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991.
Peng-Bo Jin Yuan-Qi Zhai Ke-Xin Yu Prof. Dr. Richard E. P. Winpenny Prof. Dr. Yan-Zhen Zheng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(24):9436-9440
The dicarbollide ion, nido-C2B9H112− is isoelectronic with cyclopentadienyl. Herein, we make dysprosiacarboranes, namely [(C2B9H11)2Ln(THF)2][Na(THF)5] (Ln=Dy, 1Dy ) and [(THF)3(μ-H)3Li]2[{η5-C6H4(CH2)2C2B9H9}Dy{η2:η5-C6H4(CH2)2C2B9H9}2Li] 3Dy and show that dicarbollide ligands impose strong magnetic axiality on the central DyIII ion. The effective energy barrier (Ueff) for the loss of magnetization can be varied by the substitution pattern on the dicarbollide. This finding is demonstrated by comparing complexes of nido-C2B9H112− and nido-[o-xylylene-C2B9H9]2−, which show a Ueff of 430(5) K and 804(7) K, respectively. The blocking temperature defined by the open hysteresis temperature of 3Dy reaches 6.8 K. Moreover, the linear complex [Dy(C2B9H11)2]− is predicted to have comparable properties with the linear [Dy(CpMe3)2]+ complex. As such, carboranyl ligands and their derivatives may provide a new type of organometallic ligand for high-performance single-molecule magnets. 相似文献
992.
Ying Liu Dr. Ximing Rong Mingze Li Prof. Maxim S. Molokeev Prof. Jing Zhao Prof. Zhiguo Xia 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(28):11731-11737
The incorporation of impurity ions or doping is a promising method for controlling the electronic and optical properties and the structural stability of halide perovskite nanocrystals (NCs). Herein, we establish relationships between rare-earth ions doping and intrinsic emission of lead-free double perovskite Cs2AgInCl6 NCs to impart and tune the optical performances in the visible light region. Tb3+ ions were incorporated into Cs2AgInCl6 NCs and occupied In3+ sites as verified by both crystallographic analyses and first-principles calculations. Trace amounts of Bi doping endowed the characteristic emission (5D4→7F6-3) of Tb3+ ions with a new excitation peak at 368 nm rather than the single characteristic excitation at 290 nm of Tb3+. By controlling Tb3+ ions concentration, the emission colors of Bi-doped Cs2Ag(In1−xTbx)Cl6 NCs could be continuously tuned from green to orange, through the efficient energy-transfer channel from self-trapped excitons to Tb3+ ions. Our study provides the salient features of the material design of lead-free perovskite NCs and to expand their luminescence applications. 相似文献
993.
Guangchen Sun Yu-Chen Wei Dr. Zhiyun Zhang Jia-An Lin Zong-Ying Liu Dr. Wei Chen Prof. Jianhua Su Prof. Pi-Tai Chou Prof. He Tian 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(42):18770-18777
Herein, we introduce the cyclic 8π-electron (C8π) molecule N,N′-diaryl-dihydrodibenzo[a,c]phenazine ( DPAC ) as a dual-functional donor to establish a series of new donor–linker–acceptor (D–L–A) dyads DLA1 – DLA5 . The excited-state bent-to-planar dynamics of DPAC regulate the energy gap of the donor, while the acceptors A1 – A5 are endowed with different energy gaps and HOMO/LUMO levels. As a result, the rate and efficiency of the excited-state electron transfer vs. energy transfer can be finely harnessed, which is verified via steady-state spectroscopy and time-resolved emission measurements. This comprehensive approach demonstrates, for the first time, the manifold of excited-state properties governed by bifunctional donor-based D–L–A dyads, including bent-to-planar, photoinduced electron transfer (PET) from excited donor to acceptor (oxidative-PET), fluorescence resonance energy transfer (FRET), bent-to-planar followed by electron transfer (PFET), and PET from donor to excited acceptor (reductive-PET). 相似文献
994.
Yue Sun Dr. Tiandu Dong Dr. Chunxin Lu Weiwen Xin Linsen Yang Pei Liu Yongchao Qian Yuanyuan Zhao Dr. Xiang-Yu Kong Prof. Liping Wen Prof. Lei Jiang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(40):17576-17581
Osmotic energy, obtained through different concentrations of salt solutions, is recognized as a form of a sustainable energy source. In the past years, membranes derived from asymmetric aromatic compounds have attracted attention because of their low cost and high performance in osmotic energy conversion. The membrane formation process, charging state, functional groups, membrane thickness, and the ion-exchange capacity of the membrane could affect the power generation performance. Among asymmetric membranes, a bipolar membrane could largely promote the ion transport. Here, two polymers with the same poly(ether sulfone) main chain but opposite charges were synthesized to prepare bipolar membranes by a nonsolvent-induced phase separation (NIPS) and spin-coating (SC) method. The maximum power density of the bipolar membrane reaches about 6.2 W m−2 under a 50-fold salinity gradient, and this result can serve as a reference for the design of bipolar membranes for osmotic energy conversion systems. 相似文献
995.
