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Journal Angew. Chem. Int. Ed. Engl.

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Relative Thermodynamic Stability of Diamond and Graphite.

Mary Anne White, Samer Kahwaji, Vera L S Freitas, Riko Siewert, Joseph A Weatherby, Maria D M C Ribeiro da Silva, Sergey P Verevkin, Erin R Johnson, Josef W Zwanziger,

Recent density-functional theory (DFT) calculations raised the possibility that diamond could be degenerate with graphite at very low temperatures. Through high-accuracy calorimetric experiments closing gaps in available data, we reinvestigate the relative thermodynamic stability of diamond and graphite. For T < 400 K, graphite is always more stable than diamond ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Concise Total Synthesis of Tronocarpine.

Atsushi Nakayama, Tenta Nakamura, Toshihiro Zaima, Saho Fujimoto, Sangita Karanjit, Kosuke Namba,

A concise total synthesis of tronocarpine, a chippiine-type indole alkaloid, was accomplished. The key feature of this total synthesis is one-pot construction of the pentacyclic skeleton containing an azabicyclo[3.3.1]nonane core by tandem cyclization from an indole derivative having all carbon side chains and functional groups. This tandem cyclization consists of ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Toward flexible zinc-ion hybrid capacitors with superhigh energy density and ultralong cycling life: the pivotal role of ZnCl2 salt-based electrolytes.

Cheng Wang, Zengxia Pei, Qiangqiang Meng, Chunmei Zhang, Xiao Sui, Ziwen Yuan, Sijie Wang, Yuan Chen,

Zinc (Zn) ion hybrid capacitors (ZIHCs) are promising energy storage devices for emerging flexible electronics, but they still suffer from trade-off in energy density and cycling life. Herein, we prove that such a dilemma can be well-addressed by deploying ZnCl 2 based electrolytes. Combining experimental studies and density functional theory ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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High Ammonia Uptake of a Metal-Organic Framework Adsorbent in a Wide Pressure Range.

Dae Won Kim, Dong Won Kang, Minjung Kang, Jung-Hoon Lee, Jong Hyeak Choe, Yun Seok Chae, Doo San Choi, Hongryeol Yun, Chang Seop Hong,

Although numerous porous adsorbents have been investigated for NH 3  capture applications, these materials often exhibit insufficient NH 3 uptake, low NH 3 affinity at the ppm level, and poor chemical stability against wet NH 3 conditions. Herein, we report the NH 3 capture properties of M 2 (dobpdc) complexes ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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An Active-Site Sulfonate Group Creates a Fast Water Oxidation Electrocatalyst That Exhibits High Activity in Acid.

Aaron G Nash, Colton J Breyer, Brett D Vincenzini, Gregory I Elliott, Jens Niklas, Oleg G Poluektov, Arnold L Rheingold, Diane K Smith, Djamaladdin G Musaev, Douglas Grotjahn,

The storage of solar energy in chemical bonds will depend on pH-universal catalysts that are not only impervious to acid, but actually thrive in it. Whereas other homogeneous water oxidation catalysts are less active in acid, here we report a catalyst that maintains high electrocatalytic turnover frequency at pH values ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Carbide Dihydrides: Carbonaceous Species Identified in Ta4+-Mediated Methane Dehydrogenation.

Jozef Lengyel, Nikita Levin, Frank J Wensink, Olga V Lushchikova, Robert N Barnett, Uzi Landman, Ueli Heiz, Joost M Bakker, Martin Tschurl,

The products of methane dehydrogenation by gas-phase Ta 4 + clusters are structurally characterized using infrared multiple photon dissociation (IRMPD) spectroscopy in conjunction with quantum chemical calculations. The obtained spectra of [4Ta,C,2H] + reveal a dominance of vibrational bands of a H 2 Ta 4 C + carbide dihydride structure ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Effects of anion carriers on capacitance and self-discharge behaviors of zinc ion capacitor.

