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901.
Dr. Qi Zhang Hui-Ru Zhang Ping-Ao Hu Prof. Yu-Cheng Wu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(65):e202201989
Cobalt chalcogenides CoX2 (X=S, Se, Te) render great performance of lithium-sulfur batteries based on catalytic capacity to alleviate shuttle effect. Given that S/Se/Te belong to the same main group, the outstanding cycling stability delivered by CoTe2 aroused the curiosity about the uniqueness of CoTe2 and intrinsic laws of cobalt chalcogenide. Herein, comprehensive theoretical study delivers new insights into the intrinsic laws of CoX2: the relative vertical distance of two X atomic layers (rather than atom electronegativity) mainly controls adsorption; CoX2 mainly regulates the charging process (rather than discharging process) thus contributes to great cycling stability. On this basis, the advantages of CoTe2 are three-fold: moderate polysulfide adsorption, facile ion transport capacity, and surprisingly great promotion of charging process. It is hope the results will facilitate the development of cobalt chalcogenides, especially tellurides as catalytic material in lithium sulfur batteries. 相似文献
902.
Dechao Zhang Dr. Xijun Xu Prof. Yanlin Qin Prof. Shaomin Ji Prof. Yanping Huo Zhuosen Wang Zhengbo Liu Jiadong Shen Prof. Jun Liu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(8):1720-1736
Conventional lithium-ion batteries, with flammable organic liquid electrolytes, have serious safety problems, which greatly limit their application. All-solid-state batteries (ASSBs) have received extensive attention from large-scale energy-storage fields, such as electric vehicles (EVs) and intelligent power grids, due to their benefits in safety, energy density, and thermostability. As the key component of ASSBs, solid electrolytes determine the properties of ASSBs. In past decades, various kinds of solid electrolytes, such as polymers and inorganic electrolytes, have been explored. Among these candidates, organic–inorganic composite solid electrolytes (CSEs) that integrate the advantages of these two different electrolytes have been regarded as promising electrolytes for high-performance ASSBs, and extensive studies have been carried out. Herein, recent progress in organic–inorganic CSEs is summarized in terms of the inorganic component, electrochemical performance, effects of the inorganic ceramic nanostructure, and ionic conducting mechanism. Finally, the main challenges and perspectives of organic–inorganic CSEs are highlighted for future development. 相似文献
903.
Hari Shankar Parul Bansal Dr. William W. Yu Dr. Prasenjit Kar 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(53):12242-12248
In the literature, lead halide perovskites are very notable for their degradation in the presence of polar solvents, such as water. In contrast, in this research, it is observed that adding a minor amount of water into the precursor solution can improve the stability and photoluminescence quantum yield of CsPbBr3 nanocrystals through a ligand-assisted reprecipitation (LARP) method. In this way, the shape and phase transformation from CsPbBr3 nanoplates to CsPbBr3/Cs4PbBr6 nanorods and Cs4PbBr6 nanowires can be controlled with increasing water content in the precursor solution. Upon adding water up to an ideal amount, CsPbBr3 maintains its phase and nanoplate morphology. The key role of water amount for tuning the crystallinity, stability, morphology, optical properties, and phase transformation of cesium lead halide perovskite nanocrystals will be beneficial in the future commercialization of optoelectronics. 相似文献
904.
905.
Jin Xie Dr. Hong-Jie Peng Yun-Wei Song Dr. Bo-Quan Li Ye Xiao Meng Zhao Dr. Hong Yuan Prof. Jia-Qi Huang Prof. Qiang Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(40):17823-17828
Use of redox mediators (RMs) is an effective strategy to enhance reaction kinetics of multi-electron sulfur electrochemistry. However, the soluble small-molecule RMs usually aggravate the internal shuttle and thus further reduce the battery efficiency and cyclability. A semi-immobilization strategy is now proposed for RM design to effectively regulate the sulfur electrochemistry while circumvent the inherent shuttle issue in a working battery. Small imide molecules as the model RMs were co-polymerized with moderate-chained polyether, rendering a semi-immobilized RM (PIPE) that is spatially restrained yet kinetically active. A small amount of PIPE (5 % in cathode) extended the cyclability of sulfur cathode from 37 to 190 cycles with 80 % capacity retention at 0.5 C. The semi-immobilization strategy helps to understand RM-assisted sulfur electrochemistry in alkali metal batteries and enlightens the chemical design of active additives for advanced electrochemical energy storage devices. 相似文献
906.
