Angewandte Chemie International Edition

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Frontispiece: A 3.3 Å‐Resolution Structure of Hyperthermophilic Respiratory Complex III Reveals the Mechanism of Its Thermal Stability

Guoliang Zhu, Hui Zeng, Shuangbo Zhang, Jana Juli, more

Angewandte Chemie International Edition > 59 > 1 > n/a - n/a

Protein Structures The hyperstability of respiratory complex III from Aquifex aeolicus allows an internal electron transfer reaction to occur at high temperature, as shown by Y. Zhu, G. H. Peng, H. Michel, F. Sun et al. in their Research Article on page 343.

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Water‐Soluble Polymeric Carbon Nitride Colloidal Nanoparticles for Highly Selective Quasi‐Homogeneous Photocatalysis

Igor Krivtsov, Dariusz Mitoraj, Christiane Adler, Marina Ilkaeva, more

Angewandte Chemie International Edition > 59 > 1 > 487 - 495

Heptazine‐based polymeric carbon nitrides (PCN) are promising photocatalysts for light‐driven redox transformations. However, their activity is hampered by low surface area resulting in low concentration of accessible active sites. Herein, we report a bottom‐up preparation of PCN nanoparticles with a narrow size distribution (ca. 10±3 nm), which are fully soluble in water showing no gelation or precipitation...

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New Members of the Editorial Board and International Advisory Board

Angewandte Chemie International Edition > 59 > 1 > 31 - 31

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Cascade Cross‐Coupling of Dienes: Photoredox and Nickel Dual Catalysis

Long Huang, Chen Zhu, Liang Yi, Huifeng Yue, more

Angewandte Chemie International Edition > 59 > 1 > 457 - 464

Chemical transformations based on cascade reactions have the potential to simplify the preparation of diverse and architecturally complex molecules dramatically. Herein, we disclose an unprecedented and efficient method for the cross‐coupling of radical precursors, dienes, and electrophilic coupling partners via a photoredox‐ and nickel‐enabled cascade cross‐coupling process. The cascade reaction...

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Engineered C–N Lyase: Enantioselective Synthesis of Chiral Synthons for Artificial Dipeptide Sweeteners

Jielin Zhang, Eleonora Grandi, Haigen Fu, Thangavelu Saravanan, more

Angewandte Chemie International Edition > 59 > 1 > 429 - 435

Aspartic acid derivatives with branched N‐alkyl or N‐arylalkyl substituents are valuable precursors to artificial dipeptide sweeteners such as neotame and advantame. The development of a biocatalyst to synthesize these compounds in a single asymmetric step is an as yet unmet challenge. Reported here is an enantioselective biocatalytic synthesis of various difficult N‐substituted aspartic acids, including...

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Unpaired 3d Electrons on Atomically Dispersed Cobalt Centres in Coordination Polymers Regulate both Oxygen Reduction Reaction (ORR) Activity and Selectivity for Use in Zinc–Air Batteries

Yuebin Lian, Wenjuan Yang, Chufeng Zhang, Hao Sun, more

Angewandte Chemie International Edition > 59 > 1 > 286 - 294

Reversible oxygen conversion is important for various green energy technologies. Herein we synthesize a series of bimetallic coordination polymers by varying the Ni/Co ratio and using HITP (HITP=2,3,6,7,10,11‐hexaiminotriphenylene) as the ligand, to interrogate the role of metal centres in modulating the activity of the oxygen reduction reaction (ORR). Co₃HITP₂ and Ni₃HITP₂ are compared. Unpaired...

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Cellulose Nanocrystal Elastomers with Reversible Visible Color

Charlotte E. Boott, Andy Tran, Wadood Y. Hamad, Mark J. MacLachlan

Angewandte Chemie International Edition > 59 > 1 > 226 - 231

Responsive photonic crystals have potential applications in mechanical sensors and soft displays; however, new materials are constantly desired to provide new innovations and improve on existing technologies. To address this, we report stretchable chiral nematic cellulose nanocrystal (CNC) elastomer composites that exhibit reversible visible color upon the application of mechanical stress. When stretched...

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Topochemical Synthesis of Two‐Dimensional Transition‐Metal Phosphides Using Phosphorene Templates

Sheng Yang, Guangbo Chen, Antonio Gaetano Ricciardulli, Panpan Zhang, more

Angewandte Chemie International Edition > 59 > 1 > 465 - 470

Transition‐metal phosphides (TMPs) have emerged as a fascinating class of narrow‐gap semiconductors and electrocatalysts. However, they are intrinsic nonlayered materials that cannot be delaminated into two‐dimensional (2D) sheets. Here, we demonstrate a general bottom‐up topochemical strategy to synthesize a series of 2D TMPs (e.g. Co₂P, Ni₁₂P₅, and Co_xFe_2−xP) by using phosphorene sheets as the phosphorus...