Zhiwei Tie Prof. Zhiqiang Niu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(48):21477-21487
Organic electroactive compounds are attractive to serve as the cathode materials of aqueous zinc-ion batteries (ZIBs) because of their resource renewability, environmentally friendliness and structural diversity. Up to now, various organic electrode materials have been developed and different redox mechanisms are observed in aqueous Zn/organic battery systems. In this Minireview, we present the recent developments in the energy storage mechanisms and design of the organic electrode materials of aqueous ZIBs, including carbonyl compounds, imine compounds, conductive polymers, nitronyl nitroxides, organosulfur polymers and triphenylamine derivatives. Furthermore, we highlight the design strategies to improve their electrochemical performance in the aspects of specific capacity, output voltage, cycle life and rate capability. Finally, we discuss the challenges and future perspectives of aqueous Zn/organic batteries. 相似文献
996.
Dr. Zhenhua Gao Baoyuan Xu Tongjin Zhang Zhen Liu Weiguang Zhang Xun Sun Yang Liu Dr. Xue Wang Dr. Zifei Wang Prof. Yongli Yan Prof. Fengqin Hu Prof. Xiangeng Meng Prof. Yong Sheng Zhao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(43):19222-19226
Micro/nanoscale photonic barcodes based on multicolor luminescent segmented heterojunctions hold potential for applications in information security. However, such multicolor heterojunctions reported thus far are exclusively based on static luminescent signals, thus restricting their application in advanced confidential information protection. Reported here is a strategy to design responsive photonic barcodes with heterobimetallic (Tb3+/Eu3+) metal—organic framework multicolor heterostructures. The spatial colors could be precisely controlled by thermally manipulating the energy-transfer process between the two lanthanides, thus achieving responsive covert photonic barcodes. Also demonstrated is that spatially resolved responsive barcodes with multi-responsive features could be created in a single heterostructure. These findings offer unique opportunities to purposely design highly integrated responsive microstructures and smart devices toward advanced anti-counterfeiting applications. 相似文献
997.
998.
Yiyi Ou Dr. Weijie Zhou Dr. Zece Zhu Dr. Fengkai Ma Dr. Rongfu Zhou Fang Su Dr. Lirong Zheng Prof. Li Ma Prof. Hongbin Liang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(52):24018-24024
Optical multiplexing based on luminescent materials with tunable color/lifetime has potential applications in information storage and security. However, the available tunable luminescent materials reported so far still suffer from several drawbacks of low efficiency or poor stability, thus restraining their further applications. Herein, we demonstrate a strategy to develop efficient and stable lanthanide coordination polymers (LCPs) with tunable luminescence as a new option for optical multiplexing. Their multicolor emission from green to red and naked-eye-sensitive green emission with tunable lifetime (from ca. 300 to ca. 600 μs) can be controlled by host differential sensitization and energy transfer between lanthanide ions. The quantum efficiencies of developed samples range from around 20 % to 46 % and the luminescence intensity/lifetime appear quite stable in polar solvents up to ten weeks. Furthermore, with the aid of inkjet printing and concepts of luminescence lifetime imaging and time-gated imaging, we illustrate their promising applications of information storage and security in spatial and temporal domains. 相似文献
999.
We present a new size-modified Poisson–Boltzmann ion channel (SMPBIC) model and use it to calculate the electrostatic potential, ionic concentrations, and electrostatic solvation free energy for a voltage-dependent anion channel (VDAC) on a biological membrane in a solution mixture of multiple ionic species. In particular, the new SMPBIC model adopts a membrane surface charge density and a natural Neumann boundary condition to reflect the charge effect of the membrane on the electrostatics of VDAC. To avoid the singularity difficulties caused by the atomic charges of VDAC, the new SMPBIC model is split into three submodels such that the solution of one of the submodels is obtained analytically and contains all the singularity points of the SMPBIC model. The other two submodels are then solved numerically much more efficiently than the original SMPBIC model. As an application of this SMPBIC submodel partitioning scheme, we derive a new formula for computing the electrostatic solvation free energy. Numerical results for a human VDAC isoform 1 (hVDAC1) in three different salt solutions, each with up to five different ionic species, confirm the significant effects of membrane surface charges on both the electrostatics and ionic concentrations. The results also show that the new SMPBIC model can describe well the anion selectivity property of hVDAC1, and that the new electrostatic solvation free energy formula can significantly improve the accuracy of the currently used formula. © 2019 Wiley Periodicals, Inc. 相似文献
1000.
Atomic-level studies of protein activity represent a significant challenge as a result of the complexity of conformational changes occurring on wide-ranging timescales, often greatly exceeding that of even the longest simulations. A prime example is the elucidation of protein allosteric mechanisms, where localized perturbations transmit throughout a large macromolecule to generate a response signal. For example, the conversion of chemical to electrical signals during synaptic neurotransmission in the brain is achieved by specialized membrane proteins called pentameric ligand-gated ion channels. Here, the binding of a neurotransmitter results in a global conformational change to open an ion-conducting pore across the nerve cell membrane. X-ray crystallography has produced static structures of the open and closed states of the proton-gated GLIC pentameric ligand-gated ion channel protein, allowing for atomistic simulations that can uncover changes related to activation. We discuss a range of enhanced sampling approaches that could be used to explore activation mechanisms. In particular, we describe recent application of an atomistic string method, based on Roux's “swarms of trajectories” approach, to elucidate the sequence and interdependence of conformational changes during activation. We illustrate how this can be combined with transition analysis and Brownian dynamics to extract thermodynamic and kinetic information, leading to understanding of what controls ion channel function. © 2019 Wiley Periodicals, Inc. 相似文献