Zhaodong Huang, Tairan Wang, Hao Song, Xinliang Li, Guojin Liang, Donghong Wang, Qi Yang, Ze Chen, Longtao Ma, Zhuoxin Liu, Biao Gao, Jun Fan, Chunyi Zhi,

Introducing pseudocapacitive behavior and ion hybrid capacitor technique were deemed effective to improve the energy density of supercapacitors. However, the current research about ion hybrid capacitor only considered the reaction of cations during the electrochemical process, leading to a flawed mechanism understanding. Here, the effects of various anions carriers on ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Synthesis and Multiplexed Activity Profiling of Synthetic Acylphloroglucinol Scaffolds.

John Porco, Brian Bachmann, Jonathan Boyce, Benjamin Reisman,

Herein, we report novel formic acid-mediated rearrangements of dearomatized acylphloroglucinols to access a structurally diverse group of synthetic acylphloroglucinol scaffolds (SASs). Density functional theory (DFT)-optimized orbital and stereochemical analyses shed light on the mechanism of these rearrangements. Products were evaluated by multiplexed activity profiling (MAP), an unbiased platform which determines ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Direct writing large-area multi-layer ultrasmooth films by an all-solution process: toward high-performance QLEDs.

Huan Liu, Min Zhang, Huanhuan Deng, Lili Meng, Hongqin Wang, Yunjun Wang,

With increasing the film area/layer, deteriorating in both smoothness and uniformity of thin-films frequently happen, which remains a barrier for making large-area quantum dot light-emitting diodes (QLEDs) by solution processes. Here, we demonstrated a facile all-solution process guided by the conical fiber array to write multi-layer ultrasmooth thin-films directly in ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Frustrated Lewis Pair Chelation as a Vehicle for Low Temperature Semiconductor Element and Polymer Deposition.

Alvaro Omaña, Rachel Green, Ryo Kobayashi, Yingjie He, Evan Antoniuk, Michael Ferguson, Yuqiao Zhou, Jonathan Veinot, Takeaki Iwamoto, Alex Brown, Eric Rivard,

The stabilization of silicon(II) and germanium(II) dihydrides by an intramolecular Frustrated Lewis Pair (FLP) ligand, PB, i Pr-2P(C6H4)BCy2 (Cy = cyclohexyl) is reported. The resulting hydride complexes [PB{SiH2}] and [PB{GeH2}] are indefinitely stable at room temperature, yet can deposit films of silicon and germanium, respectively, upon mild thermolysis in solution. ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Synthesis of Vinylene-Linked Two-Dimensional Conjugated Polymers via the Horner-Wadsworth-Emmons Reaction.

Dominik L Pastoetter, Shunqi Xu, Mino Borrelli, Matthew Addicoat, Bishnu P Biswal, Silvia Paasch, Arezoo Dianat, Heidi Thomas, Reinhard Berger, Sebastian Reineke, Eike Brunner, Gianaurelio Cuniberti, Marcus Richter, Xinliang Feng,

Interest in linear conjugated polymers has significantly increased in recent decades due to their semiconducting properties and promising applications in organic optoelectronics. To date, the extension of linear conjugated polymers into two-dimensional conjugated polymers (2D CPs), which can also be regarded as 2D π-conjugated covalent organic frameworks (COFs), remains largely ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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NIR-Sensitized Cationic and Hybrid Radical/Cationic Polymerization and Crosslinking.

Yulian Pang, Atsushi Shiraishi, Dietmar Keil, Sergey Popov, Veronika Strehmel, Hongjun Jao, Jochen S Gutmann, Yinquan Zou, Bernd Strehmel,

NIR sensitized cationic polymerization proceeded with good efficiency as studied with epoxides, vinyl ether, and oxetanes.  A heptacyanine functioned as sensitizer while iodonium salts served as coinitiator.  The anion uptakes a special function as concluded by a series selected from fluorinated phosphates (a: [PF6]-, b: [PF3(C2F5)3]-, c: [PF3(n-C4F9)3]), aluminates (d: ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Phase-junction Electrocatalysts towards Enhanced Hydrogen Evolution Reaction in Alkaline Media.

