Angewandte Chemie International Edition

Cover image for Vol. 56 Issue 5

January 24, 2017

Volume 56, Issue 5

Pages 1161–1421

  1. Cover Pictures

    1. Top of page
    2. Cover Pictures
    3. Frontispiece
    4. Editorials
    5. Graphical Abstract
    6. News
    7. Author Profiles
    8. News
    9. Reviews
    10. Communications
    1. You have free access to this content
      Cover Picture: Self-Templating Synthesis of Hollow Co3O4 Microtube Arrays for Highly Efficient Water Electrolysis (Angew. Chem. Int. Ed. 5/2017) (page 1161)

      Dr. Yun Pei Zhu, Dr. Tian Yi Ma, Prof. Mietek Jaroniec and Prof. Shi Zhang Qiao

      Version of Record online: 28 DEC 2016 | DOI: 10.1002/anie.201612285

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      An electrochemical self-templating strategy for the synthesis of hollow hierarchical Co3O4 microtube arrays with well-defined internal cavities and porous shells is described by S. Z. Qiao and co-workers in their Communication on page 1324 ff. These structural features facilitate mass transfer and lead to excellent electrocatalytic activity in oxygen and hydrogen evolution as well as in overall water splitting.

    2. You have free access to this content
      Inside Cover: Molecular Polygons Probe the Role of Intramolecular Strain in the Photophysics of π-Conjugated Chromophores (Angew. Chem. Int. Ed. 5/2017) (page 1162)

      Philipp Wilhelm, Dr. Jan Vogelsang, Georgiy Poluektov, Nina Schönfelder, Tristan J. Keller, Dr. Stefan-Sven Jester, Prof. Dr. Sigurd Höger and Prof. Dr. John M. Lupton

      Version of Record online: 4 JAN 2017 | DOI: 10.1002/anie.201612287

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      The π-system of conjugated macromolecules can be bent in a controlled fashion by incorporating chromophores in molecular polygon templates. This distortion is clearly seen in scanning-tunneling micrographs of the molecules. In their Communication on page 1234 ff. S. Höger, J. M. Lupton et al. show that bending leads to isotropic polarization in absorption and fluorescence but also affects the elementary photophysics. On the single-molecule level, a correlation emerges between luminescence spectrum and lifetime, which arises from subtle variations in the bending radius between molecules.

    3. You have free access to this content
      Inside Back Cover: Gas-Phase Formation of the Disilavinylidene (H2SiSi) Transient (Angew. Chem. Int. Ed. 5/2017) (page 1423)

      Dr. Tao Yang, Dr. Beni B. Dangi, Prof. Dr. Ralf I. Kaiser, Kang-Heng Chao, Dr. Bing-Jian Sun, Prof. Dr. Agnes H. H. Chang, Dr. Thanh Lam Nguyen and Prof. Dr. John F. Stanton

      Version of Record online: 4 JAN 2017 | DOI: 10.1002/anie.201612283

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      Mapped on the image of the reactive differential cross section, the hitherto elusive disilavinylidene molecule (H2SiSi) is found to be initially formed in the gas-phase reaction of ground-state atomic silicon (Si) with silane (SiH4) and in equilibrium with the mono-bridged (Si(H)SiH) and di-bridged (Si(H2)Si) isomers. As shown by R. I. Kaiser, A. H. H. Chang, J. F. Stanton et al. in their Communication on page 1264 ff., the dynamics are distinct from those of the isovalent carbon/methane system, and provide a rare glimpse of unusual silicon chemistry.

    4. You have free access to this content
      Back Cover: Glucose-Responsive Sequential Generation of Hydrogen Peroxide and Nitric Oxide for Synergistic Cancer Starving-Like/Gas Therapy (Angew. Chem. Int. Ed. 5/2017) (page 1424)

      Dr. Wenpei Fan, Nan Lu, Prof. Peng Huang, Dr. Yi Liu, Zhen Yang, Dr. Sheng Wang, Dr. Guocan Yu, Dr. Yijing Liu, Dr. Junkai Hu, Dr. Qianjun He, Prof. Junle Qu, Prof. Tianfu Wang and Prof. Xiaoyuan Chen

      Version of Record online: 12 JAN 2017 | DOI: 10.1002/anie.201612479

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      Efficient tumor eradication by endogenous synergistic cancer therapy has been developed by combining NO gas therapy with starvation of tumor cells. In their Communication on page 1229 ff., P. Huang, T. Wang, X. Chen et al. describe a biocompatible porous nanocapsule formula made of an organosilicate that transports glucose oxidase and l-arginine into tumor cells simultaneously. This glucose-responsive nanomedicine shows sequential generation of H2O2 and NO.

  2. Frontispiece

    1. Top of page
    2. Cover Pictures
    3. Frontispiece
    4. Editorials
    5. Graphical Abstract
    6. News
    7. Author Profiles
    8. News
    9. Reviews
    10. Communications
    1. You have free access to this content
      Frontispiece: Channeling Exciton Migration into Electron Transfer in Formamidinium Lead Bromide Perovskite Nanocrystal/Fullerene Composites

      Dr. Vijayakumar C. Nair, Chinnadurai Muthu, Prof. Andrey L. Rogach, Reiko Kohara and Prof. Vasudevanpillai Biju

      Version of Record online: 17 JAN 2017 | DOI: 10.1002/anie.201780561

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      Fluorescence Quenching In their Communication on page 1214, V. C. Nair, V. Biju et al. report on the trapping of migrating excitons in a perovskite thin film by doping with C60 molecules, leading to quantitative quenching of the nanocrystal fluorescence.

