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991.
Prof. Dr. Qian Miao Dr. Farzaneh Rouhani Dr. Hamed Moghanni-Bavil-Olyaei Dr. Kuan-Guan Liu Xue-Mei Gao Jing-Zhe Li Xiu-De Hu Prof. Dr. Zhi-Min Jin Prof. Mao-Lin Hu Prof. Ali Morsali 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(43):9518-9526
As redox-active based supercapacitors are known as highly desirable next-generation supercapacitor electrodes, the targeted design of two ferrocene-functionalized (Fc(COOH)2) clusters based on coinage metals, [(PPh3)2AgO2CFcCO2Ag(PPh3)2]2 ⋅ 7 CH3OH (SC1: super capacitor) and [(PPh3)3CuO2CFcCO2Cu(PPh3)3] ⋅ 3 CH3OH (SC2), is reported. Both structures are fully characterized by various techniques. The structures are utilized as energy storage electrode materials, giving 130 F g−1 and 210 F g−1 specific capacitance at 1.5 A g−1 in Na2SO4 electrolyte, respectively. The obtained results show that the presence of CuI instead of AgI improves the supercapacitive performance of the cluster. Further, to improve the conductivity, the PSC2 ([(PPh3)2CuO2CFcCO2]∞), a polymeric structure of SC2, was synthesized and used as an energy storage electrode. PSC2 displays high conductivity and gives 455 F g−1 capacitance at 3 A g−1. The PSC2 as a supercapacitor electrode presents a high power density (2416 W kg−1), high energy density (161 Wh kg−1), and long cycle life over 4000 cycles (93 %). These results could lead to the amplification of high-performance supercapacitors in new areas to develop real applications and stimulate the use of the targeted design of coordination polymers without hybridization or compositions with additive materials. 相似文献
992.
Tuuli A. Hakala Sarah Davies Dr. Zenon Toprakcioglu Dr. Barbara Bernardim Dr. Gonçalo J. L. Bernardes Prof. Tuomas P. J. Knowles 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(27):5965-5969
Nanoparticles are widely studied as carrier vehicles in biological systems because their size readily allows access through cellular membranes. Moreover, they have the potential to carry cargo molecules and as such, these factors make them especially attractive for intravenous drug delivery purposes. Interest in protein-based nanoparticles has recently gained attraction due to particle biocompatibility and lack of toxicity. However, the production of homogeneous protein nanoparticles with high encapsulation efficiencies, without the need for additional cross-linking or further engineering of the molecule, remains challenging. Herein, we present a microfluidic 3D co-flow device to generate human serum albumin/celastrol nanoparticles by co-flowing an aqueous protein solution with celastrol in ethanol. This microscale co-flow method resulted in the formation of nanoparticles with a homogeneous size distribution and an average size, which could be tuned from ≈100 nm to 1 μm by modulating the flow rates used. We show that the high stability of the particles stems from the covalent cross-linking of the naturally present cysteine residues within the particles formed during the assembly step. By choosing optimal flow rates during synthesis an encapsulation efficiency of 75±24 % was achieved. Finally, we show that this approach achieves significantly enhanced solubility of celastrol in the aqueous phase and, crucially, reduced cellular toxicity. 相似文献
993.
Summary New chiral cyclopentadienyl-titanium and-zirconium complexes Cp2TiCl2, CpCpTiCl2 and Cp2ZrCl2 (Cp=5 -cyclopentadienyl and Cp=substituted cyclopentadienyl), have been synthesized. The (S,S)-3 complex, which forms red plate crystals, has been studied by x-ray analysis. It belongs to the monoclinic space groupC2, witha 23.963(3),b 6.6470(6),c 12.6618(9) Å, 103.089(7)°, V=1964.4(3) Å3 and Z=4. The structure was relined to an R factor of 0.048 for 868 observed reflections. 相似文献
994.
