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“Facial-Mask” Technology for More Efficient Batteries

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“Facial-Mask” Technology for More Efficient Batteries
  • Author(s)

    Nae-Lih Wu
  • Biography

    Dr. Nae-Lih Wu is a Distinguished Professor in the Chemical Engineering Department at National Taiwan University (NTU). His research interests include materials for electrochemical energy-storage devices, including supercapacitors and rechargeable batteries, advanced in-situ/in-operando synchrotron analytic methodologies, and nano-materials synthesis and applications. He is currently an associate editor of Journal of the Electrochemical Society.

  • Academy/University/Organization

    National Taiwan University
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 A low-cost and high-capacity battery system for energy storage is crucial to the development of the green energy industry. Lithium-ion batteries are foreseen to be the major battery technology for the next decades. Although the theoretical charge-storage capacity of a battery is determined by the bulk properties of its electrode active materials, its various practical performance indices, such as practical capacity, charge-discharge rate capability, and cycle stability and safety, heavily depend on the properties of the electrolyte-active material interface. To tailor the interface with beneficial properties, we have been promoting the concept of applying a pre-coating of polymeric soft materials with designed functional groups onto the surfaces of the active materials. In a way, the coatings behave like cosmetic facial-masks to “condition” the properties of the surfaces of the electrode active materials. As an example, we have recently successfully fabricated an ultrathin ( ≦ 100 nm) “facial-mask” on a high-capacity Li anode to effectively suppress dendrite formation and enable extended charge-discharge life with high efficiency. The coating is an organic-inorganic composite ionomer membrane that expels anions in the electrolyte and allows only Li ions to pass through. The Li-ion-selective property of the “facial-mask” helps to evenly distribute Li ions over the entire electrode surface so that formation of dendrite can be avoided. Meanwhile, the organic polymer matrix possesses the high mechanical strength and dimensional rigidity needed for long-life operation. This invention paves the way toward the realization of Li-metal anode technology for advanced high-capacity Li-ion batteries.


In view of the impact of global warming on the environment, the green energy industry has been listed as a key industry for future development around the world. For renewable energy sources, such as solar energy and wind power, the most important part in the development of the power generation systems is the availability of a low-cost and high-capacity battery system for energy storage. Meanwhile, the key to the success of the electric vehicle industry also relies on the development of battery technology. Lithium-ion batteries are foreseen to be the major battery technology for the next decades. Effectively enhancing the performance of battery materials of lithium-ion batteries can certainly boost the future development of green energy technology.

Li-ion batteries consist of positive and negative electrodes that can accommodate Li ions in different energy states (Figure 1). Li ions shuttle between the two electrodes during charge and discharge to store or release electric currents, respectively. Although the theoretical charge-storage capacity of a battery is determined by the bulk properties of its electrode active materials, the various practical performance indices, such as practical capacity, charge-discharge rate capability, cycle stability and safety of the battery, heavily depend on the conditions of the interfaces between the electrolyte and the active materials. In the traditional method for modifying the interface properties for better battery performance, chemical additives are introduced into the electrolyte, where they undergo redox reactions and form coatings on the active material surfaces upon charge/discharge of a battery. However, the composition and structure of such an interfacial coating is determined by very complex and very often unpredictable relations among the additives, parent electrolyte, and charge-discharge protocols. The additives may not be sustainable but are consumed during the course of battery operation. In 2015 we proposed a new approach where polymeric soft coatings with tailored functional groups are applied to the surfaces of the active materials before they are subjected to electrode manufacturing. The compositions and structures of the coatings can be pre-designed with oriented function(s) for each of its components. In a way, the coatings may behave like cosmetic facial-masks to “condition” the properties of the active-material surfaces. The pre-design concept enables the selection of a wide variety of chemical compositions containing different combinations of organic and inorganic materials. 

Figure 1. Schematic diagram showing the working principle of a Lithium-ion battery.
Figure 1. Schematic diagram showing the working principle of a Lithium-ion battery.
 
The state-of-the-art commercial Li-ion batteries use graphite as the negative (anode) electrode. There is a current research trend of exploring high-capacity negative electrode points for the replacement of graphite with Li metal, providing more than four-fold enhancement in charge-storage capacity. However, the Li metal anode suffers from dendrite formation upon lithiation and low coulombic efficiency, which is defined as the ratio between the discharge and charge capacities. Li dendrite formation during battery operation could lead to short-circuit and hazards such as fire and explosion. In tackling these critical issues for Li-metal anodes, our research team successfully fabricated an ultrathin ( ≦ 100 nm) “facial-mask” for Li anodes which effectively suppressed Li dendrite formation and enabled extended charge/discharge cycles with high coulombic efficiency. The coating, referred to as SPEEK-Li/POSS (Figure 2), is an ionomer membrane composed of Li-exchanged sulfonated polyether ether ketone (SPEEK-Li) embedded with a polyhedral oligosilsesquioxane (POSS). SPEEK-Li possesses high mechanical strength and dimensional rigidity needed for long-life operation. Furthermore, the negatively charged sulfonate function groups of the polymer expel anions in the electrolyte and only allow Li ions to pass through. The Li-ion-selective property of the “facial-mask” helps to evenly distribute Li ions over the entire electrode surface so that dendrite formation can be avoided. The cage-like POSS inorganic fillers are uniformly distributed within the POSS-Li matrix, and substantially enhance the ductility of the polymer matrix. This cation-selective “facial-mask” enables the formation of a dendrite-free uniform Li metal layer on a current collector (copper) with high capacity reversibility and excellent long-term cycling stability even for high Li plating capacity. The potential of this technology for practical applications has also been demonstrated by the operation of a battery consisting of a commercial LiFePO4 positive electrode and a SPEEK-Li/POSS coated Li-thin film negative electrode. The invention paves the way to the realization of Li-metal anode technology for advanced Li-ion batteries.
 
Figure 2. Schematic diagram showing the molecular design of an ultra-thin (<100 nm) organic-inorganic
Figure 2. Schematic diagram showing the molecular design of an ultra-thin (<100 nm) organic-inorganic "facial-mask" for lithium metal anodes to suppress lithium dendrites. (Source: “An Ultrathin Ionomer Interphase for High-Efficiency Li Anode in Carbonate-Based Electrolyte”, Nature Communications 10 (2019) 5824 (https://doi.org/10.1038/s41467-019-13783-1).)
 
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