  3. Editorials

    1. Top of page
    2. Cover Pictures
    3. Frontispiece
    4. Editorials
    5. Graphical Abstract
    6. News
    7. Author Profiles
    8. News
    9. Reviews
    10. Communications
    1. You have free access to this content
      DNA-Encoded Compound Libraries as Open Source: A Powerful Pathway to New Drugs (pages 1164–1165)

      Prof. Richard A. Lerner and Prof. Dr. Sydney Brenner

      Version of Record online: 17 JAN 2017 | DOI: 10.1002/anie.201612143

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      “… We envisioned an iterative system where a unique DNA tag identifier that encoded the event was appended to each newly formed molecule. These vast collections of molecules are known today as DNA- encoded chemical libraries (DECLs), and allow scientists to do selections on the benchtop that previously required access to large and complex high-throughput screening centers …” Read more in the Guest Editorial by Richard A. Lerner and Sydney Brenner.

  4. Graphical Abstract

    1. Top of page
    2. Cover Pictures
    3. Frontispiece
    4. Editorials
    5. Graphical Abstract
    6. News
    7. Author Profiles
    8. News
    9. Reviews
    10. Communications
  5. News

    1. Top of page
    2. Cover Pictures
    3. Frontispiece
    4. Editorials
    5. Graphical Abstract
    6. News
    7. Author Profiles
    8. News
    9. Reviews
    10. Communications
  6. Author Profiles

    1. Top of page
    2. Cover Pictures
    3. Frontispiece
    4. Editorials
    5. Graphical Abstract
    6. News
    7. Author Profiles
    8. News
    9. Reviews
    10. Communications
    1. Rongchao Jin (page 1186)

      Version of Record online: 7 SEP 2016 | DOI: 10.1002/anie.201607781

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      “My favorite saying is ‘two heads are better than one’. I am waiting for the day when someone will discover human life forms on another planet ...” This and more about Rongchao Jin can be found on page 1186.

  7. News

    1. Top of page
    2. Cover Pictures
    3. Frontispiece
    4. Editorials
    5. Graphical Abstract
    6. News
    7. Author Profiles
    8. News
    9. Reviews
    10. Communications
  8. Reviews

    1. Top of page
    2. Cover Pictures
    3. Frontispiece
    4. Editorials
    5. Graphical Abstract
    6. News
    7. Author Profiles
    8. News
    9. Reviews
    10. Communications
    1. Solar Cells

      Stability of Perovskite Solar Cells: A Prospective on the Substitution of the A Cation and X Anion (pages 1190–1212)

      Ze Wang, Zejiao Shi, Taotao Li, Prof. Yonghua Chen and Prof. Wei Huang

      Version of Record online: 28 NOV 2016 | DOI: 10.1002/anie.201603694

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      Stability rising: The recent advances in improving the chemical stability of perovskite materials in terms of substitution of A-cation and X-anion are reviewed. The aim is to open new perspectives for the rational design of perovskite materials to create perovskite solar cells with unprecedented stability for outdoor applications.

  9. Communications

    1. Top of page
    2. Cover Pictures
    3. Frontispiece
    4. Editorials
    5. Graphical Abstract
    6. News
    7. Author Profiles
    8. News
    9. Reviews
    10. Communications
    1. Photophysics | Hot Paper

      Channeling Exciton Migration into Electron Transfer in Formamidinium Lead Bromide Perovskite Nanocrystal/Fullerene Composites (pages 1214–1218)

      Dr. Vijayakumar C. Nair, Chinnadurai Muthu, Prof. Andrey L. Rogach, Reiko Kohara and Prof. Vasudevanpillai Biju

      Version of Record online: 30 DEC 2016 | DOI: 10.1002/anie.201610070

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      Exciton migration among closely packed formamidinium lead bromide perovskite nanocrystals in thin films extends their fluorescence lifetime. By doping the film with C60 molecules, migrating excitons can be efficiently trapped, which quantitatively quenches the fluorescence of the nanocrystals.

    2. Prebiotic Chemistry

      Ribonucleotides and RNA Promote Peptide Chain Growth (pages 1219–1223)

      Dipl.-Chem. (FH) Helmut Griesser, Dr. Peter Tremmel, Dr. Eric Kervio, Camilla Pfeffer, Prof. Dr. Ulrich E. Steiner and Prof. Dr. Clemens Richert

      Version of Record online: 21 DEC 2016 | DOI: 10.1002/anie.201610650

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      Capture accelerates coupling: When amino acids condense with ribonucleotides, they form phosphoramidates, which show faster chain growth than free amino acids, facilitating the transition to a “peptide-RNA world”.

