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971.
Xuemei Ma Dr. Hongwei Fu Jingyi Shen Dr. Dianwei Zhang Dr. Jiawan Zhou Prof. Chunyi Tong Prof. Apparao M. Rao Prof. Jiang Zhou Prof. Ling Fan Prof. Bingan Lu 《Angewandte Chemie (International ed. in English)》2023,62(49):e202312973
Ether-based electrolytes are promising for secondary batteries due to their good compatibility with alkali metal anodes and high ionic conductivity. However, they suffer from poor oxidative stability and high toxicity, leading to severe electrolyte decomposition at high voltage and biosafety/environmental concerns when electrolyte leakage occurs. Here, we report a green ether solvent through a rational design of carbon-chain regulation to elicit steric hindrance, such a structure significantly reducing the solvent‘s biotoxicity and tuning the solvation structure of electrolytes. Notably, our solvent design is versatile, and an anion-dominated solvation structure is favored, facilitating a stable interphase formation on both the anode and cathode in potassium-ion batteries. Remarkably, the green ether-based electrolyte demonstrates excellent compatibility with K metal and graphite anode and a 4.2 V high-voltage cathode (200 cycles with average Coulombic efficiency of 99.64 %). This work points to a promising path toward the molecular design of green ether-based electrolytes for practical high-voltage potassium-ion batteries and other rechargeable batteries. 相似文献
972.
Songshan Bi Huimin Wang Yanyu Zhang Min Yang Qingjie Li Jinlei Tian Prof. Zhiqiang Niu 《Angewandte Chemie (International ed. in English)》2023,62(49):e202312982
Iodine (I2) shows great promising as the active material in aqueous batteries due to its distinctive merits of high abundance in ocean and low cost. However, in conventional aqueous I2-based batteries, the energy storage mechanism of I−/I2 conversion is only two-electron redox reaction, limiting their energy density. Herein, six-electron redox chemistry of I2 electrodes is achieved via the synergistic effect of redox-ion charge-carriers and halide ions in electrolytes. The redox-active Cu2+ ions in electrolytes induce the conversion between Cu2+ ions and I2 to CuI at low potential. Simultaneously, the Cl− ions in electrolytes activate the I2/ICl redox couple at high potential. As a result, in our case, I2-based battery system with six-electron redox is developed. Such energy storage mechanism with six-electron redox leads to high discharge potential and capacity, excellent rate capability, as well as stable cycling behavior of I2 electrodes. Impressively, six-electron-redox I2 cathodes can match various aqueous metal (e.g. Zn, Mn and Fe) anodes to construct metal||I2 hybrid batteries. These hybrid batteries not only deliver enhanced capacities, but also exhibit higher operate voltages, which contributes to superior energy densities. Therefore, this work broadens the horizon for the design of high-energy aqueous I2-based batteries. 相似文献
973.
Dr. Chunlei Jiang Jiaxiao Yan Doufeng Wang Kunye Yan Lei Shi Yongping Zheng Chengde Xie Prof. Hui-Ming Cheng Prof. Yongbing Tang 《Angewandte Chemie (International ed. in English)》2023,62(51):e202314509
The pulverization of alloying anodes significantly restricts their use in lithium-ion batteries (LIBs). This study presents a dual-phase solid electrolyte interphase (SEI) design that incorporates finely dispersed Al nanoparticles within the LiPON matrix. This distinctive dual-phase structure imparts high stiffness and toughness to the integrated SEI film. In comparison to single-phase LiPON film, the optimized Al/LiPON dual-phase SEI film demonstrates a remarkable increase in fracture toughness by 317.8 %, while maintaining stiffness, achieved through the substantial dissipation of strain energy. Application of the dual-phase SEI film on an Al anode leads to a 450 % enhancement in cycling stability for lithium storage in dual-ion batteries. A similar enhancement in cycling stability for silicon anodes, which face severe volume expansion issues, is also observed, demonstrating the broad applicability of the dual-phase SEI design. Specifically, homogeneous Li−Al alloying has been observed in conventional LIBs, even when paired with a high mass loading LiNi0.5Co0.3Mn0.2O2 cathode (7 mg cm−2). The dual-phase SEI film design can also accelerate the diffusion kinetics of Li-ions through interface electronic structure regulation. This dual-phase design can integrate stiffness and toughness into a single SEI film, providing a pathway to enhance both the structural stability and rate capability of alloying anodes. 相似文献
974.
