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1. Sulfur impregnation in polypyrrole-modified MnO ₂ nanotubes: efficient polysulfide adsorption for improved lithium–sulfur battery performance

   https://doi.org/10.1039/c8nr10353d  

   Du, Pengcheng ; Wei, Wenli ; Dong, Yuman ; Liu, Dong ; Wang, Qi ; Peng, Yi ; Chen, Shaowei ; Liu, Peng ( May 2019 , Nanoscale)

   Rechargeable lithium–sulfur batteries have emerged as a viable technology for next generation electrochemical energy storage, and the sulfur cathode plays a critical role in determining the device performance. In this study, we prepared functional composites based on polypyrrole-coated MnO 2 nanotubes as a highly efficient sulfur host (sulfur mass loading 63.5%). The hollow interior of the MnO 2 nanotubes not only allowed for accommodation of volumetric changes of sulfur particles during the cycling process, but also confined the diffusion of lithium polysulfides by physical restriction and chemical adsorption, which minimized the loss of polysulfide species. In addition, the polypyrrole outermore »layer effectively enhanced the electrical conductivity of the cathode to facilitate ion and electron transport. The as-prepared MnO 2 -PPy-S composite delivered an initial specific capacity of 1469 mA h g −1 and maintained an extremely stable cycling performance, with a small capacity decay of merely 0.07% per cycle at 0.2C within 500 cycles, a high average coulombic efficiency of 95.7% and an excellent rate capability at 470 mA h g −1 at the current density of 3C.« less
2. In situ synthesis and in operando NMR studies of a high-performance Ni ₅ P ₄ -nanosheet anode

   https://doi.org/10.1039/C8TA05433A  

   Feng, Xuyong ; Tang, Mingxue ; O'Neill, Sean ; Hu, Yan-Yan ( November 2018 , Journal of Materials Chemistry A)

   Nickel phosphide (Ni 5 P 4 ) nanosheets are synthesized using in situ chemical vapor deposition of P on Ni foam. The thickness of the as-synthesized Ni 5 P 4 film is determined to be ∼5 nm, using atomic force microscopy (AFM). The small thickness shortens the diffusion path of Li ions and results in fast ion transport. In addition, the 2D Ni 5 P 4 nanosheets seamlessly connect to the Ni foam, which facilitates electron transfer between Ni 5 P 4 and the Ni current collector. Therefore, the binder/carbon free-nickel supported Ni 5 P 4 shows fast rate performancemore »as an anode for lithium-ion batteries (LIBs). The specific capacity of 2D Ni 5 P 4 is obtained as 600 mA h g −1 at a cycling rate of 0.1C, approaching the theoretical capacity of 768 mA h g −1 . Even at a rate of 0.5C, the capacity remains as 450 mA h g −1 over 100 cycles. A capacity >100 mA h g −1 is retained at a very high rate of 20C. Ni 5 P 4 also exhibits a low voltage of ∼0.5 V with respect to Li metal, which makes it a suitable negative electrode for LIBs. In operando 31 P NMR and 7 Li NMR are employed to probe the lithiation and de-lithiation mechanisms upon electrochemical cycling.« less
3. Facile synthesis of hierarchical MoS ₂ –carbon microspheres as a robust anode for lithium ion batteries

   https://doi.org/10.1039/C6TA03310E  

   Chen, Gen ; Wang, Shengping ; Yi, Ran ; Tan, Longfei ; Li, Hongbo ; Zhou, Meng ; Yan, Litao ; Jiang, Yingbing ; Tan, Shuai ; Wang, Donghai ; et al ( January 2016 , Journal of Materials Chemistry A)

   Molybdenum disulfide (MoS 2 ) may be a promising alternative for lithium ion batteries (LIBs) because it offers a unique layered crystal structure with a large and tunable distance between layers. This enables the anticipated excellent rate and cycling stability because they can promote the reversible lithium ion intercalation and de-intercalation without huge volume change which consequently prevents the pulverization of active materials during repeated charge and discharge processes. Herein, we prepared hierarchical MoS 2 –carbon (MoS 2 –C) microspheres via a continuous and scalable ultrasonic nebulization assisted route. The structure, composition, and electrochemical properties are investigated in detail. Themore »MoS 2 –C microspheres consist of few-layer MoS 2 nanosheets bridged by carbon, which separates the exfoliated MoS 2 layers and prevents their aggregation and restacking, thus leading to improved kinetic, enhanced conductivity and structural integrity. The novel architecture offers additional merits such as overall large size and high packing density, which promotes their practical applications. The MoS 2 –C microspheres have been demonstrated with excellent electrochemical performances in terms of low resistance, high capacity even at large current density, stable cycling performance, etc. The electrodes exhibited 800 mA h g −1 at 1000 mA g −1 over 170 cycles. At a higher current density of 3200 mA g −1 , a capacity of 730 mA h g −1 can be also maintained. The MoS 2 –C microspheres are practically applicable not only because of the continuous and large scale synthesis via the current strategy, but also the possess a robust and integrated architecture which ensures the excellent electrochemical properties.« less
4. Ultrahigh capacity 2D anode materials for lithium/sodium-ion batteries: an entirely planar B ₇ P ₂ monolayer with suitable pore size and distribution