Therese Planke Katarina Cirnski Dr. Jennifer Herrmann Prof. Dr. Rolf Müller Prof. Dr. Andreas Kirschning 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(19):4289-4296
Cystobactamids belong to the group of arene-based oligoamides that effectively inhibit bacterial type IIa topoisomerases. Cystobactamid 861-2 is the most active member of these antibiotics. Most amide bonds present in the cystobactamids link benzoic acids with anilines and it was found that some of these amide bonds undergo chemical and enzymatic hydrolysis, especially the one linking ring C with ring D. This work reports on the chemical synthesis and biological evaluation of thirteen new cystobactamids that still contain the methoxyaspartate hinge. However, we exchanged selected amide bonds either by the urea or the triazole groups and modified ring A in the latter case. While hydrolytic stability could be improved with these structural substitutes, the high antibacterial potency of cystobactamid 861-2 could only be preserved in selected cases. This includes derivatives, in which the urea group is positioned between rings A and B and where the triazole is found between rings C and D. 相似文献
995.
Juan Li Shuang Hou Tiezhong Liu Liangke Wang Chen Mei Yayun Guo Prof. Lingzhi Zhao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(9):2013-2024
Improving the performance of anode materials for lithium-ion batteries (LIBs) is a hotly debated topic. Herein, hollow Ni−Co skeleton@MoS2/MoO3 nanocubes (NCM-NCs), with an average size of about 193 nm, have been synthesized through a facile hydrothermal reaction. Specifically, MoO3/MoS2 composites are grown on Ni−Co skeletons derived from nickel–cobalt Prussian blue analogue nanocubes (Ni−Co PBAs). The Ni−Co PBAs were synthesized through a precipitation method and utilized as self-templates that provided a larger specific surface area for the adhesion of MoO3/MoS2 composites. According to Raman spectroscopy results, as-obtained defect-rich MoS2 is confirmed to be a metallic 1T-phase MoS2. Furthermore, the average particle size of Ni−Co PBAs (≈43 nm) is only about one-tenth of the previously reported particle size (≈400 nm). If assessed as anodes of LIBs, the hollow NCM-NC hybrids deliver an excellent rate performance and superior cycling performance (with an initial discharge capacity of 1526.3 mAh g−1 and up to 1720.6 mAh g−1 after 317 cycles under a current density of 0.2 A g−1). Meanwhile, ultralong cycling life is retained, even at high current densities (776.6 mAh g−1 at 2 A g−1 after 700 cycles and 584.8 mAh g−1 at 5 A g−1 after 800 cycles). Moreover, at a rate of 1 A g−1, the average specific capacity is maintained at 661 mAh g−1. Thus, the hierarchical hollow NCM-NC hybrids with excellent electrochemical performance are a promising anode material for LIBs. 相似文献
996.
Aleksandr Zaichenko Dr. Daniel Schröder Prof. Dr. Jürgen Janek Prof. Dr. Doreen Mollenhauer 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(11):2395-2404
Recent experimental investigations demonstrated the generation of singlet oxygen during charging at high potentials in lithium/oxygen batteries. To contribute to the understanding of the underlying chemical reactions a key step in the mechanism of the charging process, namely, the dissociation of the intermediate lithium superoxide to oxygen and lithium, was investigated. Therefore, the corresponding dissociation paths of the molecular model system lithium superoxide (LiO2) were studied by CASSCF/CASPT2 calculations. The obtained results indicate the presence of different dissociation paths over crossing points of different electronic states, which lead either to the energetically preferred generation of triplet oxygen or the energetically higher lying formation of singlet oxygen. The dissociation to the corresponding superoxide anion is energetically less preferred. The understanding of the detailed reaction mechanism allows the design of strategies to avoid the formation of singlet oxygen and thus to potentially minimize the degradation of materials in alkali metal/oxygen batteries. The calculations demonstrate a qualitatively similar but energetically shifted behavior for the homologous alkali metals sodium and potassium and their superoxide species. Fundamental differences were found for the covalently bound hydroperoxyl radical. 相似文献
997.