Titi Li Sanlue Hu Chenggang Wang Dun Wang Minwei Xu Caiyun Chang Xijin Xu Cuiping Han 《Angewandte Chemie (International ed. in English)》2023,62(51):e202314883
The high thermodynamic instability and side reactions of Zn-metal anode (ZMA), especially at high current densities, greatly impede the commercialization of aqueous zinc-ion batteries (AZIBs). Herein, a fluorine-rich double protective layer strategy is proposed to obtain the high reversibility of AZIBs through the introduction of a versatile tetradecafluorononane-1,9-diol (TDFND) additive in aqueous electrolyte. TDFND molecule with large adsorption energy (−1.51 eV) preferentially absorbs on the Zn anode surface to form a Zn(OR)2− (R=−CH2−(CF2)7−CH2−) cross-linking complex network, which balances space electric field and controls the Zn2+ ion flux, thus enabling the uniform and compact deposition of Zn (002) crystal planes. Meanwhile, TDFND with low Lowest unoccupied molecular orbital (LUMO, 0.10 eV) energy level is priorly decomposed to regulate the interfacial chemistry of ZMA by building a ZnF2-rich solid electrode/electrolyte interface (SEI) layer. It is found that a 14 nm-thick SEI layer delivers excellent structural integrity to suppress parasitic reactions by blocking the direct contact of active water and ZMA. Consequently, the Zn electrode exhibits a superior cycling life over 430 h at 10 mA cm−2 and a high average Coulombic efficiency of 99.8 % at 5 mA cm−2. Furthermore, a 68 mAh pouch cell delivers 80.3 % capacity retention for 1000 cycles. 相似文献
975.
Taoyi Kong Jun Liu Xing Zhou Dr. Jie Xu Yihua Xie Jiawei Chen Prof. Xianfeng Li Prof. Yonggang Wang 《Angewandte Chemie (International ed. in English)》2023,62(6):e202214819
As a green route for large-scale energy storage, aqueous organic redox flow batteries (AORFBs) are attracting extensive attention. However, most of the reported AORFBs were operated in an inert atmosphere. Herein, we clarify this issue by using the reported AORFB (i.e., 3, 3′-(9,10-anthraquinone-diyl)bis(3-methylbutanoicacid) (DPivOHAQ)||Ferrocyanide) as an example. We demonstrate that the dissolved O2 can oxidize the discharged DPivOHAQ in anolyte, leading to capacity-imbalance between anolyte and catholyte. Therefore, this cell shows continuous capacity fading when operated in an air atmosphere. We propose a simple strategy for this challenge, in which the oxygen evolution reaction (OER) in catholyte is employed to balance oxygen reduction reaction (ORR) in anolyte. When using the Ni(OH)2-modifed carbon felt (CF) as a current collector for catholyte, this cell shows an excellent stability in air atmosphere because the Ni(OH)2-induced OER capacity in catholyte exactly balances the ORR capacity in anolyte. Such O2-balance strategy facilitates AORFBs’ practical application. 相似文献
976.
Hong Zhang Bin Song Weiwei Zhang Bowen An Lin Fu Songtao Lu Yingwen Cheng Qianwang Chen Ke Lu 《Angewandte Chemie (International ed. in English)》2023,62(6):e202217009
The sluggish polysulfide redox kinetics and the uncontrollable sulfur speciation pathway, leading to serious shuttling effect and high activation barrier associated with sulfur cathode. We describe here the use of core–shell structured composite matrixes containing abundant catalytic sites for nearly fully reversible cycling of sulfur cathodes for Na-S batteries. The bidirectional tandem electrocatalysis provide successive reversible conversion of both long- and short-chain polysulfides, whereas Fe2O3 accelerates Na2S8/Na2S6 to Na2S4 conversion and the redox-active Fe(CN)64−-doped polypyrrole shell catalyzes Na2S4 reduction to Na2S. The electrochemically reactive Na2S can be readily charged back to sulfur with minimal overpotential. Simultaneously, stable cycling of Na-S pouch cell with a high reversible capacity of 696 mAh g−1 is also demonstrated. The bidirectional confined tandem catalysis renders the manipulation of sulfur redox electrochemistry for practical Na-S cells. 相似文献
977.