    3. Amino Acid-Specific, Ribonucleotide-Promoted Peptide Formation in the Absence of Enzymes (pages 1224–1228)

      Dipl.-Chem. (FH) Helmut Griesser, M.Sc. Maren Bechthold, Dr. Peter Tremmel, Dr. Eric Kervio and Prof. Dr. Clemens Richert

      Version of Record online: 21 DEC 2016 | DOI: 10.1002/anie.201610651

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      Specificity without enzymes: Ribonucleotide-promoted peptide formation strongly depends on the structure of the amino acid, as detected in a screen of all 20 of the proteinogenic amino acids and the four ribonucleotides, helping to explain how peptides could have formed in the “RNA world”.

    4. Drug Delivery | Very Important Paper

      Glucose-Responsive Sequential Generation of Hydrogen Peroxide and Nitric Oxide for Synergistic Cancer Starving-Like/Gas Therapy (pages 1229–1233)

      Dr. Wenpei Fan, Nan Lu, Prof. Peng Huang, Dr. Yi Liu, Zhen Yang, Dr. Sheng Wang, Dr. Guocan Yu, Dr. Yijing Liu, Dr. Junkai Hu, Dr. Qianjun He, Prof. Junle Qu, Prof. Tianfu Wang and Prof. Xiaoyuan Chen

      Version of Record online: 9 DEC 2016 | DOI: 10.1002/anie.201610682

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      Synergistic therapy: A biocompatible and biodegradable nanomedicine based on glucose oxidase/l-arginine co-loaded hollow mesoporous organosilica nanoparticles has been successfully constructed for converting intratumoral glucose into high concentrations of toxic hydrogen peroxide and nitric oxide. An endogenous synergistic cancer therapy for efficient tumor eradication has been developed.

    5. Chromophores

      Molecular Polygons Probe the Role of Intramolecular Strain in the Photophysics of π-Conjugated Chromophores (pages 1234–1238)

      Philipp Wilhelm, Dr. Jan Vogelsang, Georgiy Poluektov, Nina Schönfelder, Tristan J. Keller, Dr. Stefan-Sven Jester, Prof. Dr. Sigurd Höger and Prof. Dr. John M. Lupton

      Version of Record online: 12 JAN 2017 | DOI: 10.1002/anie.201610723

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      Bent π-systems: The π-system of conjugated macromolecules can be bent in a controlled fashion by incorporating chromophores in molecular polygon templates. Bending leads to isotropic polarization in absorption and fluorescence but also influences excited-state properties. On the single-molecule level, a correlation emerges between luminescence spectrum and lifetime, which arises from subtle variations in the bending radius of the molecules.

    6. Bioconjugation

      Effect of PEG Architecture on the Hybridization Thermodynamics and Protein Accessibility of PEGylated Oligonucleotides (pages 1239–1243)

      Fei Jia, Xueguang Lu, Xuyu Tan, Dali Wang, Xueyan Cao and Prof. Ke Zhang

      Version of Record online: 29 DEC 2016 | DOI: 10.1002/anie.201610753

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      Opposing effects: The hybridization thermodynamics and protein accessibility of a series of PEG–DNA conjugates were compared. The DNA was found to experience two effects from the PEG component: an excluded volume effect and a chemical interaction effect, which work in opposite directions on duplex stability and are polymer-architecture-dependent.

    7. Cage Compounds

      Chiral Self-Sorting of [2+3] Salicylimine Cage Compounds (pages 1244–1248)

      Dr. Daniel Beaudoin, Dr. Frank Rominger and Prof. Dr. Michael Mastalerz

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/anie.201610782

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      Sorted out: An inherently chiral C3-symmetric triaminotribenzotriquinacene was condensed in racemic and enantiomerically pure form with a bis(salicylaldehyde) to form [2+3] salicylimine cage compounds. Investigations revealed that entropy favors narcissistic self-sorting in solution, and selective social self-sorting can be achieved by exploiting the difference in solubility between the homochiral and heterochiral cages.

    8. Synthetic Methods

      Chemoselective Suzuki–Miyaura Cross-Coupling via Kinetic Transmetallation (pages 1249–1253)

      James W. B. Fyfe, Dr. Neal J. Fazakerley and Dr. Allan J. B. Watson

      Version of Record online: 16 DEC 2016 | DOI: 10.1002/anie.201610797

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      Set phases to stun: Chemoselective Suzuki–Miyaura cross-coupling can be achieved by kinetic discrimination of boronic acids and BPin esters during transmetallation. Simultaneous electrophile control allows sequential chemoselective cross-couplings in a single operation in the absence of protecting groups.

    9. RNA–Protein Interactions

      You have full text access to this OnlineOpen article
      Native Top-Down Mass Spectrometry of TAR RNA in Complexes with a Wild-Type tat Peptide for Binding Site Mapping (pages 1254–1258)

      Eva-Maria Schneeberger and Priv.-Doz. Dr. Kathrin Breuker

      Version of Record online: 21 DEC 2016 | DOI: 10.1002/anie.201610836

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      Right on TARget: Native top-down MS provides time-resolved information on TAR–tat complex stoichiometry and reveals tat binding sites at the single-residue level of TAR RNA.

