chemistry - A European Journal, Chemistry – An Asian Journal, ChemistryOpen, ChemPlusChem, Zeitschrift für Chemie

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January 23, 2015

Hot Paper: Palladium versus Platinum: The Metal in the Catalytic Center of a Molecular Photocatalyst Determines the Mechanism of the Hydrogen Production with Visible Light

Michael G. Pfeffer, Dr. Bernhard Schäfer, Dr. Grigory Smolentsev, Dr. Jens Uhlig, Dr. Elena Nazarenko, Dr. Julien Guthmuller, Dr. Christian Kuhnt, Dr. Maria Wächtler, Prof. Dr. Benjamin Dietzek, Prof. Dr. Villy Sundström and Prof. Dr. Sven Rau

Palladium versus Platinum: The Metal in the Catalytic Center of a Molecular Photocatalyst Determines the Mechanism of the Hydrogen Production with Visible LightShow your metal: The mechanism of the visible light-driven hydrogen production with an intramolecular photocatalyst depends on the nature of the catalytically active metal center. In Ru–M systems, where M=Pt or Pd, palladium forms metal colloids as initial step, whereas platinum shows a high stability and there is no change in the (N^N)PtCl2 coordination sphere.

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January 23, 2015

Hot Paper: Total Synthesis of (−)-Caprazamycin A

Hugh Nakamura, Dr. Chihiro Tsukano, Motohiro Yasui, Shinsuke Yokouchi, Dr. Masayuki Igarashi and Prof. Dr. Yoshiji Takemoto

Total Synthesis of (−)-Caprazamycin AAbra‘capraza’: Caprazamycin A has significant antibacterial activity against Mycobacterium tuberculosis (TB). The first total synthesis is herein reported and features the scalable preparation of the syn-β-hydroxy amino acid with a thiourea-catalyzed diastereoselective aldol reaction, construction of a diazepanone with an unstable fatty-acid side chain, and global deprotection with hydrogenation.

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January 22, 2015

VIP: Remarkably Enhanced Gas Separation by Partial Self-Conversion of a Laminated Membrane to Metal–Organic Frameworks

Dr. Yi Liu, Dr. Jia Hong Pan, Nanyi Wang, Frank Steinbach, Dr. Xinlei Liu and Prof. Jürgen Caro

Remarkably Enhanced Gas Separation by Partial Self-Conversion of a Laminated Membrane to Metal–Organic FrameworksFrom LDH to MOF: The partial transformation of a ZnAl-NO3 layered double hydroxide (LDH) membrane to a ZIF-8 metal–organic framework (MOF) top layer led to the formation of the composite membrane ZIF-8-ZnAl-NO3 LDH. This membrane is characterized by remarkably enhanced H2/CH4 gas separation and H2 permeance.

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January 21, 2015

Hot Paper: Heterogeneous Water Oxidation: Surface Activity versus Amorphization Activation in Cobalt Phosphate Catalysts

Diego González-Flores, Irene Sánchez, Dr. Ivelina Zaharieva, Katharina Klingan, Jonathan Heidkamp, Dr. Petko Chernev, Dr. Prashanth W. Menezes, Prof. Dr. Matthias Driess, Prof. Dr. Holger Dau and Dr. Mavis L. Montero

Heterogeneous Water Oxidation: Surface Activity versus Amorphization Activation in Cobalt Phosphate CatalystsThe complete transformation during catalytic operation of crystalline and surface-active Co3(PO4)2⋅8 H2O into amorphous and volume-active cobalt oxide reveals basic features of heterogeneous water oxidation catalysis, which is discussed as a convolution of three phenomena: surface catalysis, volume catalysis, and restructuring of the material under operation.

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January 21, 2015

VIP: Lithium Imide Synergy with 3d Transition-Metal Nitrides Leading to Unprecedented Catalytic Activities for Ammonia Decomposition

Jianping Guo, Peikun Wang, Prof. Dr. Guotao Wu, Prof. Dr. Anan Wu, Daqiang Hu, Prof. Dr. Zhitao Xiong, Prof. Dr. Junhu Wang, Pei Yu, Fei Chang, Zheng Chen and Prof. Dr. Ping Chen

Lithium Imide Synergy with 3d Transition-Metal Nitrides Leading to Unprecedented Catalytic Activities for Ammonia DecompositionBeyond an electronic promoter: A synergy between Li2NH and 3d transition-metal nitrides leads to unprecedented catalytic activities for NH3 decomposition. Li2NH acts as more than just an electronic promoter: it is an NH3 transmitting agent and favors the formation of a higher N-content intermediate, thereby altering the overall reaction energetics.

