共查询到20条相似文献,搜索用时 31 毫秒
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Dr. Heng Zhang Dr. Chunmei Li Dr. Gebrekidan Gebresilassie Eshetu Prof. Stéphane Laruelle Prof. Sylvie Grugeon Prof. Karim Zaghib Prof. Christian Julien Prof. Alain Mauger Prof. Dominique Guyomard Prof. Teófilo Rojo Dr. Nuria Gisbert-Trejo Prof. Stefano Passerini Prof. Xuejie Huang Prof. Zhibin Zhou Prof. Patrik Johansson Prof. Maria Forsyth 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(2):542-546
Lithium-ion batteries (LIBs) have become ubiquitous power sources for small electronic devices, electric vehicles, and stationary energy storage systems. Despite the success of LIBs which is acknowledged by their increasing commodity market, the historical evolution of the chemistry behind the LIB technologies is laden with obstacles and yet to be unambiguously documented. This Viewpoint outlines chronologically the most essential findings related to today's LIBs, including commercial electrode and electrolyte materials, but furthermore also depicts how the today popular and widely emerging solid-state batteries were instrumental at very early stages in the development of LIBs. 相似文献
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Dr. Ying Huang Prof. Bo Chen Jian Duan Fei Yang Tengrui Wang Zhengfeng Wang Dr. Wenjuan Yang Dr. Chenchen Hu Prof. Wei Luo Prof. Yunhui Huang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(9):3728-3733
Solid-state Li metal batteries (SSLMBs) have attracted considerable interests due to their promising energy density as well as high safety. However, the realization of a well-matched Li metal/solid-state electrolyte (SSE) interface remains challenging. Herein, we report g-C3N4 as a new interface enabler. We discover that introducing g-C3N4 into Li metal can not only convert the Li metal/garnet-type SSE interface from point contact to intimate contact but also greatly enhance the capability to suppress the dendritic Li formation because of the greatly enhanced viscosity, decreased surface tension of molten Li, and the in situ formation of Li3N at the interface. Thus, the resulting Li-C3N4|SSE|Li-C3N4 symmetric cell gives a significantly low interfacial resistance of 11 Ω cm2 and a high critical current density (CCD) of 1500 μA cm−2. In contrast, the same symmetric cell configuration with pristine Li metal electrodes has a much larger interfacial resistance (428 Ω cm2) and a much lower CCD (50 μA cm−2). 相似文献
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Dr. Janine George Dr. David Waroquiers Dr. Davide Di Stefano Dr. Guido Petretto Prof. Dr. Gian-Marco Rignanese Prof. Dr. Geoffroy Hautier 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(19):7639-7645
The Pauling rules have been used for decades to rationalise the crystal structures of ionic compounds. Despite their importance, there has been no statistical assessment of the performances of these five empirical rules so far. Here, we rigorously and automatically test all five Pauling rules for a large data set of around 5000 known oxides. We discuss each Pauling rule separately, stressing their limits and range of application in terms of chemistries and structures. We conclude that only 13 % of the oxides simultaneously satisfy the last four rules, indicating a much lower predictive power than expected. 相似文献
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Stefanie Hermann Martin Wessig Dennis Kollofrath Melanie Gerigk Kay Hagedorn Dr. James A. Odendal Dr. Matthias Hagner Dr. Markus Drechsler Philipp Erler Prof. Dr. Mikhail Fonin Prof. Dr. Georg Maret Prof. Dr. Sebastian Polarz 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(20):5567-5571
Gaining external control over self-organization is of vital importance for future smart materials. Surfactants are extremely valuable for the synthesis of diverse nanomaterials. Their self-assembly is dictated by microphase separation, the hydrophobic effect, and head-group repulsion. It is desirable to supplement surfactants with an added mode of long-range and directional interaction. Magnetic forces are ideal, as they are not shielded in water. We report on surfactants with heads containing tightly bound transition-metal centers. The magnetic moment of the head was varied systematically while keeping shape and charge constant. Changes in the magnetic moment of the head led to notable differences in surface tension, aggregate size, and contact angle, which could also be altered by an external magnetic field. The most astonishing result was that the use of magnetic surfactants as structure-directing agents enabled the formation of porous solids with 12-fold rotational symmetry. 相似文献
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Sebastian Vogel Dr. Maxim Bykov Dr. Elena Bykova Sebastian Wendl Dr. Simon D. Kloß Dr. Anna Pakhomova Prof. Dr. Natalia Dubrovinskaia Prof. Dr. Leonid Dubrovinsky Prof. Dr. Wolfgang Schnick 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(7):2752-2756