    10. Liquid Crystals

      Not Only Columns: High Hole Mobility in a Discotic Nematic Mesophase Formed by Metal-Containing Porphyrin-Core Dendrimers (pages 1259–1263)

      Alberto Concellón, Dr. Mercedes Marcos, Dr. Pilar Romero, Prof. José Luis Serrano, Dr. Roberto Termine and Dr. Attilio Golemme

      Version of Record online: 28 DEC 2016 | DOI: 10.1002/anie.201611017

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      Hole-ier than thou: A new class of nematic discotic porphyrin-core dendrimers that have coumarin functional units around the porphyrin core is reported. Such dendrimers exhibit nematic discotic phases with a high degree of macroscopic orientational order and, if the porphyrins are metalated, hole mobilities values typical of more ordered columnar phases are obtained.

    11. Silicon Chemistry

      Gas-Phase Formation of the Disilavinylidene (H2SiSi) Transient (pages 1264–1268)

      Dr. Tao Yang, Dr. Beni B. Dangi, Prof. Dr. Ralf I. Kaiser, Kang-Heng Chao, Dr. Bing-Jian Sun, Prof. Dr. Agnes H. H. Chang, Dr. Thanh Lam Nguyen and Prof. Dr. John F. Stanton

      Version of Record online: 2 JAN 2017 | DOI: 10.1002/anie.201611107

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      Si/C isoelectronicity: The gas-phase bimolecular reaction of the ground-state silicon with silane (SiH4) under single-collision conditions provides a rare glimpse at previously disregarded silicon chemistry on the molecular level, which further develops our understanding of the concept of isoelectronicity proposed about a century ago.

    12. Membrane Proteins

      Dipolar Relaxation Dynamics at the Active Site of an ATPase Regulated by Membrane Lateral Pressure (pages 1269–1272)

      Elisabeth Fischermeier, Petr Pospíšil, Ahmed Sayed, Martin Hof, Marc Solioz and Karim Fahmy

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/anie.201611582

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      Using the Legionella pneumophila P1B-type ATPase transmembrane architecture, site-specific labeling of native internal cysteines with a polarity-sensitive fluorophore was established. This enabled dipolar relaxation studies in a solubilized form of the protein and in its lipid-embedded state in nanodiscs. Time-dependent fluorescence shifts revealed site-specific hydration and dipole mobility around the conserved ion-binding motif.

    13. Antibodies

      Three-Dimensional Ordered Antibody Arrays Through Self-Assembly of Antibody–Polymer Conjugates (pages 1273–1277)

      Dr. Xue-Hui Dong, Dr. Allie C. Obermeyer and Prof. Dr. Bradley D. Olsen

      Version of Record online: 28 DEC 2016 | DOI: 10.1002/anie.201607085

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      New IgGs on the block: Three-dimensional long-range ordered arrays of antibodies were fabricated using well-defined full-length antibody–polymer conjugates. The assembly is based on the principles of block copolymer self-assembly.

    14. p53 Rescue Motif

      The Mechanism of p53 Rescue by SUSP4 (pages 1278–1282)

      Do-Hyoung Kim, Dr. Chewook Lee, Dr. Si-Hyung Lee, Prof. Kyung-Tae Kim, Joan J. Han, Eun-Ji Cha, Ji-Eun Lim, Ye-Jin Cho, Prof. Seung-Hee Hong and Dr. Kyou-Hoon Han

      Version of Record online: 21 DEC 2016 | DOI: 10.1002/anie.201607819

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      To the rescue! A 29-residue p53 rescue motif in SUSP4 contains an N-terminal transient helix acting as an affinity modulator to mdm2, a hydrophobic linker that inserts into a novel hydrophobic crevice near the p53-binding pocket of mdm2, and a C-terminal transient helix that binds to the well-known p53-binding pocket in mdm2(3–109).

    15. Interband Transition

      Interband Absorption Enhanced Optical Activity in Discrete Au@Ag Core–Shell Nanocuboids: Probing Extended Helical Conformation of Chemisorbed Cysteine Molecules (pages 1283–1288)

      Zhi Yong Bao, Prof. Wei Zhang, Dr. Yong-Liang Zhang, Jijun He, Prof. Jiyan Dai, Dr. Chi-Tung Yeung, Dr. Ga-Lai Law and Dr. Dang Yuan Lei

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/anie.201607563

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      Plasmonic reporter: Discrete Au@Ag core–shell nanocuboids capped with cysteine molecules exhibit two bisignate circular dichroism (CD) resonances in the UV region. One corresponds to the molecular electronic CD of cysteine, the other is an induced, unusual CD band originating from the formation of extended helical networks among neighboring cysteine molecules, which is dramatically amplified by the interband absorption of Ag.

    16. Multicomponent Reactions

      A Four-Component Reaction Strategy for Pyrimidine Carboxamide Synthesis (pages 1289–1293)

      Dr. Wei Guo, Jianhua Liao, Dongqing Liu, Jiawei Li, Fanghua Ji, Prof. Dr. Wanqing Wu and Prof. Dr. Huanfeng Jiang

      Version of Record online: 14 DEC 2016 | DOI: 10.1002/anie.201608433

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      Three to four to one: A palladium-catalyzed oxidative 3 starting materials–4 component reaction (3SM-4CR) strategy for the synthesis of pyrimidine carboxamides from amidines, styrene, and DMF. DMF serves as a dual synthon, a one-carbon-atom synthon and amide synthon. This is a fascinating protocol for the preparation of pyrimidine carboxamides and has potential applications in the pharmaceutical industry.