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January 20, 2015

VIP: A D-Peptide Ligand of Nicotine Acetylcholine Receptors for Brain-Targeted Drug Delivery

Xiaoli Wei, Dr. Changyou Zhan, Qing Shen, Prof. Wei Fu, Cao Xie, Jie Gao, Chunmei Peng, Prof. Ping Zheng and Prof. Weiyue Lu

A <span class="smallCaps">D</span>-Peptide Ligand of Nicotine Acetylcholine Receptors for Brain-Targeted Drug DeliveryA D-peptide ligand of nicotine acetylcholine receptors (nAChRs), termed DCDX, was developed. The function of DCDX as a D-peptide antagonist of nAChRs was experimentally and computationally validated. DCDX exhibits exceptional stability during nAChRs-mediated transcytosis and in blood circulation, offering potential for brain-targeting drug delivery in the treatment of central nervous system diseases.

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January 20, 2015

VIP: Synergistic Interplay of a Non-Heme Iron Catalyst and Amino Acid Coligands in H2O2 Activation for Asymmetric Epoxidation of α-Alkyl-Substituted Styrenes

Olaf Cussó, Dr. Xavi Ribas, Dr. Julio Lloret-Fillol and Dr. Miquel Costas

Synergistic Interplay of a Non-Heme Iron Catalyst and Amino Acid Coligands in H2O2 Activation for Asymmetric Epoxidation of α-Alkyl-Substituted StyrenesCome on styrene: Using amino acids as coligands for bioinspired non-heme iron catalysts, the substrate scope of epoxidation reactions with aqueous H2O2 is extended to the challenging α-styrenes. Thus, these systems can be adapted for new substrates classes simple by changing the amino acid coligand.

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January 20, 2015

VIP: Electron Tunneling Rates in Respiratory Complex I Are Tuned for Efficient Energy Conversion

Prof. Dr. Simon de Vries, Dr. Katerina Dörner, Marc J. F. Strampraad and Prof. Dr. Thorsten Friedrich

Electron Tunneling Rates in Respiratory Complex I Are Tuned for Efficient Energy ConversionThe reduction of ubiquinone by NADH is catalyzed by flavin mononucleotide and a chain of seven iron–sulfur centers. The electron transfer rates between the centers indicate that the Fe–S chain synchronizes the electron transfer rate to match the time scale of the conformational changes required for proton translocation.

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January 19, 2015

Angewandte Chemie 4/2015: Curiosity and Applications

Angewandte Chemie 4/2015: Curiosity and ApplicationsIn this issue, I. Willner et al. review principles and applications of DNA switches. How can drug delivery, opening/closure of pores, and switchable catalysis be enabled? In a Minireview, D. Leonori and V. K. Aggarwal discuss stereospecific couplings of secondary and tertiary boronic esters. The Highlight deals with the range of oxidation states of iridium (P. Pyykkö and W.-H. Xu).

In the Communications section, D. C. Johnson et al. describe how the synthesis of inorganic structural isomers can be achieved by diffusion-constrained self-assembly of designed precursors (see picture). C. Poriel et al. report on derivatives of dihydroindenofluorene isomers as host materials for phosphorescent OLEDs. K. Tomooka et al. present the concise synthesis, structural analysis, and reactions of heteratom-embedded medium-sized cycloalkynes.

Browse issue 4/2015 now.

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January 15, 2015

VIP: Tetracyclopenta[def,jkl,pqr,vwx]tetraphenylene: A Potential Tetraradicaloid Hydrocarbon

Dr. Shunpei Nobusue, Hirokazu Miyoshi, Dr. Akihiro Shimizu, Dr. Ichiro Hisaki, Kotaro Fukuda, Prof. Masayoshi Nakano and Prof. Yoshito Tobe

Tetracyclopenta[def,jkl,pqr,vwx]tetraphenylene: A Potential Tetraradicaloid HydrocarbonAromatic? A tetramesityl derivative of hitherto unknown tetracyclopenta[def,jkl,pqr,vwx]tetraphenylene, a potential tetraradicaloid hydrocarbon, was synthesized. It exhibits remarkable antiaromaticity as a result of the peripheral 20-π-electron circuit. In solution, it adopts closed-shell D2h structures that rapidly equilibrate via the D4h structure, and in crystals, it adopts an approximate D2h structure.