Owing to its outstanding elastic properties, the nitride spinel γ-Si3N4 is of considered interest for materials scientists and chemists. DFT calculations suggest that Si3N4-analog beryllium phosphorus nitride BeP2N4 adopts the spinel structure at elevated pressures as well and shows outstanding elastic properties. Herein, we investigate phenakite-type BeP2N4 by single-crystal synchrotron X-ray diffraction and report the phase transition into the spinel-type phase at 47 GPa and 1800 K in a laser-heated diamond anvil cell. The structure of spinel-type BeP2N4 was refined from pressure-dependent in situ synchrotron powder X-ray diffraction measurements down to ambient pressure, which proves spinel-type BeP2N4 a quenchable and metastable phase at ambient conditions. Its isothermal bulk modulus was determined to 325(8) GPa from equation of state, which indicates that spinel-type BeP2N4 is an ultraincompressible material. 相似文献
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Dr. Jiangman Sun Dr. Xiao Dong Dr. Yajie Wang Dr. Kuo Li Dr. Haiyan Zheng Dr. Lijuan Wang Dr. George D. Cody Dr. Christopher A. Tulk Jamie J. Molaison Dr. Xiaohuan Lin Dr. Yufei Meng Dr. Changqing Jin Dr. Ho-kwang Mao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(23):6653-6657
Geometric isomerism in polyacetylene is a basic concept in chemistry textbooks. Polymerization to cis-isomer is kinetically preferred at low temperature, not only in the classic catalytic reaction in solution but also, unexpectedly, in the crystalline phase when it is driven by external pressure without a catalyst. Until now, no perfect reaction route has been proposed for this pressure-induced polymerization. Using in situ neutron diffraction and meta-dynamic simulation, we discovered that under high pressure, acetylene molecules react along a specific crystallographic direction that is perpendicular to those previously proposed. Following this route produces a pure cis-isomer and more surprisingly, predicts that graphane is the final product. Experimentally, polycyclic polymers with a layered structure were identified in the recovered product by solid-state nuclear magnetic resonance and neutron pair distribution functions, which indicates the possibility of synthesizing graphane under high pressure. 相似文献
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Dr. Aleksandr Savateev Dr. Nadezda V. Tarakina Dr. Volker Strauss Dr. Tanveer Hussain Katharina ten Brummelhuis José Manuel Sánchez Vadillo Yevheniia Markushyna Stefano Mazzanti Dr. Alexander P. Tyutyunnik Dr. Ralf Walczak Dr. Martin Oschatz Prof. Dirk M. Guldi Prof. Amir Karton Prof. Markus Antonietti 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(35):15172-15180
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Julie L. Fenton Prof. Raymond E. Schaak 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(23):6564-6567
The ability to selectively form one crystal structure among several options in a polymorphic system is an important goal in solid-state synthesis. Nanocrystal cation exchange, which proceeds rapidly under mild conditions, can retain key structural features and yield otherwise inaccessible phases, but the extent to which crystal structure can be retained and therefore selectively targeted during such reactions has been limited. Here, we show that nanocrystals of digenite Cu2−xS transform to zincblende MnS and CoS upon cation exchange. Zincblende MnS and CoS, which are metastable in bulk, retain both the tetrahedral cation coordination and cubic close packed anion sublattice of digenite Cu2−xS. Comparison with wurtzite MnS and CoS, which have been accessed previously through analogous cation exchange of roxbyite Cu2−xS, demonstrates the selective formation of the related zincblende vs. wurtzite polymorphs by cation exchange of structurally distinct templates. 相似文献
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Li Hong Dr. Jovana V. Milić Paramvir Ahlawat Dr. Marko Mladenović Dr. Dominik J. Kubicki Farzaneh Jahanabkhshi Dr. Dan Ren María C. Gélvez-Rueda Dr. Marco A. Ruiz-Preciado Dr. Amita Ummadisingu Dr. Yuhang Liu Chengbo Tian Linfeng Pan Dr. Shaik M. Zakeeruddin Prof. Anders Hagfeldt Prof. Ferdinand C. Grozema Prof. Ursula Rothlisberger Prof. Lyndon Emsley Prof. Hongwei Han Prof. Michael Graetzel 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(12):4721-4727
Formamidinium (FA) lead iodide perovskite materials feature promising photovoltaic performances and superior thermal stabilities. However, conversion of the perovskite α-FAPbI3 phase to the thermodynamically stable yet photovoltaically inactive δ-FAPbI3 phase compromises the photovoltaic performance. A strategy is presented to address this challenge by using low-dimensional hybrid perovskite materials comprising guaninium (G) organic spacer layers that act as stabilizers of the three-dimensional α-FAPbI3 phase. The underlying mode of interaction at the atomic level is unraveled by means of solid-state nuclear magnetic resonance spectroscopy, X-ray crystallography, transmission electron microscopy, molecular dynamics simulations, and DFT calculations. Low-dimensional-phase-containing hybrid FAPbI3 perovskite solar cells are obtained with improved performance and enhanced long-term stability. 相似文献
