Yanbao Fu

Multilayer nanoassembly of Sn-nanopillar arrays sandwiched between graphene layers for high-capacity lithium storage

Sn nanopillar arrays embedded between graphene sheets were assembled using a conventional film deposition and annealing process. The as-formed three-dimensional (3D) multilayered nanostructure was directly used as an anode material for rechargeable lithium-ion batteries without adding any polymer binder and carbon black. Electrochemical measurements showed very high reversible capacity and excellent cycling performance at a current density as high as 5 A g−1. These results demonstrated that nanocomposite materials with highly functional 1D and 2D components can be synthesized by employing conventional top-down manufacturing methods and self-assembly principles.

Nonflammable perfluoropolyether-based electrolytes for lithium batteries

Significance This research article describes a unique class of nonflammable electrolytes for lithium-ion batteries that are based on functionalized perfluoropolyethers (PFPEs). It demonstrates that PFPEs may be used as a major component in operating batteries. These electrolytes not only are completely nonflammable, but they also exhibit unprecedented high transference numbers and low electrochemical polarization, indicative of longer battery life. The results in this work may represent a significant step toward a lithium-ion battery with improved safety and pave the way for the development of new electrolytes that can address the persisting challenges of current battery technologies. The flammability of conventional alkyl carbonate electrolytes hinders the integration of large-scale lithium-ion batteries in transportation and grid storage applications. In this study, we have prepared a unique nonflammable electrolyte composed of low molecular weight perfluoropolyethers and bis(trifluoromethane)sulfonimide lithium salt. These electrolytes exhibit thermal stability beyond 200 °C and a remarkably high transference number of at least 0.91 (more than double that of conventional electrolytes). Li/LiNi1/3Co1/3Mn1/3O2 cells made with this electrolyte show good performance in galvanostatic cycling, confirming their potential as rechargeable lithium batteries with enhanced safety and longevity.

Toward practical application of functional conductive polymer binder for a high-energy lithium-ion battery design.

Silicon alloys have the highest specific capacity when used as anode material for lithium-ion batteries; however, the drastic volume change inherent in their use causes formidable challenges toward achieving stable cycling performance. Large quantities of binders and conductive additives are typically necessary to maintain good cell performance. In this report, only 2% (by weight) functional conductive polymer binder without any conductive additives was successfully used with a micron-size silicon monoxide (SiO) anode material, demonstrating stable and high gravimetric capacity (>1000 mAh/g) for ∼500 cycles and more than 90% capacity retention. Prelithiation of this anode using stabilized lithium metal powder (SLMP) improves the first cycle Coulombic efficiency of a SiO/NMC full cell from ∼48% to ∼90%. The combination enables good capacity retention of more than 80% after 100 cycles at C/3 in a lithium-ion full cell.

Rational Design and Facial Synthesis of Li3V2(PO4)3@C Nanocomposites Using Carbon with Different Dimensions for Ultrahigh-Rate Lithium-Ion Batteries

Li3V2(PO4)3 (LVP) particles dispersed in different inorganic carbons (LVP@C) have been successfully synthesized via an in situ synthesis method. The inorganic carbon materials with different dimensions including zero-dimensional Super P (SP) nanospheres, one-dimensional carbon nanotubes (CNTs), two-dimensional graphene nanosheets, and three-dimensional graphite particles. The effects of carbon dimensions on the structure, morphology, and electrochemical performance of LVP@C composites have been systematically investigated. The carbon materials can maintain their original morphology even after oxidation (by NH4VO3) and high-temperature sintering (850 °C). LVP@CNT exhibits the best electrochemical performances among all of the samples. At an ultrahigh discharge rate of 100C, it presents a discharge capacity of 91.94 mAh g(-1) (69.13% of its theoretical capacity) and maintains 79.82% of its original capacity even after 382 cycles. Its excellent electrochemical performance makes LVP@CNT a promising cathode candidate for lithium-ion batteries.

A systematic investigation of polymer binder flexibility on the electrode performance of lithium-ion batteries.

The mechanical failure at the electrode interfaces (laminate/current collector and binder/particle interfaces) leads to particle isolation and delamination, which has been regarded as one of the main reasons for the capacity decay and cell failure of lithium-ion batteries (LIBs). Polymer binder provides the key function for a good interface property and for maintaining the electrode integrity of LIBs. Triethylene glycol monomethyl ether (TEG) moieties were incorporated into polymethacrylic acid (PMAA) to different extents at the molecular level. Microscratch tests of the graphite electrodes based on these binders indicate that the electrode is more flexible with 5 or 10% TEG in the polymer binders. Crack generation is inhibited by the flexible TEG-containing binder, compared to that of the unmodified PMAA-based electrode, leading to the better cycling performance of the flexible electrode. With a 10% TEG moiety in the binder, the graphite half-cell reaches a reversible capacity of >270 mAh/g at the 1C rate, compared to a value of ∼190 mAh/g for the unmodified PMAA binder.