   https://doi.org/10.1039/D0TA02767G  

   Zhu, Changyan ; Lin, Shiru ; Zhang, Min ; Li, Quan ; Su, Zhongmin ; Chen, Zhongfang ( May 2020 , Journal of Materials Chemistry A)

   Lithium-ion batteries (LIBs) are widely used energy storage devices, and sodium-ion batteries (SIBs) are promising alternatives to LIBs because sodium is of high abundance and low toxicity. However, a dominant obstacle for the advancement of LIBs and SIBs is the lack of high capacity anode materials, especially for SIBs. Here, we propose that three characteristics, namely appropriate pore size, suitable pore distribution, and an entirely planar topology, can help achieve ultrahigh capacity 2D anode materials. Under such guidelines, we constructed a B 7 P 2 monolayer, and investigated its potential as a LIB/SIB anode material by means of density functionalmore »theory (DFT) computations. Encouragingly, the B 7 P 2 monolayer possesses all the essential properties of a high-capacity LIB/SIB anode: its high stability ensures the experimental feasibility of synthesis, its metallicity does not change upon Li/Na adsorption and desorption, the Li/Na can well diffuse on the surface, and the open-circuit voltage is in a good range. Most importantly, the B 7 P 2 monolayer has a high storage capacity of 3117 mA h g −1 for both LIBs and SIBs, and this capacity value ranks among the highest for 2D SIB anode materials. This study offers us some good clues to design/discover other anode materials with ultrahigh capacities, and serves us another vivid example that (implicit and hidden) trends/rules in the literature can guide us in the design of functional materials more efficiently.« less
5. Novel Cu(Zn)–Ge–P compounds as advanced anode materials for Li-ion batteries

   https://doi.org/10.1039/d0ee03553j  

   Li, Wenwu ; Shen, Pengfei ; Yang, Lufeng ; Chen, Anjie ; Wang, Jeng-Han ; Li, Yunyong ; Chen, Hailong ; Liu, Meilin ( April 2021 , Energy & Environmental Science)

   Both electronic and ionic conductivities are of high importance to the performance of anode materials for Li-ion batteries. Many large capacity anode materials (such as Ge) do not have sufficiently high electronic and ionic conductivities required for high-rate cycling. Here, we report a novel ternary compound, copper germanium phosphide (CuGe 2 P 3 ), as a high-rate anode. Being synthesized via a facile and scalable mechanochemistry method, CuGe 2 P 3 has a cation-disordered sphalerite structure and offers higher ionic and electronic conductivities and better tolerance to volume change during cycling than Ge, as confirmed by first principles calculations andmore »experimental characterization, including high-resolution synchrotron X-ray diffraction, HRTEM, SAED, XPS and Raman spectroscopy. Furthermore, the results suggest that CuGe 2 P 3 has a reversible Li-storage mechanism of conversion reaction. When composited with graphite by virtue of a two-stage ball-milling process, the yolk–shell structure of the amorphous carbon-coated CuGe 2 P 3 nanocomposite (CuGe 2 P 3 /C@Graphene) delivers a high initial coulombic efficiency (91%), a superior cycling stability (1312 mA h g −1 capacity after 600 cycles at 0.2 A g −1 and 876 mA h g −1 capacity after 1600 cycles at 2 A g −1 ), and an excellent rate capability (386 mA h g −1 capacity at 30 A g −1 ), surpassing most Ge-based anodes reported to date. Moreover, a series of cation-disordered new phases in the Cu(Zn)–Ge–P family with various cation ratios offer similar Li-storage properties, achieving high reversible capacities with high initial coulombic efficiencies and desirable redox chemistry with improved safety.« less