Qiang Fu, Xianjie Wang, Jiecai Han, Jun Zhong, Zhang Tongrui, Tai Yao, Chengyan Xu, Tangling Gao, Shibo Xi, Ce Liang, Lingling Xu, Ping Xu, Bo Song,

To ensure the sustainable hydrogen production via water electrolysis technique, robust, earth-abundant and high-efficient electrocatalyst is highly required. Nowadays, to overcome the limitation of conventional single-phase component , constructing hybrid system could lead to further improvement in electrocatalytic activity. Interface engineering in composite catalysts is thus critical to determine the ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Precise alkoxyamine-design enables automated tandem mass spectrometry sequencing of digital poly(phosphodiester)s.

Kévin Launay, Jean-Arthur Amalian, Eline Laurent, Laurence Oswald, Abdelaziz Al Ouahabi, Alexandre Burel, Florent Dufour, Christine Carapito, Jean-Louis Clément, Jean-François Lutz, Laurence Charles, Didier Gigmes,

Increasing data storage density is one of the major challenges of the information industry. To be widely applicable, writing and reading information have to be dense, convenient and fast. A major step towards reliable reading of information coded in the sequence of long poly(phosphodiester)s was previously achieved by introducing an ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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A General and Highly Selective Palladium-Catalyzed Hydroamidation of 1,3-Diynes.

Jiawang Liu, Carolin Schneider, Ji Yang, Zhihong Wei, Haijun Jiao, Robert Franke, Ralf Jackstell, Matthias Beller,

A chemo-, regio- and stereoselective mono-hydroamidation of (un)symmetrical 1,3-diynes is described. Key for the success of this novel transformation is the utilization of an advanced palladium catalyst system with the specific ligand L6 (Neolephos). The synthetic value of this general approach to synthetically useful α-alkynyl-α, β-unsaturated amides is showcased by ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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LEAD-m6A-seq for Locus-specific Detection of N6-methyladenosine and Quantification of Differential Methylation.

Chuan He, Yuru Wang, Zijie Zhang, Caraline Sepich-Poore, Lisheng Zhang, Yu Xiao,

N 6 -methyladenosine (m 6 A) is a crucial RNA chemical mark which plays important roles in various biological processes. The development of highly multiplexed, cost-effective, and easy-to-operate methodologies for locus-specific analysis of m 6 A is critical for advancing our understanding of the roles of this modification. Here, we report ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Reductive Hexamerization of CO Involving Cooperativity Between Magnesium(I) Reductants and [Mo(CO)6]: Synthesis of Well-Defined Magnesium Benzenehexolate Complexes.

Cameron Jones, Albert Paparo, K Yuvaraj, Aidan J R Matthews, Iskander Douair, Laurent Maron,

Reactions of two magnesium(I) compounds, [{(ArNacnac)Mg}2] (ArNacnac = [HC(MeCNAr)2]-Ar = mesityl (Mes) or o-xylyl (Xyl)), with CO in the presence of [Mo(CO)6] lead to the reductive hexamerization of CO, and formation of magnesium benzenehexolate complexes, [{(ArNacnac)Mg}6(C6O6)]. [Mo(CO)6] is not consumed in these reactions, but is apparently required to initiate (or ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Amino-Supported Solid Palladium Catalyst for Chemo- and Stereoselective Domino Reactions.

Jan-E Bäckvall, Man-Bo Li, Jie Yang, Ying Yang, Guo-Yong Xu, Gen Luo, Jianping Yang,

An amino-supported solid palladium-catalyzed oxidative domino reaction has been developed for the diastereoselective construction of alkyne-substituted cyclopentenol compounds. This hetero-ge-neous catalyst exhibits high efficiency and excellent chemoselectivity, as well as good recyclability. The chemoselectivity of the domino reactions was readily controlled by switching the solvent and catalyst. Chiral syntheses and ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Cobalt-Catalyzed Markovnikov-Type Selective Hydroboration of Terminal Alkynes.