    17. Inhibitors

      Azaindoles as Zinc-Binding Small-Molecule Inhibitors of the JAMM Protease CSN5 (pages 1294–1297)

      Dr. Eva Altmann, Dr. Paul Erbel, Dr. Martin Renatus, Dr. Michael Schaefer, Dr. Anita Schlierf, Adelaide Druet, Laurence Kieffer, Mickael Sorge, Keith Pfister, Dr. Ulrich Hassiepen, Matthew Jones, Dr. Simon Ruedisser, Daniela Ostermeier, Dr. Bruno Martoglio, Dr. Anne B. Jefferson and Dr. Jean Quancard

      Version of Record online: 16 DEC 2016 | DOI: 10.1002/anie.201608672

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      CSN5 is the zinc metalloprotease subunit of the COP9 signalosome, which is an important regulator of cullin-RING E3 ubiquitin ligases. A new class of CSN5 inhibitors (orange) was discovered and shown to interact with the active-site zinc ion in an unprecedented binding mode. Optimized nanomolar CSN5 inhibitors result in decreased levels of the oncoprotein Skp2 and reduce the viability of HCT116 cells.

    18. Synthetic Methods

      Regioselective One-Pot Synthesis of Triptycenes via Triple-Cycloadditions of Arynes to Ynolates (pages 1298–1302)

      Satoshi Umezu, Gabriel dos Passos Gomes, Tatsuro Yoshinaga, Mikei Sakae, Dr. Kenji Matsumoto, Dr. Takayuki Iwata, Prof. Dr. Igor Alabugin and Prof. Dr. Mitsuru Shindo

      Version of Record online: 28 DEC 2016 | DOI: 10.1002/anie.201609111

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      Three alkynes and one triple bond: The title reaction constitutes a four-step process involving three cycloadditions and electrocyclic ring opening of the strained Dewar anthracene. Each of the three related but structurally distinct classes of nucleophiles (ynolate, enolate, and anthracenolate) reacts with o-benzyne in the same predictable manner controlled by chelation and negative hyperconjugation.

    19. Modified RNA

      Polymerase-Mediated Site-Specific Incorporation of a Synthetic Fluorescent Isomorphic G Surrogate into RNA (pages 1303–1307)

      Yao Li, Dr. Andrea Fin, Dr. Lisa McCoy and Prof. Yitzhak Tor

      Version of Record online: 21 DEC 2016 | DOI: 10.1002/anie.201609327

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      An enzyme-mediated approach is used for the assembly of singly modified RNA constructs in which specific G residues are replaced with thG, an emissive isomorphic G surrogate. By strategic modifications, a mechanistic insight into the ribozyme-mediated cleavage is gained. Emissive features of the modified nucleoside and responsiveness to environmental changes are used to monitor cleavage in real time by steady-state fluorescence spectroscopy.

    20. Self-Assembly

      Water-Rich Fluid Material Containing Orderly Condensed Proteins (pages 1308–1312)

      Dr. Tatsuya Nojima and Prof. Dr. Tomokazu Iyoda

      Version of Record online: 19 DEC 2016 | DOI: 10.1002/anie.201609974

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      Fluid protein–surfactant complex: A water-rich but water-segregated fluid material containing densely packed native proteins is instantly formed by simple mixing of a protein solution with a solution containing specific amounts of both anionic and cationic surfactants.

    21. Bonding Models

      Chemical Bonding Analysis as a Guide for the Preparation of New Compounds: The Case of VIrGe and HfPtGe (pages 1313–1318)

      Dr. David Bende, Dr. Frank R. Wagner, Dr. Olga Sichevych and Prof. Yuri Grin

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/anie.201610029

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      Chemical bonding models are powerful tools for the systematic preparation of new compounds. In this contribution, quantum-chemical calculations in position space reveal important trends of chemical bonding that have led to the discovery of two MgAgAs-type (half-Heusler) compounds: high-temperature VIrGe and low-temperature HfPtGe.

    22. Drug Delivery

      A Redox-Activatable Fluorescent Sensor for the High-Throughput Quantification of Cytosolic Delivery of Macromolecules (pages 1319–1323)

      Dr. Zhaohui Wang, Dr. Min Luo, Dr. Chengqiong Mao, Dr. Qi Wei, Dr. Tian Zhao, Yang Li, Dr. Gang Huang and Prof. Jinming Gao

      Version of Record online: 16 DEC 2016 | DOI: 10.1002/anie.201610302

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      A quantitative redox-activatable sensor (qRAS) for real-time monitoring of cytosolic delivery of macromolecules was developed. The qRAS probe made possible a high-throughput screening of polymers toward efficient cytosolic delivery of macromolecules on a plate reader. This new sensor will accelerate the development of macromolecular therapeutics for various diseases.