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Zheng Niu Elke Prade Eleni Malideli Kathleen Hille Alexander Jussupow Yonatan G. Mideksa Li-Mei Yan Chen Qian Markus Fleisch Ana C. Messias Riddhiman Sarkar Michael Sattler Don C. Lamb Matthias J. Feige Carlo Camilloni Aphrodite Kapurniotu Bernd Reif 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(14):5820-5830
Designed peptides derived from the islet amyloid polypeptide (IAPP) cross-amyloid interaction surface with Aβ (termed interaction surface mimics or ISMs) have been shown to be highly potent inhibitors of Aβ amyloid self-assembly. However, the molecular mechanism of their function is not well understood. Using solution-state and solid-state NMR spectroscopy in combination with ensemble-averaged dynamics simulations and other biophysical methods including TEM, fluorescence spectroscopy and microscopy, and DLS, we characterize ISM structural preferences and interactions. We find that the ISM peptide R3-GI is highly dynamic, can adopt a β-like structure, and oligomerizes into colloid-like assemblies in a process that is reminiscent of liquid–liquid phase separation (LLPS). Our results suggest that such assemblies yield multivalent surfaces for interactions with Aβ40. Sequestration of substrates into these colloid-like structures provides a mechanistic basis for ISM function and the design of novel potent anti-amyloid molecules. 相似文献
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Dr. Chao Wang Min Hu Dr. Yueying Chu Xue Zhou Dr. Qiang Wang Dr. Guodong Qi Dr. Shenhui Li Prof. Dr. Jun Xu Prof. Dr. Feng Deng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(18):7265-7269
The understanding of catalyst deactivation represents one of the major challenges for the methanol-to-hydrocarbon (MTH) reaction over acidic zeolites. Here we report the critical role of intermolecular π-interactions in catalyst deactivation in the MTH reaction on zeolites H-SSZ-13 and H-ZSM-5. π-interaction-induced spatial proximities between cyclopentenyl cations and aromatics in the confined channels and/or cages of zeolites are revealed by two-dimensional solid-state NMR spectroscopy. The formation of naphtalene as a precursor to coke species is favored due to the reaction of aromatics with the nearby cyclopentenyl cations and correlates with both acid density and zeolite topology. 相似文献
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Vitaly L. Sushkevich René Verel Jeroen A. van Bokhoven 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(2):920-928
The reaction of methane with copper-exchanged mordenite with two different Si/Al ratios was studied by means of in situ NMR and infrared spectroscopies. The detection of NMR signals was shown to be possible with high sensitivity and resolution, despite the presence of a considerable number of paramagnetic CuII species. Several types of surface-bonded compounds were found after reaction, namely molecular methanol, methoxy species, dimethyl ether, mono- and bidentate formates, CuI monocarbonyl as well as carbon monoxide and dioxide, which were present in the gas phase. The relative fractions of these species are strongly influenced by the reaction temperature and the structure of the copper sites and is governed by the Si/Al ratio. While methoxy species bonded to Brønsted acid sites, dimethyl ether and bidentate formate species are the main products over copper-exchange mordenite with a Si/Al ratio of 6; molecular methanol and monodentate formate species were observed mainly over the material with a Si/Al ratio of 46. These observations are important for understanding the methane partial oxidation mechanism and for the rational design of the active materials for this reaction. 相似文献
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Henry W. Orton Dr. Jan Stanek Dr. Tobias Schubeis Dylan Foucaudeau Claire Ollier Dr. Adrian W. Draney Dr. Tanguy Le Marchand Dr. Diane Cala-De Paepe Prof. Dr. Isabella C. Felli Prof. Dr. Roberta Pierattelli Prof. Dr. Sebastian Hiller Dr. Wolfgang Bermel Dr. Guido Pintacuda 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(6):2400-2405
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Dr. Qun Cao Dr. Deborah E. Crawford Chengcheng Shi Prof. Stuart L. James 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(11):4508-4513
A continuous, scalable, and solvent-free method for the synthesis of various naphthalic imides and perylene diimides (PDIs) using twin-screw extrusion (TSE) is reported. Using TSE, naphthalic imides were obtained quantitatively without the need for excess amine reactant or product purification. With good functional-group tolerance, alkyl and benzyl amine derived PDIs (incl. commercial dyes) were obtained in 50–99 % yield. Use of K2CO3, enabled synthesis of more difficult aniline-derived PDIs. Furthermore, an automated continuous TSE process for Pigments Black 31 and 32 is demonstrated, with a throughput rate of about 1500 g day−1, corresponding to a space time yield of about 30×103 kg m−3 day−1, which is 1–2 orders of magnitude greater than for solvent-based batch methods. These methods provide substantial waste reductions and improved efficiency compared to conventional solvent-based methods. 相似文献