Bo Wang Dr. Wencheng Du Dr. Yang Yang Dr. Yufei Zhang Dr. Qi Zhang Prof. Xianhong Rui Dr. Hongbo Geng Prof. Cheng Chao Li 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(29):6554-6560
Lithium ion batteries (LIBs) at present still suffer from low rate capability and poor cycle life during fast ion insertion/extraction processes. Searching for high-capacity and stable anode materials is still an ongoing challenge. Herein, a facile strategy for the synthesis of ultrathin GeS2 nanosheets with the thickness of 1.1 nm is reported. When used as anodes for LIBs, the two-dimensional (2D) structure can effectively increase the electrode/electrolyte interface area, facilitate the ion transport, and buffer the volume expansion. Benefiting from these merits, the as-synthesized GeS2 nanosheets deliver high specific capacity (1335 mAh g−1 at 0.15 A g−1), extraordinary rate performance (337 mAh g−1 at 15 A g−1) and stable cycling performance (974 mAh g−1 after 200 cycles at 0.5 A g−1). Importantly, our fabricated Li-ion full cells manifest an impressive specific capacity of 577 mAh g−1 after 50 cycles at 0.1 A g−1 and a high energy density of 361 Wh kg−1 at a power density of 346 W kg−1. Furthermore, the electrochemical reaction mechanism is investigated by the means of ex-situ high-resolution transmission electron microscopy. These results suggest that GeS2 can use to be an alternative anode material and encourage more efforts to develop other high-performance LIBs anodes. 相似文献
998.
Dr. Kalaiselvi Natarajan Daniel Müller-Klieser Stefan Rubner Prof. Dr. Thorsten Berg 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(1):148-154
We present a new approach for the identification of inhibitors of phosphorylation-dependent protein–protein interaction domains, in which phenolic fragments are adapted by in silico O-phosphorylation before docking-based screening. From a database of 10 369 180 compounds, we identified 85 021 natural product-derived phenolic fragments, which were virtually O-phosphorylated and screened for in silico binding to the STAT3 SH2 domain. Nine screening hits were then synthesized, eight of which showed a degree of in vitro inhibition of STAT3. After analysis of its selectivity profile, the most potent inhibitor was then developed to Stafia-1, the first small molecule shown to preferentially inhibit the STAT family member STAT5a over the close homologue STAT5b. A phosphonate prodrug based on Stafia-1 inhibited STAT5a with selectivity over STAT5b in human leukemia cells, providing the first demonstration of selective in vitro and intracellular inhibition of STAT5a by a small-molecule inhibitor. 相似文献
999.
Kanna Adachi Tomoshi Yamada Hayate Ishizuka Mana Oki Shunsuke Tsunogae Noriko Shimada Osamu Chiba Tatsuya Orihara Prof. Dr. Masafumi Hidaka Prof. Dr. Takatsugu Hirokawa Dr. Minami Odagi Prof. Dr. Keiichi Konoki Prof. Dr. Mari Yotsu-Yamashita Prof. Dr. Kazuo Nagasawa 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(9):2025-2033
A novel series of C12-keto-type saxitoxin (STX) derivatives bearing an unusual nonhydrated form of the ketone at C12 has been synthesized, and their NaV-inhibitory activity has been evaluated in a cell-based assay as well as whole-cell patch-clamp recording. Among these compounds, 11-benzylidene STX ( 3 a ) showed potent inhibitory activity against neuroblastoma Neuro 2A in both cell-based and electrophysiological analyses, with EC50 and IC50 values of 8.5 and 30.7 nm , respectively. Interestingly, the compound showed potent inhibitory activity against tetrodotoxin-resistant subtype of NaV1.5, with an IC50 value of 94.1 nm . Derivatives 3 a – d and 3 f showed low recovery rates from NaV1.2 subtype (ca 45–79 %) compared to natural dcSTX ( 2 ), strongly suggesting an irreversible mode of interaction. We propose an interaction model for the C12-keto derivatives with NaV in which the enone moiety in the STX derivatives 3 works as Michael acceptor for the carboxylate of Asp1717. 相似文献
1000.
Shuping Zhang Dr. Hongpan Rong Tianyi Yang Bing Bai Prof. Jiatao Zhang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(18):4025-4031
Dilute alloy nanostructures have been demonstrated to possess distinct catalytic properties. Noble-metal-induced reduction is one effective synthesis strategy to construct dilute alloys and modify the catalytic performance of the host metal. Herein, we report the synthesis of ultrafine PtRu dilute alloy nanodendrites (PtRu NDs, molar ratio Ru/Pt is 1:199) by the reduction of RuIII ions induced by Pt metal. For the methanol oxidation reaction, PtRu NDs showed the highest forward peak current density (2.66 mA cm−2, 1.14 A/mgPt) and the best stability compared to those of pure-Pt nanodendrites (pure-Pt NDs), commercial PtRu/C and commercial Pt/C catalysts. 相似文献