    23. Electrocatalysis | Very Important Paper

      Self-Templating Synthesis of Hollow Co3O4 Microtube Arrays for Highly Efficient Water Electrolysis (pages 1324–1328)

      Dr. Yun Pei Zhu, Dr. Tian Yi Ma, Prof. Mietek Jaroniec and Prof. Shi Zhang Qiao

      Version of Record online: 30 NOV 2016 | DOI: 10.1002/anie.201610413

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      Hollow and hierarchical: An electrochemical self-templating strategy was developed for the fabrication of hollow Co3O4 microtube arrays with hierarchical porosity. The resultant structures showed excellent electrocatalytic activity and durability towards oxygen and hydrogen evolution and are thus capable of catalyzing full water splitting.

    24. Supramolecular Chemistry | Hot Paper

      Transient Helicity: Fuel-Driven Temporal Control over Conformational Switching in a Supramolecular Polymer (pages 1329–1333)

      Shikha Dhiman, Ankit Jain and Prof. Subi J. George

      Version of Record online: 29 DEC 2016 | DOI: 10.1002/anie.201610946

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      A bio-inspired synthetic supramolecular system is reported that undergoes changes in its helical conformation transiently as an active material and at the expense of ATP molecules as fuel in an “enzyme-in-tandem” approach.

    25. Imaging Agents

      You have full text access to this OnlineOpen article
      Mechanism-Based Fluorogenic trans-Cyclooctene–Tetrazine Cycloaddition (pages 1334–1337)

      Dr. Arcadio Vázquez, Dr. Rastislav Dzijak, Dr. Martin Dračínský, MSc. Robert Rampmaier, MSc. Sebastian J. Siegl and Dr. Milan Vrabel

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/anie.201610491

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      Click-in color: A conceptually new approach enables the formation of fluorescent 1,4-dihydropyridazine products upon reaction of various 1,2,4,5-tetrazines with particular trans-cyclooctene isomers. The chemistry was applied for rapid fluorogenic labeling of subcellular compartments in live cells.

    26. Radical Fragmentation

      Radical Desulfur-Fragmentation and Reconstruction of Enol Triflates: Facile Access to α-Trifluoromethyl Ketones (pages 1338–1341)

      Xiaolong Su, Honggui Huang, Prof. Dr. Yaofeng Yuan and Prof. Dr. Yi Li

      Version of Record online: 21 DEC 2016 | DOI: 10.1002/anie.201608507

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      Reconstruction business: Oxidative fragmentation and reconstruction of enol triflates is a new strategy for the synthesis of α-CF3 ketones. Preliminary mechanistic studies indicated oxidative fragmentation to release a CF3 radical from the triflyl group of the enol triflate and subsequent addition of the CF3 radical to another enol triflate forms the desired α-CF3 ketone.

    27. Trifluoromethylation

      Synthesis of α-Trifluoromethylated Ketones from Vinyl Triflates in the Absence of External Trifluoromethyl Sources (pages 1342–1345)

      Dr. Takuji Kawamoto, Rio Sasaki and Prof. Dr. Akio Kamimura

      Version of Record online: 3 NOV 2016 | DOI: 10.1002/anie.201608591

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      Sure BEt3: A BEt3-induced conversion of vinyl triflates into α-trifluoromethylated ketones is reported. The reaction proceeds by the addition of a trifluoromethyl radical to the vinyl triflate and subsequent fragmentation of a trifluoromethane sulfonyl radical. This reaction was used to develop an efficient one-pot two-step procedure for the trifluoromethylation of ketones.

    28. Sandwich Complexes

      Substrate Binding by a Parallel Metal Sheet Sandwich Complex: A Unique Role of an Additional Metal Atom (pages 1346–1350)

      Yuki Ishikawa, Dr. Koji Yamamoto and Prof. Tetsuro Murahashi

      Version of Record online: 21 DEC 2016 | DOI: 10.1002/anie.201610784

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      Clean sheet: A unique metal addition to the edge of a triangular Pd3 sandwich cluster is reported. While the edge coordination sites of a parallel Pd3 sandwich complex is narrow because of two sterically encumbering π-ligands, association of an additional metal atom at the edge site gives a wider coordination site. The binding of cyclopentadienyl by a Pd3 sandwich cluster is facilitated by an additional metal atom.

    29. Asymmetric Synthesis

      Rhodium(I)-Catalyzed Intermolecular Aza-[4+3] Cycloaddition of Vinyl Aziridines and Dienes: Atom-Economical Synthesis of Enantiomerically Enriched Functionalized Azepines (pages 1351–1355)

      Chao-Ze Zhu, Dr. Jian-Jun Feng and Prof. Dr. Junliang Zhang

      Version of Record online: 14 DEC 2016 | DOI: 10.1002/anie.201609608

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      Strike a happy medium: The title reaction, in which the vinyl aziridine acts as an aza-three-atom component, provided highly functionalized azepines in an enantioselective manner with net inversion of configuration (see scheme; Si is a silyl protecting group). This strategy features the use of readily available substrates, high selectivity, mild reaction conditions, ease of scale-up, and versatile functionalization of the products.