Junfei Zhang Yunling Wu Miao Liu Lu Huang Yanguang Li Yingpeng Wu 《Angewandte Chemie (International ed. in English)》2023,62(8):e202215408
Aluminum-ion batteries (AIBs) have attracted great attentions in recent years. Organic materials such as polythiophene (PT) are promising cathode for AIBs. However, the capacity and cyclic stability of conventional organic cathode such as PT are limited by the inadequate degree of reaction and the unstable nature of organic materials. To obtain high-performance organic cathode, a new PT with the ability of self-adaptive re-organization was prepared. During cycling, its molecular chain can be re-organized, and the polymerization mode will change from Cα−Cα (α-PT) to Cβ−Cβ (β-PT). This change leads to smaller steric hindrance and faster kinetics during ion insertion which can lower the reaction energy barrier and stabilize the molecular structure. Benefited by this, AIBs with this cathode can deliver a specific capacity of 180 mAh g−1 (@2 A g−1) and a superb stability of 100 000 cycles at 10 A g−1. High energy density and power density can also be achieved with this cathode. 相似文献
978.
Tingting Lv Dr. Guoyin Zhu Dr. Shengyang Dong Prof. Qingquan Kong Yi Peng Shu Jiang Guangxun Zhang Zilin Yang Prof. Shengyang Yang Prof. Xiaochen Dong Prof. Huan Pang Prof. Yizhou Zhang 《Angewandte Chemie (International ed. in English)》2023,62(5):e202216089
Vanadium-based oxides with high theoretical specific capacities and open crystal structures are promising cathodes for aqueous zinc-ion batteries (AZIBs). In this work, the confined synthesis can insert metal ions into the interlayer spacing of layered vanadium oxide nanobelts without changing the original morphology. Furthermore, we obtain a series of nanomaterials based on metal-confined nanobelts, and describe the effect of interlayer spacing on the electrochemical performance. The electrochemical properties of the obtained Al2.65V6O13 ⋅ 2.07H2O as cathodes for AZIBs are remarkably improved with a high initial capacity of 571.7 mAh ⋅ g−1 at 1.0 A g−1. Even at a high current density of 5.0 A g−1, the initial capacity can still reach 205.7 mAh g−1, with a high capacity retention of 89.2 % after 2000 cycles. This study demonstrates that nanobelts confined with metal ions can significantly improve energy storage applications, revealing new avenues for enhancing the electrochemical performance of AZIBs. 相似文献
979.
Xiaoyu Luan Dr. Lu Qi Zhiqiang Zheng Yaqi Gao Prof. Yurui Xue Prof. Yuliang Li 《Angewandte Chemie (International ed. in English)》2023,62(8):e202215968
Rechargeable aqueous zinc ion batteries (AZIBs) promise high energy density, low redox potential, low cost and safety; however, their cycle performances are seriously insufficient to restrict the progress in this field. We propose a new concept of atomic electrode formed on the graphdiyne (GDY). This new idea electrode was synthesized by selectively, uniformly, and stably anchoring Zn atoms on GDY at the beginning of plating. The Zn atoms are induced to grow into larger size Zn clusters, which continue to grow into nanoflat. Finally, a new heterojunction interface is formed on GDY without any Zn dendrites and side reactions, even at high current densities. Such stepwise induction of growth greatly suppresses the formation of Zn dendrites, resulting in high electroplating/stripping reversibility and lifespan of AZIBs. 相似文献
980.
Dr. Can Guo Jie Zhou Yuting Chen Huifen Zhuang Jie Li Jianlin Huang Yuluan Zhang Prof. Yifa Chen Prof. Shun-Li Li Prof. Ya-Qian Lan 《Angewandte Chemie (International ed. in English)》2023,62(11):e202300125
The inhomogeneous consumption of anions and direct contact between electrolyte and anode during the Zn-deposition process generate Zn-dendrites and side reactions that can aggravate the space-charge effect to hinder the practical implementation of zinc-metal batteries (ZMBs). Herein, electrospray has been applied for the scalable fabrication (>10 000 cm2 in a batch-experiment) of hetero-metallic cluster covalent-organic-frameworks (MCOF-Ti6Cu3) nanosheet-coating (MNC) with integrated micro space electrostatic field for ZMBs anode protection. The MNC@Zn symmetric cell presents ultralow overpotential (≈72.8 mV) over 10 000 cycles at 1 mAh cm−2 with 20 mA cm−2, which is superior to bare Zn and state-of-the-art porous crystalline materials. Theoretical calculations reveal that MNC with integrated micro space electrostatic field can facilitate the deposition-kinetic and homogenize the electric field of anode to significantly promote the lifespan of ZMBs. 相似文献