Jieping Chen, Xuzhong Shen, Zhan Lu,

Here, we reported a cobalt-catalyzed Markovnikov-type hydroboration of terminal alkynes with HBpin to access α -alkenyl boronates with good regioselectivity and atom economy. A new ligand has been developed for cobalt hydride catalyst which has been used for a unique Markovnikov selective insertion of terminal alkynes into metal hydride bond. ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Chemistry Evolves, Terms Evolve, but Phenomena Do Not Evolve: From Chalcogen-Chalcogen Interactions to Chalcogen Bonding.

Simon Kolb, Gwyndaf A Oliver, Daniel B Werz,

Chalcogen bonding is important in numerous aspects of chemistry, both in the solid state and in solution. Surveying the literature, it becomes clear that during its rebranding from chalcogen-chalcogen interactions, some parts of the community have somewhat neglected to recall its discovery and the initial studies referring to it in ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Directional bonding in {Nb10} inorganic frameworks.

May Nyman, Nicolas P Martin,

Metal-oxo clusters offer opportunity to assemble inorganic and metal-organic frameworks by a controlled building-block approach, which led to the revolutionary discoveries of zeolites and MOFs. Polyoxometalate clusters are soluble in water, but more challenging to link into frameworks-the inert oxo-caps that provide solubility are resistant to replacement or further connectivity. ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Pentacyclic Nano-Trefoil.

Huiyeong Ju, Yumiko Tsuruoka, Miho Hyano, Eunji Lee, Ki-Min Park, Mari Ikeda, Jun-Ichi Ishii, Shunsuke Kuwahara, Yoichi Habata,

Tetra-armed cyclen ( 1 ) bearing two 4-(4'-pyridyl)benzyl and two 3,5-difluorobenzyl groups and its Ag + complexes were prepared and structurally characterized. The complex formed between 1 and Ag + undergoes a reversible structural transformation between a 2:2 dimeric complex and a 3:5 pentacyclic trefoil complex with changes in the ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Hexafluoroisopropanol-Promoted Haloamidation and Halolactonization of Unactivated Alkenes.

Chenxiao Qi, Guillaume Force, Vincent Gandon, David Leboeuf,

Pyrrolidine and piperidine derivatives bearing halide functional groups are prevalent building blocks in drug discovery as halides can serve as an anchor for post-modifications. In principle, one of the simplest ways to build these frameworks is the haloamination of alkenes. While several progresses have been made in this field, notably ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Dual Intramolecular Electron Transfer for In Situ Coreactant-Embedded Electrochemiluminescence Microimaging of Membrane Protein.

Huangxian Ju, Ningning Wang, Hang Gao, Yunzhi Li, Guangming Li, Weiwei Chen, Zhongchao Jin, Jianping Lei, Qin Wei,

The demand for transporting coreactant to emitter and short lifetime of the radicals in electrochemiluminescence (ECL) emission inhibit greatly its application in cytosensing and microscopic imaging. Herein we designed a dual intramolecular electron transfer strategy and tertiary amine conjugated polymer dots (TEA-Pdots) to develop a coreactant-embedded ECL mechanism and microimaging ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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Photoinduced Aerobic Iodoarene-Catalyzed Spirocyclization of N-Oxy-Amides to N-Fused Spirolactams.

Kevin Cariou, Loïc Habert,

Iodoarene catalysis is a powerful methodology that usually requires an excess of oxidant, or of redox mediator if the terminal oxidant is dioxygen, to generate the key hypervalent iodine intermediate to proceed efficiently. We report that, using the spiro-cyclization of amides as a benchmark reaction, aerobic iodoarene catalysis can be ... Read more >>

Angew. Chem. Int. Ed. Engl. (Angewandte Chemie (International ed. in English))
[2020, :]

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