    30. Phosphorus Heterocycles | Hot Paper

      2,4,6-Tri(hydroxy)-1,3,5-triphosphinine, P3C3(OH)3: The Phosphorus Analogue of Cyanuric Acid (pages 1356–1360)

      Riccardo Suter, Yanbo Mei, Matthew Baker, Dr. Zoltan Benkő, Dr. Zhongshu Li and Prof. Dr. Hansjörg Grützmacher

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/anie.201610156

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      Done in three ticks: The trimerization of boryl-substituted phosphaalkynes allows the straightforward synthesis of triphosphabenzenes on a multi-gram scale. These compounds give stable metal complexes and can be further functionalized at the oxygen centers.

    31. Polycyclic Aromatic Hydrocarbons | Hot Paper

      One-Step Annulative π-Extension of Alkynes with Dibenzosiloles or Dibenzogermoles by Palladium/o-chloranil Catalysis (pages 1361–1364)

      Dr. Kyohei Ozaki, Keiichiro Murai, Wataru Matsuoka, Dr. Katsuaki Kawasumi, Dr. Hideto Ito and Prof. Dr. Kenichiro Itami

      Version of Record online: 21 DEC 2016 | DOI: 10.1002/anie.201610374

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      Extending circumstances: An efficient one-step annulative π-extension reaction of alkynes provides facile access to diarylphenanthrenes and related nanographene precursors. In the presence of a cationic palladium/o-chloranil catalyst system, a variety of diarylacetylenes are transformed through the use of dibenzosiloles or dibenzogermoles as π-extending agents into 9,10-diarylphenanthrenes with good functional-group tolerance.

    32. Main-Group Chemistry

      N,P-Heterocyclic Germylene/B(C6F5)3 Adducts: A Lewis Pair with Multi-reactive Sites (pages 1365–1370)

      Natalia Del Rio, Dr. Morelia Lopez-Reyes, Dr. Antoine Baceiredo, Dr. Nathalie Saffon-Merceron, Dr. Dennis Lutters, Prof. Dr. Thomas Müller and Dr. Tsuyoshi Kato

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/anie.201610455

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      Multitasking: An N,P-heterocyclic germylene/B(C6F5)3 Lewis adduct presents multi-reactive sites (Lewis pair, germylene, Ge=P π-bond). In contrast to simple frustrated Lewis pairs or divalent Group 14 element species, the germylene adduct is able to activate two small molecules simultaneously. This unique property was successfully applied to selective and metal-free catalytic CO2 hydrosilylation to H2C(OSiEt3)2.

    33. Asymmetric Catalysis

      Rhodium-Catalyzed Asymmetric Synthesis of β-Branched Amides (pages 1371–1375)

      Zhao Wu, Summer D. Laffoon, Trang T. Nguyen, Jacob D. McAlpin and Prof. Dr. Kami L. Hull

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/anie.201610500

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      A domino process: A RhI/chiral BINAP catalysis is reported for the one-step modular synthesis of chiral β-branched amides with various amine nucleophiles. β-dialkyl, β-diaryl, and β-alkylaryl stereocenters are established under identical conditions with excellent enantio- and diastereoselectivity in a ligand-controlled manner.

    34. Cyclotrimerization

      Selective Metal-free HB(C6F5)2 Catalyzed Allene Cyclotrimerization: Formation of 1,3,5-Trimethylenecyclohexane and Its Tris-hydroboration Product (pages 1376–1380)

      Dr. Xin Tao, Dr. Gerald Kehr, Dr. Constantin G. Daniliuc and Prof. Gerhard Erker

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/anie.201610530

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      Triskelions with borane: Allene is cyclotrimerized under metal-free conditions by the HB(C6F5)2 borane catalyst to selectively give 1,3,5-trimethylenecyclohexane. Three-fold hydroboration of the 1,3,5-cyclotrimer with Piers’ borane gives the all-cis 1,3,5-CH2B(C6F5)2 substituted cyclohexane product (see scheme).

    35. C−H Activation

      Combination of Cp*RhIII-Catalyzed C−H Activation and a Wagner–Meerwein-Type Rearrangement (pages 1381–1384)

      Dr. Xiaoming Wang, Andreas Lerchen, Tobias Gensch, Tobias Knecht, Dr. Constantin G. Daniliuc and Prof. Frank Glorius

      Version of Record online: 21 DEC 2016 | DOI: 10.1002/anie.201610117

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      Nicely (re)arranged: A combination of Cp*RhIII-catalyzed C−H activation and Wagner–Meerwein-type rearrangement was successfully achieved for the first time. Thus, bridged polycyclic molecules that are not readily accessible by other means were accessed under mild conditions with high efficiency (as low as 0.5 mol % Rh catalyst) in the coupling of N-phenoxyacetamide with 7-azabenzonorbornadiene.

    36. DNA Damage

      Elucidation of the Dexter-Type Energy Transfer in DNA by Thymine–Thymine Dimer Formation Using Photosensitizers as Artificial Nucleosides (pages 1385–1389)

      MSc. Linda Antusch, Dr. Nadine Gaß and Prof. Dr. Hans-Achim Wagenknecht

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/anie.201610065

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      How far can it go? Internal photosensitizers induce triplet energy transfer over a distance of up to 37.4 Å to generate thymine dimers. The weak exponential distance dependence for dimer formation is in agreement with a Dexter-type triplet–triplet energy transfer mechanism.