Kyungbae Oh Prof. Dr. Kisuk Kang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(42):18615-18620
The successful launch of solid-state batteries relies on the discovery of solid electrolytes with remarkably high ionic conductivity. Extensive efforts have identified several important superionic conductors (SICs) and broadened our understanding of their superionic conductivity. Herein, we propose a new design strategy to facilitate ionic conduction in SICs by planting immobile repulsion centers. Our ab initio molecular dynamics simulations on the model system Na11Sn2PS12 demonstrate that the sodium ionic conductivity can be increased by approximately one order of magnitude by simply doping large Cs ions as repulsion centers in the characteristic vacant site of Na11Sn2PS12. Planting immobile repulsion centers locally induces the formation of high-energy sites, leading to a fast track for ionic conduction owing to the unique interactions among mobile ions in SICs. Seemingly non-intuitive approaches tailor the ionic diffusion by exploiting these immobile repulsion centers. 相似文献
907.
Dr. Dong Luo Xiaokai Ding Dr. Jianming Fan Zuhao Zhang Dr. Peizhi Liu Dr. Xiaohua Yang Prof. Junjie Guo Prof. Shuhui Sun Prof. Zhan Lin 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(51):23261-23266
Low initial Coulombic efficiency (ICE) is an obstacle for practical application of Li-rich Mn-based layered oxides (LLOs), which is closely related with the irreversible oxygen evolution owing to the overoxidized reaction of surface labile oxygen. Here we report a NH4F-assisted surface multicomponent integration technology to accurately control the ICE, by which oxygen vacancies, spinel-layered coherent structure, and F-doping are skillfully integrated on the surface of treated LLOs microspheres. Though the regulation on the removed amount of labile oxygen by surface integrated structure, the ICE of LLOs cathodes can adjust from starting value to 100 %. X-ray absorption spectroscopy, refined X-ray diffraction, and scanning transmission electron microscopy show that the removed labile oxygen mainly comes from Li2MnO3-like structure. Even operating at a high cut-off voltage of 5 V, the capacity retention of integrated sample at 200 mA g−1 is still larger than 98 % after 100 cycles. 相似文献
908.
Dr. Longtao Ma Dr. Shengmei Chen Xinliang Li Ao Chen Dr. Binbin Dong Dr. Chunyi Zhi 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(52):24044-24052
Zn batteries are usually considered as safe aqueous systems that are promising for flexible batteries. On the other hand, any liquids, including water, being encapsulated in a deformable battery may result in problems. Developing completely liquid-free all-solid-state Zn batteries needs high-quality solid-state electrolytes (SSEs). Herein, we demonstrate in situ polymerized amorphous solid poly(1,3-dioxolane) electrolytes, which show high Zn ion conductivity of 19.6 mS cm−1 at room temperature, low interfacial impedance, highly reversible Zn plating/stripping over 1800 h cycles, uniform and dendrite-free Zn deposition, and non-dry properties. The in-plane interdigital-structure device with the electrolyte completely exposed to the open atmosphere can be operated stably for over 30 days almost without weight loss or electrochemical performance decay. Furthermore, the sandwich-structure device can normally operate over 40 min under exposure to fire. Meanwhile, the interfacial impedance and the capacity using in situ-formed solid polymer electrolytes (SPEs) remain almost unchanged after various bending tests, a key criterion for flexible/wearable devices. Our study demonstrates an approach for SSEs that fulfill the requirement of no liquid and mechanical robustness for practical solid-state Zn batteries. 相似文献
909.
Angélica Forgionny Nancy Y. Acelas Carlos Jimenez-Orozco Elizabeth Flórez 《International journal of quantum chemistry》2020,120(15):e26258
A systematic DFT study was performed to evaluate the effect of oxygenated functional groups for Hg2+ adsorption in aqueous systems. This work includes several aspects usually neglected in many current works, namely, ground-state multiplicity, solvation effects, establishment of thermodynamic parameters, atomic charge transfer, and modeling of infrared spectra. In addition, two carbonaceous models were studied to account for both the effect of the carbonaceous matrix and the oxygenated functional groups on the Hg2+ binding. Adsorption energies indicated that Hg2+ adsorption on the unsaturated model is favored in the following order: phenol > lactone > semiquinone > carboxyl, whereas for the saturated model, the Hg2+ adsorption energy decrease order is: carboxyl > semiquinone > lactone. Thermodynamic parameters confirmed that the adsorption process is spontaneous (unsaturated model), while the infrared spectra provided an insight at the atomic level about the experimentally reported bands. Our results contributed to a deeper understanding of the current experimental information on the effect of the surface functional groups on the Hg2+ adsorption over carbonaceous materials as different active sites can be present on oxygenated carbonaceous materials for metal adsorption. The results also create new ways to improve the performance of adsorption capability of mercury and other pollutants. 相似文献