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881.
Pan Yang Dr. Zhenzhen Wu Shouyue Wang Dr. Meng Li Dr. Hao Chen Shangshu Qian Mengting Zheng Prof. Yun Wang Prof. Sheng Li Prof. Jingxia Qiu Prof. Shanqing Zhang 《Angewandte Chemie (International ed. in English)》2023,62(49):e202311460
Organic electrode materials (OEMs), valued for their sustainability and structural tunability, have been attracting increasing attention for wide application in sodium-ion batteries (SIBs) and other rechargeable batteries. However, most OEMs are plagued with insufficient specific capacity or poor cycling stability. Therefore, it′s imperative to enhance their specific capacity and cycling stability through molecular design. Herein, we designed and synthesized a heteroaromatic molecule 2,3,8,9,14,15-hexanol hexaazatrinaphthalene (HATN-6OH) by the synergetic coupling of catechol (the precursor of ortho-quinone)/ortho-quinone functional groups and HATN conjugated core structures. The abundance of catechol/ortho-quinone and imine redox-active moieties delivers a high specific capacity of nine-electron transfer for SIBs. Most notably, the π–π interactions and intermolecular hydrogen bond forces among HATN-6OH molecules secure the stable long-term cycling performance of SIBs. Consequently, the as-prepared HATN-6OH electrode exhibited a high specific capacity (554 mAh g−1 at 0.1 A g−1), excellent rate capability (202 mAh g−1 at 10 A g−1), and stable long-term cycling performance (73 % after 3000 cycles at 10 A g−1) in SIBs. Additionally, the nine-electron transfer mechanism is confirmed by systematic density functional theory (DFT) calculation, attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR), and Raman analysis. The achievement of the synergetic coupling of the redox-active sites on OEMs could be an important key to the enhancement of SIBs and other metal-ion batteries. 相似文献
882.
Haoyu Li Yu Ren Yue Zhu Jiaming Tian Xinyi Sun Chuanchao Sheng Ping He Shaohua Guo Haoshen Zhou 《Angewandte Chemie (International ed. in English)》2023,62(41):e202310143
The moderate reversibility of Zn anodes, as a long-standing challenge in aqueous zinc-ion batteries, promotes the exploration of suitable electrolyte additives continuously. It is crucial to establish the absolute predominance of smooth deposition within multiple interfacial reactions for stable zinc anodes, including suppressing side parasitic reactions and facilitating Zn plating process. Trehalose catches our attention due to the reported mechanisms in sustaining biological stabilization. In this work, the inter-disciplinary application of trehalose is reported in the electrolyte modification for the first time. The pivotal roles of trehalose in suppressed hydrogen evolution and accelerated Zn deposition have been investigated based on the principles of thermodynamics as well as reaction kinetics. The electrodeposit changes from random accumulation of flakes to dense bulk with (002)-plane exposure due to the unlocked crystal-face oriented deposition with trehalose addition. As a result, the highly reversible Zn anode is obtained, exhibiting a high average CE of 99.8 % in the Zn/Cu cell and stable cycling over 1500 h under 9.0 % depth of discharge in the Zn symmetric cell. The designing principles and mechanism analysis in this study could serve as a source of inspiration in exploring novel additives for advanced Zn anodes. 相似文献
883.
Xin-Hai Meng Dr. Xu-Dong Zhang Dr. Hang Sheng Dr. Min Fan Ting Lin Dr. Dongdong Xiao Jianxin Tian Prof. Rui Wen Wen-Zhe Liu Prof. Ji-Lei Shi Prof. Li-Jun Wan Prof. Yu-Guo Guo 《Angewandte Chemie (International ed. in English)》2023,62(22):e202302170
Layered transition metal oxide cathodes have been one of the dominant cathodes for lithium-ion batteries with efficient Li+ intercalation chemistry. However, limited by the weak layered interaction and unstable surface, mechanical and chemical failure plagues their electrochemical performance, especially for Ni-rich cathodes. Here, adopting a simultaneous elemental-structural atomic arrangement control based on the intrinsic Ni−Co−Mn system, the surface role is intensively investigated. Within the invariant oxygen sublattice of the crystal, a robust surface with the synergistic concentration gradient and layered-spinel intertwined structure is constructed on the model single-crystalline Ni-rich cathode. With mechanical strain dissipation and chemical erosion suppression, the cathode exhibits an impressive capacity retention of 82 % even at the harsh 60 °C after 150 cycles at 1 C. This work highlights the coupling effect of structure and composition on the chemical-mechanical properties, and the concept will spur more researches on the cathodes that share the same sublattice. 相似文献
884.