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January 14, 2015

Hot Paper: Gas-Separation Membranes Loaded with Porous Aromatic Frameworks that Improve with Age

Dr. Cher Hon Lau, Dr. Kristina Konstas, Dr. Aaron W. Thornton, Dr. Amelia C. Y. Liu, Dr. Stephen Mudie, Dr. Danielle F. Kennedy, Dr. Shaun C. Howard, Dr. Anita J. Hill and Dr. Matthew R. Hill

Gas-Separation Membranes Loaded with Porous Aromatic Frameworks that Improve with AgeLike red wine, membranes can improve with age. Small cavities of a permeable membrane (PIM-1) are prevented from collapsing using PAF-1 nanoparticles. Larger cavities however collapse over time. The result is that as the membrane ages, the transport of small gas molecules over larger gas molecules is preferred. Thus the membrane’s gas-separation properties improve with age.

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January 14, 2015

VIP: Controlling the Subtle Energy Balance in Protic Ionic Liquids: Dispersion Forces Compete with Hydrogen Bonds

Dr. Koichi Fumino, M. Sc. Verlaine Fossog, B. Sc. Peter Stange, Dr. Dietmar Paschek, Prof. Dr. Rolf Hempelmann and Prof. Dr. Ralf Ludwig

Controlling the Subtle Energy Balance in Protic Ionic Liquids: Dispersion Forces Compete with Hydrogen BondsThe winner is … Dispersion forces compete with hydrogen bonds in a protic ionic liquid. The energy balance can be controlled by the hydrogen-bond interaction strength of the anion and the alkyl-chain lengths of the cation. The energy of conversion between the H-bonded and the dispersion-dominated ion pairs can be determined experimentally by far-infrared spectroscopy. Dispersion-corrected DFT methods are essential for reproducing the experimental results.

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January 23, 2015
Hot Paper: Palladium versus Platinum: The Metal in the Catalytic Center of a Molecular Photocatalyst Determines the Mechanism of the Hydrogen Production with Visible Light

January 23, 2015
Hot Paper: Total Synthesis of (−)-Caprazamycin A

January 22, 2015
VIP: Remarkably Enhanced Gas Separation by Partial Self-Conversion of a Laminated Membrane to Metal–Organic Frameworks

January 21, 2015
Hot Paper: Heterogeneous Water Oxidation: Surface Activity versus Amorphization Activation in Cobalt Phosphate Catalysts

January 21, 2015
VIP: Lithium Imide Synergy with 3d Transition-Metal Nitrides Leading to Unprecedented Catalytic Activities for Ammonia Decomposition

January 20, 2015
VIP: A D-Peptide Ligand of Nicotine Acetylcholine Receptors for Brain-Targeted Drug Delivery

January 20, 2015
VIP: Synergistic Interplay of a Non-Heme Iron Catalyst and Amino Acid Coligands in H2O2 Activation for Asymmetric Epoxidation of α-Alkyl-Substituted Styrenes

January 20, 2015
VIP: Electron Tunneling Rates in Respiratory Complex I Are Tuned for Efficient Energy Conversion

January 19, 2015
Angewandte Chemie 4/2015: Curiosity and Applications

January 15, 2015
VIP: Tetracyclopenta[def,jkl,pqr,vwx]tetraphenylene: A Potential Tetraradicaloid Hydrocarbon

January 14, 2015
Hot Paper: Gas-Separation Membranes Loaded with Porous Aromatic Frameworks that Improve with Age

January 14, 2015
VIP: Controlling the Subtle Energy Balance in Protic Ionic Liquids: Dispersion Forces Compete with Hydrogen Bonds

January 10, 2015
Hot Paper: Tunable Release of Multiplex Biochemicals by Plasmonically Active Rotary Nanomotors

January 09, 2015
Hot Paper: Nickel-Catalyzed Monoarylation of Ammonia

January 09, 2015
Hot Paper: Antibody Activation using DNA-Based Logic Gates

January 09, 2015
Hot Paper: Ratiometric Fluorescence Imaging of Cellular Polarity: Decrease in Mitochondrial Polarity in Cancer Cells