    37. Asymmetric Synthesis

      Catalytic Enantioselective and Diastereoselective Allylic Alkylation with Fluoroenolates: Efficient Access to C3-Fluorinated and All-Carbon Quaternary Oxindoles (pages 1390–1395)

      Dr. Kaluvu Balaraman and Prof. Dr. Christian Wolf

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/anie.201608752

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      3,3-Disubstituted fluorooxindoles with vicinal chiral centers were obtained in high yields and with excellent enantio-, diastereo-, and regioselectivity through catalytic asymmetric fluoroenolate alkylation with allylic acetates. The synthetic usefulness of the products is demonstrated by the incorporation of additional functionalities and the formation of 3-fluorinated oxindoles exhibiting an array of four adjacent chiral centers.

    38. Photoaffinity Labeling

      A Whole Proteome Inventory of Background Photocrosslinker Binding (pages 1396–1401)

      M. Sc. Philipp Kleiner, Dr. Wolfgang Heydenreuter, M. Sc. Matthias Stahl, Dr. Vadim S. Korotkov and Prof. Dr. Stephan A. Sieber

      Version of Record online: 16 DEC 2016 | DOI: 10.1002/anie.201605993

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      In affinity-based protein profiling, small molecules are equipped with a photocrosslinker for irreversible binding to a protein target. The background protein labeling observed with such photocrosslinkers was analyzed by gel-free quantitative proteomics, and characteristic off-targets were identified for each photoreactive group. This is of importance for the reliable identification of biologically relevant binders in photoprobe experiments.

    39. Cascade Reactions

      A Photoredox-Induced Stereoselective Dearomative Radical (4+2)-Cyclization/1,4-Addition Cascade for the Synthesis of Highly Functionalized Hexahydro-1H-carbazoles (pages 1402–1406)

      Dirk Alpers, Malte Gallhof, Julian Witt, Dr. Frank Hoffmann and Prof. Dr. Malte Brasholz

      Version of Record online: 9 JAN 2017 | DOI: 10.1002/anie.201610974

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      One photon, four bonds: A photoredox-induced dearomative radical (4+2)-cyclization/1,4-addition cascade with 3-(2-iodoethyl)indoles and acceptor-substituted alkenes enables the synthesis of highly substituted hexahydro-1H-carbazoles. This method involves the simultaneous formation of four bonds and three contiguous stereocenters with high stereoselectivity. PC=photocatalyst.

    40. Metal Oxide Nanoparticles

      Hydroxylation Induced Alignment of Metal Oxide Nanocubes (pages 1407–1410)

      MSc. Daniel Thomele, Dr. Gilles R. Bourret, Prof. Dr. Johannes Bernardi, Prof. Dr. Michel Bockstedte and Prof. Dr. Oliver Diwald

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/anie.201608538

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      Water power: With the help of water vapor, MgO nanocubes can be reorganized into regular staggered one-dimensional stacks. This transformation involves an initial alignment of MgO cubes, the formation of intermediate elongated Mg(OH)2 structures, and their reconversion into MgO cubes which are arranged in staggered structures.

    41. Strong Acids

      1,1,3,3-Tetratriflylpropene (TTP): A Strong, Allylic C–H Acid for Brønsted and Lewis Acid Catalysis (pages 1411–1415)

      Denis Höfler, Dr. Manuel van Gemmeren, Petra Wedemann, Dr. Karl Kaupmees, Prof. Dr. Ivo Leito, Dr. Markus Leutzsch, Julia B. Lingnau and Prof. Dr. Benjamin List

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/anie.201609923

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      Acid strength by design: Tetratrifylpropene (TTP) has been developed as a highly acidic, allylic C–H acid for Brønsted and Lewis acid catalysis and was tested in Mukaiyama aldol, Hosomi–Sakurai, and Friedel–Crafts acylation reactions. X-ray analyses, NMR experiments, acidity measurements, and theoretical studies provide further insights to rationalize the remarkable reactivity of TTP.

    42. Polymer Glycomimetics

      Polymeric Selectin Ligands Mimicking Complex Carbohydrates: From Selectin Binders to Modifiers of Macrophage Migration (pages 1416–1421)

      Dr. Kai E. Moog, Dr. Matthias Barz, Dr. Matthias Bartneck, Dr. Figen Beceren-Braun, Dr. Nicole Mohr, Dr. Zhuojun Wu, Lydia Braun, Dr. Jens Dernedde, Dr. Elisa A. Liehn, Prof. Dr. Frank Tacke, Prof. Dr. Twan Lammers, Prof. Dr. Horst Kunz and Prof. Dr. Rudolf Zentel

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/anie.201610395

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      Complex carbohydrates like sialyl-LewisX (SLeX) play a role in cell–cell recognition and inflammatory processes. A biocompatible polymer that presents SLeX multivalently was compared with corresponding polymeric glycomimetics. For one of the mimetics the selectin binding affinity is similar to that of the SLeX–polymer system. It inhibits macrophage migration and offers new perspectives for therapy of severe inflammatory diseases.

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