Increasing interest in flexible/wearable electronics, clean energy, electrical vehicles, and so forth is calling for advanced energy‐storage devices, such as high‐performance lithium‐ion batteries (LIBs), which can not only store energy efficiently and safely, but also possess additional properties, such as good mechanical properties to bear deformations or even to be used as structural components. These expectations first indicate the directions, but also raise new challenges for the advancement of energy materials. As one of the critical components in LIBs, the electrolyte connecting the two electrodes is vital for achieving the desired performances in batteries. In this Review, the developments of various liquid electrolytes (organic, ionic liquid, and aqueous electrolytes), solid electrolytes (solid polymer and inorganic solid), as well as gel electrolytes is briefly summarized and discussed. For each type of electrolyte, the challenging issues and possible solutions are discussed. In particular, safety, ionic conductivity, and contact/interface issues are emphasized. Finally, from a composite point of view, strategies for the development of high‐performance electrolytes with all‐round properties are proposed.
Simultaneous achievement of good electrochemical and mechanical properties is crucial for practical applications of solid ion conductors. Conventional polymer conductors suffer from low conductivity, low transference number, and deteriorated mechanical properties with the enhancement of conductivity, resulting from the coupling between ion transport and polymer movement. Here we present a successful fabrication and fundamental understanding of a high performance soy protein-based solid conductor. The conductor shows ionic conductivity of ∼10 S/cm, transference number of 0.94, and modulus of 1 GPa at room temperature, and still remains flexible and easily processable. Molecular simulations indicate that this is due to appropriate manipulation of the protein structures for effective exploitation of protein functional groups. A decoupled transport mechanism, which is able to explain all results, is proposed. The new insights can be utilized to provide guidelines for design, optimization, and fabrication of high performance biosolid conductors.
Polyetherimide (PEI) has excellent mechanical and thermal properties, and exceptional fire resistance. Developing even broader multi-functionality in PEI/carbon nanotube (CNT) composites for industrial applications is an alluring but challenging goal, due to processing difficulties related to the high pressure and temperature needed to achieve effective flow for this polymer, and costly and complex treatments of the CNTs. Here we report the fabrication of PEI nanocomposite films using low-cost commercially functionalized multi-walled carbon nanotubes (MWNTs), and a simple and innovative process, achieving exceptional properties with only 0.5 wt% of MWNTs, including an increase in electrical conductivity of 12 orders of magnitude, accompanied by an unprecedented increase of 86 degrees C in thermal decomposition temperature (higher service temperature). Field emission scanning electron microscopy revealed a high degree of uniform dispersion among the MWNTs, superb polymer-MWNT interaction and formation of a spatially homogeneous nanotube network within the matrix. The enhancement in these properties suggests great potential use for this developed processing approach and the resulting nanocomposites for multi-functional coating or interfacing materials in aerospace and electronic industries.
Developing supermechanically resilient hard carbon materials that can quickly accommodate sodium ions is highly demanded in fabricating durable anodes for wearable sodium‐ion batteries. Here, an interconnected spiral nanofibrous hard carbon fabric with both remarkable resiliency (e.g., recovery rate as high as 1200 mm s−1) and high Young's modulus is reported. The hard carbon nanofabrics are prepared by spinning and then carbonizing the reaction product of polyacrylonitrile and polar molecules (melamine). The resulting unique hard carbon possesses a highly disordered carbonaceous structure with enlarged interlayer spacing contributed from the strong electrostatic repulsion of dense pyrrolic nitrogen atoms. Its excellent resiliency remains after intercalation/deintercalation of sodium ions. The outstanding sodium‐storage performance of the derived anode includes excellent gravimetric capacity, high‐power capability, and long‐term cyclic stability. More significantly, with a high loading mass, the hard carbon anode displays a high‐power capacity (1.05 mAh cm−2 at 2 A g−1) and excellent cyclic stability. This study provides a unique strategy for the design and fabrication of new hard carbon materials for advanced wearable energy storage systems.
The diffusion of polysulfides in lithium-sulfur (Li-S) batteries represents a critical issue deteriorating the electrochemical performance. Here, borrowing the concepts from air filtration, we design and fabricate a protein-based nanofilter for effectively trapping polysulfides but facilitating Li transport. The unique porous structures are formed through a protein-directed self-assembly process, and the surfaces are functionalized by the protein residues. The experiments and molecular simulation results demonstrate that our polysulfide nanofilter can effectively trap the dissolved polysulfides and promote Li transport in Li-S batteries. When the polysulfide nanofilter is added in a Li-S battery, the electrochemical performance of the battery is significantly improved. Moreover, the contribution of the protein nanofilter to the ion transport is further analyzed by correlating filter properties and battery performance. This study is of universal significance for the understanding, design, and fabrication of advanced battery interlayers that can help realize good management of the ion transport inside advanced energy storage devices.
Lithium (Li) dendrites in Li anodes, and dissolution and migration of manganese (Mn) ions in LiMn2O4 (LMO) cathodes, have hampered these extraordinary electrode materials from being efficiently applied in high performance Li batteries. Here, a novel, bifunctional, biobased composite gel polymer electrolyte (c‐GPE) is created to simultaneously deal with the two critical issues. The skeleton of c‐GPE is constructed from a sandwich structure composed of porous polydopamine spheres and two layers of the environmentally friendly soy protein isolate‐based nanofiber membranes, and the carbonized polydopamine spheres are coated without any binder on the surface of the membranes. After a facile and innocuous preparation process, the skeleton material displays excellent thermal stability and good affinity to liquid electrolyte, which endows c‐GPE with significant functions of effective mitigation of the dissolution of Mn ions, and chelation of the fleeing Mn ions, as well as the dramatic suppression of Li dendrite growth. Consequently, the LMO/Li batteries involving c‐GPE show a great improvement in the cycling stability and rate performance compared with those of the cells based on commercial Celgard 2400. This work will be quite promising to meet the distinct requirements from Li batteries and provide a high‐efficiency and safe biobased GPE for next generation energy storage systems.
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