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Photoredox Catalytic α‐Alkoxypentafluorosulfanylation of α‐Methyl‐ and α‐Phenylstyrene Using SF₆

David Rombach, Hans‐Achim Wagenknecht

Angewandte Chemie International Edition > 59 > 1 > 300 - 303

SF₆ was applied as pentafluorosulfanylation reagent to prepare ethers with a vicinal SF₅ substituent through a one‐step method involving photoredox catalysis. This method shows a broad substrate scope with respect to applicable alcohols for the conversion of α‐methyl and α‐phenyl styrenes. The products bear a new structural motif with two functional groups installed in one step. The alkoxy group allows...

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Hydrazide‐Catalyzed Polyene Cyclization: Asymmetric Organocatalytic Synthesis of cis‐Decalins

Samuel J. Plamondon, Josephine M. Warnica, Dainis Kaldre, James L. Gleason

Angewandte Chemie International Edition > 59 > 1 > 253 - 258

Polyene cyclizations offer rapid entry into terpenoid ring systems. Although enantioselective cyclizations of (E)‐polyenes to form trans‐decalin ring systems are well precedented, highly enantioselective cyclizations of (Z)‐polyenes to form the corresponding cis‐decalins have not been reported. Here, we describe the first application of iminium catalysis to the initiation of polyene cyclizations....

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Inverting External Asymmetric Induction via Selective Energy Transfer Catalysis: A Strategy to β‐Chiral Phosphonate Antipodes

Carina Onneken, Kathrin Bussmann, Ryan Gilmour

Angewandte Chemie International Edition > 59 > 1 > 330 - 334

Enantiodivergent, catalytic reduction of activated alkenes relays stereochemical information encoded in the antipodal chiral catalysts to the pro‐chiral substrate. Although powerful, the strategy remains vulnerable to costs and availability of sourcing both catalyst enantiomers. Herein, a stereodivergent hydrogenation of α,β‐unsaturated phosphonates is disclosed using a single enantiomer of the catalyst...

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Characterization of Radical SAM Adenosylhopane Synthase, HpnH, which Catalyzes the 5′‐Deoxyadenosyl Radical Addition to Diploptene in the Biosynthesis of C₃₅ Bacteriohopanepolyols

Shusuke Sato, Fumitaka Kudo, Michel Rohmer, Tadashi Eguchi

Angewandte Chemie International Edition > 59 > 1 > 237 - 241

Adenosylhopane is a crucial intermediate in the biosynthesis of bacteriohopanepolyols, which are widespread prokaryotic membrane lipids. Herein, it is demonstrated that reconstituted HpnH, a putative radical S‐adenosyl‐l‐methionine (SAM) enzyme, commonly encoded in the hopanoid biosynthetic gene cluster, converts diploptene into adenosylhopane in the presence of SAM, flavodoxin, flavodoxin reductase,...

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Highly Selective Production of Ethylene by the Electroreduction of Carbon Monoxide

Ruixue Chen, Hai‐Yan Su, Deyu Liu, Rui Huang, more

Angewandte Chemie International Edition > 59 > 1 > 154 - 160

Conversion of carbon monoxide to high value‐added ethylene with high selectivity by traditional syngas conversion process is challenging because of the limitation of Anderson‐Schulz–Flory distribution. Herein we report a direct electrocatalytic process for highly selective ethylene production from CO reduction with water over Cu catalysts at room temperature and ambient pressure. An unprecedented...

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Stereoselective Csp³−Csp² Cross‐Couplings of Chiral Secondary Alkylzinc Reagents with Alkenyl and Aryl Halides

Juri Skotnitzki, Alexander Kremsmair, Daniel Keefer, Ye Gong, more

Angewandte Chemie International Edition > 59 > 1 > 320 - 324

We report palladium‐catalyzed cross‐coupling reactions of chiral secondary non‐stabilized dialkylzinc reagents, prepared from readily available chiral secondary alkyl iodides, with alkenyl and aryl halides. This method provides α‐chiral alkenes and arenes with very high retention of configuration (dr up to 98:2) and satisfactory overall yields (up to 76 % for 3 reaction steps). The configurational...

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Hot Branching Dynamics in a Light‐Harvesting Iron Carbene Complex Revealed by Ultrafast X‐ray Emission Spectroscopy

Hideyuki Tatsuno, Kasper S. Kjær, Kristjan Kunnus, Tobias C. B. Harlang, more

Angewandte Chemie International Edition > 59 > 1 > 364 - 372

Iron N‐heterocyclic carbene (NHC) complexes have received a great deal of attention recently because of their growing potential as light sensitizers or photocatalysts. We present a sub‐ps X‐ray spectroscopy study of an Fe^IINHC complex that identifies and quantifies the states involved in the deactivation cascade after light absorption. Excited molecules relax back to the ground state along two pathways:...