High capacity and high density functional conductive polymer and SiO anode for high-energy lithium-ion batteries.

High capacity and high density functional conductive polymer binder/SiO electrodes are fabricated and calendered to various porosities. The effect of calendering is investigated in the reduction of thickness and porosity, as well as the increase of density. SiO particle size remains unchanged after calendering. When compressed to an appropriate density, an improved cycling performance and increased energy density are shown compared to the uncalendered electrode and overcalendered electrode. The calendered electrode has a high-density of ∼1.2 g/cm(3). A high loading electrode with an areal capacity of ∼3.5 mAh/cm(2) at a C/10 rate is achieved using functional conductive polymer binder and simple and effective calendering method.

Conductive Polymer Binder for High-Tap-Density Nanosilicon Material for Lithium-Ion Battery Negative Electrode Application

High-tap-density silicon nanomaterials are highly desirable as anodes for lithium ion batteries, due to their small surface area and minimum first-cycle loss. However, this material poses formidable challenges to polymeric binder design. Binders adhere on to the small surface area to sustain the drastic volume changes during cycling; also the low porosities and small pore size resulting from this material are detrimental to lithium ion transport. This study introduces a new binder, poly(1-pyrenemethyl methacrylate-co-methacrylic acid) (PPyMAA), for a high-tap-density nanosilicon electrode cycled in a stable manner with a first cycle efficiency of 82%-a value that is further improved to 87% when combined with graphite material. Incorporating the MAA acid functionalities does not change the lowest unoccupied molecular orbital (LUMO) features or lower the adhesion performance of the PPy homopolymer. Our single-molecule force microscopy measurement of PPyMAA reveals similar adhesion strength between polymer binder and anode surface when compared with conventional polymer such as homopolyacrylic acid (PAA), while being electronically conductive. The combined conductivity and adhesion afforded by the MAA and pyrene copolymer results in good cycling performance for the high-tap-density Si electrode.

SBR–PVDF based binder for the application of SLMP in graphite anodes

A styrene butadiene rubber (SBR)–polyvinylidene difluoride (PVDF) based binder system has been developed for an electrochemical system that is not compatible with the conventional N-methyl pyrrolidinone (NMP) solvent used to cast most Li-ion electrode slurries. This polymer systems binding properties decouple the mechanical and ionic-transport properties. It demonstrates comparable mechanical properties to SBR-based electrodes and cell performance to traditional PVDF-based electrodes. This new binder design however enables the incorporation of stabilized lithium metal powder (SLMP) into a graphite anode to improve its first cycle coulombic efficiency.

Biomimetic Ant-Nest Electrode Structures for High Sulfur Ratio Lithium–Sulfur Batteries

The lithium-sulfur (Li-S) rechargeable battery has the benefit of high gravimetric energy density and low cost. Significant research currently focuses on increasing the sulfur loading and sulfur/inactive-materials ratio, to improve life and capacity. Inspired by natures ant-nest structure, this research results in a novel Li-S electrode that is designed to meet both goals. With only three simple manufacturing-friendly steps, which include slurry ball-milling, doctor-blade-based laminate casting, and the use of the sacrificial method with water to dissolve away table salt, the ant-nest design has been successfully recreated in an Li-S electrode. The efficient capabilities of the ant-nest structure are adopted to facilitate fast ion transportation, sustain polysulfide dissolution, and assist efficient precipitation. High cycling stability in the Li-S batteries, for practical applications, has been achieved with up to 3 mg·cm(-2) sulfur loading. Li-S electrodes with up to a 85% sulfur ratio have also been achieved for the efficient design of this novel ant-nest structure.

Fumed Silica-Based Single-Ion Nanocomposite Electrolyte for Lithium Batteries

A composite lithium electrolyte composed of polyelectrolyte-grafted nanoparticles and polyethylene glycol dimethyl ether (PEGDME) is synthesized and characterized. Polyanions immobilized by the silica nanoparticles have reduced anion mobility. Composite nanoparticles grafted by poly(lithium 4-styrenesulfonate) only have moderate conductivity at 60 °C. Almost an order increase of the conductivity to ∼10(-6) S/cm is achieved by co-polymerization of the poly(ethylene oxide) methacrylate with sodium 4-styrenesulfonate, which enhances dissociation between lithium cation and polyanion and facilitates lithium ion transfer from the inner part of the polyelectrolyte layer. This composite electrolyte has the potential to suppress lithium dendrite growth and enable the use of lithium metal anode in rechargeable batteries.