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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2018,130(30):9423-9427
Accessing the data points in the crystal structure landscape of a molecule is a challenging task, either experimentally or computationally. We have charted the crystal structure landscape of 4‐bromocinnamic acid (4BCA) experimentally and computationally: experimental doping is achieved with 4‐methylcinnamic acid (4MCA) to obtain new crystal structures; computational doping is performed with 4‐chlorocinnamic acid (4CCA) as a model system, because of the difficulties associated in parameterizing the Br atom. The landscape of 4CCA is explored experimentally in turn, also by doping it with 4MCA, and is found to bear a close resemblance to the landscape of 4BCA, justifying the ready miscibility of these two halogenated cinnamic acids to form solid solutions without any change in crystal structure. In effect, 4MCA, 4CCA and 4BCA form a commutable group of crystal structures, which may be realized experimentally or computationally, and constitute the landscape. Unlike the results obtained by Kitaigorodskii, all but two of the multiple solid solutions obtained in the methyl‐doping experiments take structures that are different from the hitherto observed crystal forms of the parent compounds. Even granted that the latter might be inherently polymorphic, this unusual observation provokes the suggestion that solid solution formation may be used to probe the crystal structure landscape. The influence of π⋅⋅⋅π interactions, weak hydrogen bonds and halogen bonds in directing the formation of these new structures is also seen. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(35):10466-10470
A novel methodology using CsF⋅Al2O3 as a highly efficient, environmentally benign, and reusable solid‐base catalyst was developed to synthesize glutamic acid derivatives by stereoselective 1,4‐addition of glycine derivatives to α,β‐unsaturated esters. CsF⋅Al2O3 showed not only great selectivity toward 1,4‐addtion reactions by suppressing the undesired formation of pyrrolidine derivations by [3+2] cycloadditions, but also offered high yields for the 1,4‐adduct with excellent anti diastereoselectivities. The catalyst was well characterized by using XRD, 19F MAS‐NMR and 19F NMR spectroscopy, FT‐IR, CO2‐TPD, and XPS. And highly basic F from Cs3AlF6 was identified as the most probable active basic site for the 1,4‐addition reactions. Continuous‐flow synthesis of 3‐methyl glutamic acid derivative was successfully demonstrated by using this solid‐base catalysis. 相似文献
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Dr. Xiaofei Hu Dr. Zifan Li Prof. Jun Chen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(21):5879-5883
Developing flexible Li-CO2 batteries is a promising approach to reuse CO2 and simultaneously supply energy to wearable electronics. However, all reported Li-CO2 batteries use liquid electrolyte and lack robust electrolyte/electrodes structure, not providing the safety and flexibility required. Herein we demonstrate flexible liquid-free Li-CO2 batteries based on poly(methacrylate)/poly(ethylene glycol)-LiClO4-3 wt %SiO2 composite polymer electrolyte (CPE) and multiwall carbon nanotubes (CNTs) cathodes. The CPE (7.14×10−2 mS cm−1) incorporates with porous CNTs cathodes, displaying stable structure and small interface resistance. The batteries run for 100 cycles with controlled capacity of 1000 mAh g−1. Moreover, pouch-type flexible batteries exhibit large reversible capacity of 993.3 mAh, high energy density of 521 Wh kg−1, and long operation time of 220 h at different degrees of bending (0–360°) at 55 °C. 相似文献
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Dong Zhou Anastasia Tkacheva Xiao Tang Bing Sun Devaraj Shanmukaraj Peng Li Fan Zhang Michel Armand Guoxiu Wang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(18):6062-6067
The low Coulombic efficiency and serious safety issues resulting from uncontrollable dendrite growth have severely impeded the practical applications of lithium (Li) metal anodes. Herein we report a stable quasi‐solid‐state Li metal battery by employing a hierarchical multifunctional polymer electrolyte (HMPE). This hybrid electrolyte was fabricated via in situ copolymerizing lithium 1‐[3‐(methacryloyloxy)propylsulfonyl]‐1‐(trifluoromethanesulfonyl)imide (LiMTFSI) and pentaerythritol tetraacrylate (PETEA) monomers in traditional liquid electrolyte, which is absorbed in a poly(3,3‐dimethylacrylic acid lithium) (PDAALi)‐coated glass fiber membrane. The well‐designed HMPE simultaneously exhibits high ionic conductivity (2.24×10?3 S cm?1 at 25 °C), near‐single ion conducting behavior (Li ion transference number of 0.75), good mechanical strength and remarkable suppression for Li dendrite growth. More intriguingly, the cation permselective HMPE efficiently prevents the migration of negatively charged iodine (I) species, which provides the as‐developed Li‐I batteries with high capacity and long cycling stability. 相似文献