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New Designs for Phototherapeutic Transition Metal Complexes

Cinzia Imberti, Pingyu Zhang, Huaiyi Huang, Peter J. Sadler

Angewandte Chemie International Edition > 59 > 1 > 61 - 73

In this Minireview, we highlight recent advances in the design of transition metal complexes for photodynamic therapy (PDT) and photoactivated chemotherapy (PACT), and discuss the challenges and opportunities for the translation of such agents into clinical use. New designs for light‐activated transition metal complexes offer photoactivatable prodrugs with novel targeted mechanisms of action. Light...

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Electrostatic Complementarity Drives Amyloid/Nucleic Acid Co‐Assembly

Allisandra K. Rha, Dibyendu Das, Olga Taran, Yonggang Ke, more

Angewandte Chemie International Edition > 59 > 1 > 358 - 363

Proteinaceous plaques associated with neurodegenerative diseases contain many biopolymers including the polyanions glycosaminoglycans and nucleic acids. Polyanion‐induced amyloid fibrillation has been implicated in disease etiology, but structural models for amyloid/nucleic acid co‐assemblies remain limited. Here we constrain nucleic acid/peptide interactions with model peptides that exploit electrostatic...

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Copper‐Catalyzed Triboration of Terminal Alkynes Using B₂pin₂: Efficient Synthesis of 1,1,2‐Triborylalkenes

Xiaocui Liu, Wenbo Ming, Alexandra Friedrich, Florian Kerner, more

Angewandte Chemie International Edition > 59 > 1 > 304 - 309

We report herein the catalytic triboration of terminal alkynes with B₂pin₂ (bis(pinacolato)diboron) using readily available Cu(OAc)₂ and PⁿBu₃. Various 1,1,2‐triborylalkenes, a class of compounds that have been demonstrated to be potential matrix metalloproteinase (MMP‐2) inhibitors, were obtained directly in moderate to good yields. The process features mild reaction conditions, a broad substrate...

article

Tomislav Friščić

Angewandte Chemie International Edition > 59 > 1 > 30 - 30

“My motto is ‘work hard, play hard'. My favorite quote is ‘research not published is equivalent to research not done' …” Find out more about Tomislav Friščić in his Author Profile.

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Catalytic Oxidations in Organic Synthesis. Science of Synthesis, Workbench Edition Edited by Kilian Muniz.

Boris J. Nachtsheim

Angewandte Chemie International Edition > 59 > 1 > 32 - 32

Thieme, 2018. 880 pp., softcover, € 259.99.—ISBN 9783132012417

INFONA - science communication portal

Angewandte Chemie International Edition

Frontispiece: A 3.3 Å‐Resolution Structure of Hyperthermophilic Respiratory Complex III Reveals the Mechanism of Its Thermal Stability

Water‐Soluble Polymeric Carbon Nitride Colloidal Nanoparticles for Highly Selective Quasi‐Homogeneous Photocatalysis

New Members of the Editorial Board and International Advisory Board

Cascade Cross‐Coupling of Dienes: Photoredox and Nickel Dual Catalysis

Engineered C–N Lyase: Enantioselective Synthesis of Chiral Synthons for Artificial Dipeptide Sweeteners

Unpaired 3d Electrons on Atomically Dispersed Cobalt Centres in Coordination Polymers Regulate both Oxygen Reduction Reaction (ORR) Activity and Selectivity for Use in Zinc–Air Batteries

Cellulose Nanocrystal Elastomers with Reversible Visible Color

Topochemical Synthesis of Two‐Dimensional Transition‐Metal Phosphides Using Phosphorene Templates

Photoredox Catalytic α‐Alkoxypentafluorosulfanylation of α‐Methyl‐ and α‐Phenylstyrene Using SF₆

Hydrazide‐Catalyzed Polyene Cyclization: Asymmetric Organocatalytic Synthesis of cis‐Decalins

Inverting External Asymmetric Induction via Selective Energy Transfer Catalysis: A Strategy to β‐Chiral Phosphonate Antipodes

Characterization of Radical SAM Adenosylhopane Synthase, HpnH, which Catalyzes the 5′‐Deoxyadenosyl Radical Addition to Diploptene in the Biosynthesis of C₃₅ Bacteriohopanepolyols

Highly Selective Production of Ethylene by the Electroreduction of Carbon Monoxide

Stereoselective Csp³−Csp² Cross‐Couplings of Chiral Secondary Alkylzinc Reagents with Alkenyl and Aryl Halides

Hot Branching Dynamics in a Light‐Harvesting Iron Carbene Complex Revealed by Ultrafast X‐ray Emission Spectroscopy

New Designs for Phototherapeutic Transition Metal Complexes

Electrostatic Complementarity Drives Amyloid/Nucleic Acid Co‐Assembly

Copper‐Catalyzed Triboration of Terminal Alkynes Using B₂pin₂: Efficient Synthesis of 1,1,2‐Triborylalkenes

Tomislav Friščić

Catalytic Oxidations in Organic Synthesis. Science of Synthesis, Workbench Edition Edited by Kilian Muniz.

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