Among various energy storage and conversion materials, functionalized natural clays display significant potentials as electrodes, electrolytes, separators, and nanofillers in energy storage and conversion devices. Natural clays have porous structures, tunable specific surface areas, remarkable thermal and mechanical stabilities, abundant reserves, and cost-effectiveness. In addition, natural clays deliver the advantages of high ionic conductivity and hydrophilicity, which are beneficial properties for solid-state electrolytes. This review article provides an overview toward the recent advancements in natural clay-based energy materials. First, it comprehensively summarizes the structure, classification, and chemical modification methods of natural clays to make them suitable in energy storage and conversion devices. Then, the particular attention is focused on the application of clays in the fields of lithium-ion batteries, lithium-sulfur batteries, zinc-ion batteries, chloride-ion batteries, supercapacitors, solar cells, and fuel cells. Finally, the possible future research directions are provided for natural clays as energy materials. This review aims at facilitating the rapid developments of natural clay-based energy materials through a fruitful discussion from inorganic and materials chemistry aspects, and also promotes the broad sphere of clay-based materials for other utilization, such as effluent treatment, heavy metal removal, and environmental remediation.

Natural Clay-Based Materials for Energy Storage and Conversion Applications.

Si/C composite embedded nano-Si in 3D porous carbon matrix and enwound by conductive CNTs as anode of lithium-ion batteries

The lithium dendrite issue is a major bottleneck that limits the utilization of lithium metal anodes in high‐energy rechargeable batteries. From the perspective of the dendrite nucleation mechanism, this work develops a new type of cation‐selective (CS) separator with anion immobilization behavior to boost the lithium metal anode. By taking advantage of the poly(vinylidene fluoride) matrix, a strong binding force with anions contributes to an excellent CS property of the separator, which is further confirmed by molecular dynamics simulations. The CS separator developed in this work presents a high lithium‐ion transference number up to 0.81. Considering such a dramatically reduced transference number of anions, it can prolong the nucleation time of lithium dendrite and thus achieve a high‐stable Li plating/stripping cycling for 1000 h at a high applied current density of 3 mA cm−2. The Li metal stabilization function of the CS separator is further studied in detail through both in‐situ and ex‐situ observations of dendrites growth. When integrating into lithium metal batteries (LMBs), the CS separators also contribute to enhanced electrochemical performances including discharge capacity, rate capability, and cycling durability. This work is anticipated to provide considerable insight for the creative design of CS separators toward dendrite‐free LMBs.

Anion Immobilization Enabled by Cation‐Selective Separators for Dendrite‐Free Lithium Metal Batteries

Multifunctional separators for high-performance lithium ion batteries

Silicon, which has been widely studied by virtue of its extremely high theoretical capacity and abundance, is recognized as one of the most promising anode materials for the next generation of lithium-ion batteries. However, silicon undergoes tremendous volume change during cycling, which leads to the destruction of the electrode structure and irreversible capacity loss, so the promotion of silicon materials in commercial applications is greatly hampered. In recent years, many strategies have been proposed to address these shortcomings of silicon. This Review focused on different coatings materials (e. g., carbon-based materials, metals, oxides, conducting polymers, etc.) for silicon materials. The role of different types of materials in the modification of silicon-based material encapsulation structure was reviewed to confirm the feasibility of the protective layer strategy. Finally, the future research direction of the silicon-based material coating structure design for the next-generation lithium-ion battery was summarized.

Research Progress on Coating Structure of Silicon Anode Materials for Lithium-Ion Batteries

In this study, a composite separator was prepared by coating a diatomite/polyvinylidene fluoride (PVDF) mixed slurry on the polyethylene terephthalate (PET) nonwoven in order to apply to lithium-ion batteries. The effect of the mass ratio of diatomite/PVDF on the physical and electrochemical performance of the composite separators was investigated. SEM observation showed that the unique pores on the diatomite disk gradually became the main pores of the diatomite/PET composite separator with the increasing content of diatomite in the coating. As the content of diatomite in the diatomite/PET composite separator coating increased from 60 to 80 wt%, the porosity, liquid electrolyte absorption rate, and ionic conductivity gradually increased and reached a maximum (63.8%, 0.866 g cm−3, 1.43 mS cm−1, respectively) at the content of 80 wt%. The contact angle of the composite separators to the electrolyte gradually decreased as the content of diatomite increased and reached a minimum of 13.00° at 80 wt%. After heat treatment at 160 °C for 0.5 h, the composite separator with a diatomite content of 80 wt% shrank merely 1.17% that showed the outstanding thermal stability than the PP separator (39.60%). Furthermore the cells assembled with diatomite composite separators showed better cycle stability and C-rate performance at room temperature, which was related to the reduced interfacial resistance and decreased polarization voltage of the cells. Among them, the composite separator with diatomite/PVDF = 80/20 (w/w) showed the most excellent cell performance due to the unique pore structure of diatomite.