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Yingqi Wang Xujie Lü Chong Zheng Xiang Liu Zonghai Chen Wenge Yang Jianhua Lin Fuqiang Huang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(23):7755-7759
Sulfide‐based superionic conductors with high ionic conductivity have been explored as candidates for solid‐state Li batteries. However, moisture hypersensitivity has made their manufacture complicated and costly and also impeded applications in batteries. Now, a sulfide‐based superionic conductor Li4Cu8Ge3S12 with superior stability was developed based on the hard/soft acid–base theory. The compound is stable in both moist air and aqueous LiOH aqueous solution. The electrochemical stability window was up to 1.5 V. An ionic conductivity of 0.9×10?4 S cm with low activation energy of 0.33 eV was achieved without any optimization. The material features a rigid Cu‐Ge‐S open framework that increases its stability. Meanwhile, the weak bonding between Li+ and the framework promotes ionic conductivity. This work provides a structural configuration in which weak Li bonding in the rigid framework promotes an environment for highly conductive and stable solid‐state electrolytes. 相似文献
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Junpeng Xie Xiaodan Li Haojie Lai Zhijuan Zhao Jinliang Li Wanggang Zhang Weiguang Xie Yiming Liu Wenjie Mai 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(41):14882-14889
Metal–organic framework‐derived NiCo2.5S4 microrods wrapped in reduced graphene oxide (NCS@RGO) were synthesized for potassium‐ion storage. Upon coordination with organic potassium salts, NCS@RGO exhibits an ultrahigh initial reversible specific capacity (602 mAh g?1 at 50 mA g?1) and ultralong cycle life (a reversible specific capacity of 495 mAh g?1 at 200 mA g?1 after 1 900 cycles over 314 days). Furthermore, the battery demonstrates a high initial Coulombic efficiency of 78 %, outperforming most sulfides reported previously. Advanced ex situ characterization techniques, including atomic force microscopy, were used for evaluation and the results indicate that the organic potassium salt‐containing electrolyte helps to form thin and robust solid electrolyte interphase layers, which reduce the formation of byproducts during the potassiation–depotassiation process and enhance the mechanical stability of electrodes. The excellent conductivity of the RGO in the composites, and the robust interface between the electrodes and electrolytes, imbue the electrode with useful properties; including, ultrafast potassium‐ion storage with a reversible specific capacity of 402 mAh g?1 even at 2 A g?1. 相似文献
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Bo Huang Hirokazu Kobayashi Tomokazu Yamamoto Takaaki Toriyama Syo Matsumura Yoshihide Nishida Katsutoshi Sato Katsutoshi Nagaoka Masaaki Haneda Wei Xie Yusuke Nanba Michihisa Koyama Fenglong Wang Shogo Kawaguchi Yoshiki Kubota Hiroshi Kitagawa 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(8):2252-2257
Ru is an important catalyst in many types of reactions. Specifically, Ru is well known as the best monometallic catalyst for oxidation of carbon monoxide (CO) and has been practically used in residential fuel cell systems. However, Ru is a minor metal, and the supply risk often causes violent fluctuations in the price of Ru. Performance‐improved and cost‐reduced solid‐solution alloy nanoparticles of the Cu‐Ru system for CO oxidation are now presented. Over the whole composition range, all of the CuxRu1?x nanoparticles exhibit significantly enhanced CO oxidation activities, even at 70 at % of inexpensive Cu, compared to Ru nanoparticles. Only 5 at % replacement of Ru with Cu provided much better CO oxidation activity, and the maximum activity was achieved by 20 at % replacement of Ru by Cu. The origin of the high catalytic performance was found as CO site change by Cu substitution, which was investigated using in situ Fourier transform infrared spectra and theoretical calculations. 相似文献