January 09, 2015
VIP: Elucidation of the Concise Biosynthetic Pathway of the Communesin Indole Alkaloids

January 08, 2015
Hot Paper: Indolo-Phakellins as β5-Specific Noncovalent Proteasome Inhibitors

January 07, 2015
Hot Paper: The Nature of Photocatalytic “Water Splitting” on Silicon Nanowires

January 07, 2015
Hot Paper: A Small-Molecule Protein–Protein Interaction Inhibitor of PARP1 That Targets Its BRCT Domain

January 07, 2015
Hot Paper: Atomically Thin Arsenene and Antimonene: Semimetal–Semiconductor and Indirect–Direct Band-Gap Transitions

January 07, 2015
Hot Paper: Enhanced Electron Penetration through an Ultrathin Graphene Layer for Highly Efficient Catalysis of the Hydrogen Evolution Reaction

January 07, 2015
Hot Paper: Visible-Light-Driven CO2 Reduction with Carbon Nitride: Enhancing the Activity of Ruthenium Catalysts

January 07, 2015
Hot Paper: Sensitive and Multiplexed On-chip microRNA Profiling in Oil-Isolated Hydrogel Chambers

December 31, 2014
Hot Paper: Generation of a Genetically Encoded, Photoactivatable Intein for the Controlled Production of Cyclic Peptides

December 31, 2014
Hot Paper: The Phosphinoboration Reaction

December 31, 2014
Hot Paper: Unraveling the Intrinsic Color of Chlorophyll

December 31, 2014
Hot Paper: Application of Fragment-Based Screening to the Design of Inhibitors of Escherichia coli DsbA

December 30, 2014
Hot Paper: Excluded-Volume Effects in Living Cells

December 30, 2014
VIP: Rational Design of a Humanized Glucagon-Like Peptide-1 Receptor Agonist Antibody

December 30, 2014
VIP: Programmable Engineering of a Biosensing Interface with Tetrahedral DNA Nanostructures for Ultrasensitive DNA Detection

December 24, 2014
Hot Paper: Krebs Cycle Metabolon: Structural Evidence of Substrate Channeling Revealed by Cross-Linking and Mass Spectrometry

December 24, 2014
Hot Paper: Live-Cell Imaging of Endogenous mRNAs with a Small Molecule

December 24, 2014
VIP: Crystalline Stereocomplexed Polycarbonates: Hydrogen-Bond-Driven Interlocked Orderly Assembly of the Opposite Enantiomers

December 22, 2014
Hot Paper: Liquid-Phase Epitaxial Growth of Two-Dimensional Semiconductor Hetero-nanostructures

December 18, 2014
Hot Paper: Cyclic Alkyl Amino Carbene (CAAC) Ruthenium Complexes as Remarkably Active Catalysts for Ethenolysis

December 18, 2014
Hot Paper: Unusual Ultra-Hydrophilic, Porous Carbon Cuboids for Atmospheric-Water Capture

December 18, 2014
Hot Paper: Phosphorus-Doped Graphitic Carbon Nitrides Grown in Situ on Carbon-Fiber Paper: Flexible and Reversible Oxygen Electrodes

December 18, 2014
Hot Paper: Hydrodeoxygenation of Vicinal OH Groups over Heterogeneous Rhenium Catalyst Promoted by Palladium and Ceria Support

December 18, 2014
Hot Paper: Synthesis of Inorganic Structural Isomers By Diffusion-Constrained Self-Assembly of Designed Precursors: A Novel Type of Isomerism

December 16, 2014
VIP: CO-Extrusion in Homogeneous Gold Catalysis: Reactivity of Gold Acyl Species Generated through Water Addition to Gold Vinylidenes

December 13, 2014
Hot Paper: Screening for Protein Phosphorylation Using Nanoscale Reactions on Microdroplet Arrays

December 13, 2014
Hot Paper: High-Resolution Single-Molecule Fluorescence Imaging of Zeolite Aggregates within Real-Life Fluid Catalytic Cracking Particles

December 13, 2014
VIP: Total Synthesis of Albicidin: A Lead Structure from Xanthomonas albilineans for Potent Antibacterial Gyrase Inhibitors

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