Fabrication of diatomite/polyethylene terephthalate composite separator for lithium-ion battery

In this study, a novel composite separator for rechargeable hybrid aqueous batteries is successfully fabricated by coating porous expanded dickite aqueous slurry using polyacrylic latex as the binder on ES (Ethylene-Propylene Side By Side) nonwoven. The porous expanded dickite is prepared by intercalation and violent chemical reaction, forming porous structure with pore size of 0.3–1.2 μm. The porous morphology of the composite separators could be fine-tuned by varying the content of expanded dickite. The air permeability, porosity, electrolyte uptake, and ionic conductivity of the composite separators gradually improve with the increase of the content of expanded dickite. The improved performance of composite separators helps to improve battery performance, especially at high expanded dickite content. The composite separators with 90 wt.% expanded dickite provide superior cell performance owing to well-tailored pore structure, as compared to a commercialized absorbed glass mat (AGM).

An expanded clay-coated separator with unique microporous structure for enhancing electrochemical performance of rechargeable hybrid aqueous batteries

The invention relates to a diatomite separator for a lithium ion battery and a preparation method of the diatomite separator and belongs to the field of separator materials. According to the method, on the basis of characteristics of submicron through-hole structure and rich surface functional groups of diatomite, diatomite is combined with an organic binding agent, and the composite separator with diatomite as a main body is prepared accordingly. The separator is high in porosity and large in pore size, has good affinity and liquid holding property for electrolyte when used as the lithium ionbattery separator, and can improve conductivity of lithium ions, so that cycling stability of the lithium ion battery in a high current charge-discharge process is improved. Besides, in order to enhance mechanical performance of the separator, basalt chopped fiber is taken as a reinforcing material in a preparation process, and therefore, the separator has better mechanical strength and flexibility and meets assembling and using requirements of the battery. The preparation method is simple, raw material cost is low, the requirement for equipment is not high, and the separator has stronger market competitiveness.

Diatomite separator for lithium ion battery and preparation method of diatomite separator

The invention relates to a diatomaceous earth-coated non-woven fabric lithium ion battery diaphragm and a preparation method therefor, and belongs to the field of a diaphragm material. According to the method, a uniform macroporous structure is established on the surface of a non-woven fabric base film based on the diatomaceous earth porous characteristic, so that porosity of the diaphragm is improved, and electrolyte affinity and electrolyte holding property of the diaphragm can be promoted, and the cycle stability in the high-current charging and discharging process of the lithium ion battery can be improved. The preparation method of the diatomaceous earth-coated non-woven fabric diaphragm mainly comprises the two steps of preparing paste (coating paste) by mixing of diatomaceous earth,a binder, a solvent, a modifier and a defoaming agent, and uniformly coating the two surfaces of the non-woven fabric with the paste. The prepared diatomaceous earth-coated non-woven fabric diaphragmhas relatively high lyophilic property, ventilation, and relatively high porosity, thermal stability and ionic conductivity, and is capable of effectively maintaining the cycle stability in the high-current charging and discharging process of the lithium ion battery; and in addition, the preparation method disclosed in the invention is simple, not high in equipment requirement, relatively low inraw material cost and relatively high in market competitiveness.

Diatomaceous earth-coated non-woven fabric lithium ion battery diaphragm and preparation method therefor

The invention relates to a porous dickite coated non-woven lithium ion battery diaphragm and a preparation method thereof, and belongs to the field of diaphragm materials. The method is as follows: firstly preparing porous dickite powder having through pores and a pore size in the range of 0.1 to 1 mu m, using the powder as a coating material to mixing with a binder, a modifier and water to prepare coating slurry, and coating the surface of a PET nonwoven fabric with the coating slurry by a dipping method to form a lithium ion battery composite diaphragm. The method utilizes the unique pore structure feature of porous dickite to construct a uniform macroporous structure on the surface of a PET non-woven fabric substrate, thereby improving the porosity of the diaphragm; by use of good affinity of the surface functional group of the dickite to an electrolyte, the electrolyte wettability of the composite membrane is improved, the internal resistance of a battery is reduced, and the chargeand discharge cycle stability of the lithium ion battery can be improved. The preparation method has simple preparation method, low equipment requirement, low raw material cost and strong market competitiveness.

Porous dickite coated non-woven lithium ion battery diaphragm and preparation method thereof

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