Peng Wang Dr. Qin Xiang Miaoyue Tian Sheng Tao Zhuofan Xu Yupeng Guo Prof. Dr. Wenping Hu Prof. Dr. Zhe Sun 《Angewandte Chemie (International ed. in English)》2023,62(46):e202313257
The synthesis of bench-stable conjugated π-radicals is challenging owing to the lack of modular approaches, which greatly hampers their practical material screens and applications. Here, we demonstrate a spin-distribution-directed regioselective substitution strategy to introduce substituents into the specific positions of an olympicenyl radical in a stepwise manner, resulting in a series of highly stable radical species. The substituents can also adjust the crystal packing by means of steric and electronic factors, enabling the changing from a π-dimer to a pseudo-one-dimensional chain. The first single crystal organic field-effect transistor device based on a graphenic radical is fabricated in air, showing a hole mobility of up to 0.021 cm2 V−1 s−1 and excellent device stability. This approach may be generalized to diverse spin-delocalized open-shell organic radicals. 相似文献
885.
886.
S. J. Cheng W. Sheng P. Hawrylak S. Raymond S. Studenikin A. Sachrajda Z. Wasilewski A. Babinski M. Potemski G. Ortner M. Bayer 《Physica E: Low-dimensional Systems and Nanostructures》2004,21(2-4):211
We present results of calculations and experiments on electron–hole complexes in InGaAs/GaAs self-assembled quantum dots in high magnetic field (B). Due to hidden symmetries, the chemical potential of an N-exciton system at special B fields becomes insensitive to the exciton number as well as the magnetic field. This results in plateau regions of high intensity in measured magneto-PL spectrum. Theoretical calculations using exact diagonalization techniques successfully explain the measured magneto-photoluminescence spectrum with B fields up to 28 T. 相似文献
887.
Zhu?He Zhaohui?LiuEmail author Sheng?Chen Lei?Weng Chuguang?Zheng 《Acta Mechanica Sinica》2005,21(2):112-120
Direct numerical simulations were conducted to investigate the behavior of heavy particles in homogeneous isotropic turbulence. The present study focused on the effect of particle inertia and drift on the autocorrelations of the particle velocity and the fluid seen by particles and the dispersion characteristics of particles. The Lagrangian integral time scale of particles monotonically increased as the magnitude of the particle response time increased, while that of the fluid seen by particles remained relatively constant; it reached a maximum when the particle response time was close to the Kolmolgorov time scale of the flow. Particle dispersion increased as the particle inertia increased for small particles, while for larger particles, it decreased as particle inertia increased; particle eddy diffusion coefficient was maximal, and greater than that of the fluid by about 30%, at the preferential concentration. The concentration field of the particles with τp/τk≈1.0 showed that particles tend to collect in regions of low vorticity (high strain) due to preferential concentration. As the drift velocity of a particle is increased it crosses the paths of fluid elements more rapidly and will tend to lose correlation with its previous velocity faster than a fluid element will. And the correlation of particle velocities along the drift direction is more persistent than that perpendicular to the direction of drift. Simulations also showed that the continuity effect and the crossing-trajectory effect are weakened for particles with infinite inertia. 相似文献
888.
A transparent this film was prepared by depositing the sol-gel mixture for the synthesis of MCM-41 mesoporous molecular sieve doped with rhodamine 6G(R6G) dye on glass substrates. The film of silica-surfactant-R6G materials, which was identified to possess hexagonally ordered mesostructure,was composed of nanocrystallites about 35 nm in diameter and 1-10μm in thickness. Cleanness of the substrates, concentration of the sol-gel mixture and rate of evaporation of the solvent were the key factors affecting transparency and homogeneity of the film. Moreover,optical change and lack in dye aggregation were observed to the R6G-functionalized MCM-41 thin film in contrast with that in ethanol solution. 相似文献
889.
890.
利用密度泛函理论中的B3LYP方法, 选择LANL2DZ基组优化Tin(2~7)团簇得到各团簇的稳定结构,然后对稳定结构的束缚能及自然轨道进行分析. 研究结果表明: Tin(n=2~7)团簇都依带帽的形式在前一个团簇的结构基础上加一个原子变化而来; 通过自然轨道分析发现, 团簇原子的轨道存在sp-d杂化, 有大约一个电子从4s转移到了3d, 原子之间亦存在电子转移, 而且除Ti7外, 团簇键长由最外层4d轨道电子和3d轨道共同决定, 在Ti7中, 团簇键长由3d轨道决定. 相似文献