Rechargeable sodium-ion batteries (SIBs) are emerging as a viable alternative to lithium-ion battery (LIB) technology, as their raw materials are economical, geographically abundant (unlike lithium), and less toxic. The matured LIB technology contributes significantly to digital civilization, from mobile electronic devices to zero electric-vehicle emissions. However, with the increasing reliance on renewable energy sources and the anticipated integration of high-energy-density batteries into the grid, concerns have arisen regarding the sustainability of lithium due to its limited availability and consequent price escalations. In this context, SIBs have gained attention as a potential energy storage alternative, benefiting from the abundance of sodium and sharing electrochemical characteristics similar to LIBs. Furthermore, high-entropy chemistry has emerged as a new paradigm, promising to enhance energy density and accelerate advancements in battery technology to meet the growing energy demands. This review uncovers the fundamentals, current progress, and the views on the future of SIB technologies, with a discussion focused on the design of novel materials. The crucial factors, such as morphology, crystal defects, and doping, that can tune electrochemistry, which should inspire young researchers in battery technology to identify and work on challenging research problems, are also reviewed. 

Unleashing the Potential of Sodium‐Ion Batteries: Current State and Future Directions for Sustainable Energy Storage

Removing electrochemical constraints on polytetrafluoroethylene as dry-process binder for high-loading graphite anodes

Lithium-ion batteries (LIBs) have recently become popular for energy storage due to their high energy density, storage capacity, and long-term cycle life. Although binders make up only a small proportion of LIBs, they have become the key to promoting the transformation of the battery preparation process. Along with the development of binders, the battery manufacturing process has evolved from the conventional slurry-casting (SC) process to a more attractive solvent-free (SF) method. Compared with traditional LIBs manufacturing method, the SF method could dramatically reduce and increase the energy density due to the reduced preparation steps and enhanced electrode loading. Polytetrafluoroethylene (PTFE), as a typical binder, has played an important role in fabricating high-performance LIBs, particularly in regards to the SF technique. In this paper, the development history and application status of PTFE binder was introduced, and then its contributions and the inherent problems involved in the SF process were described and analyzed. Finally, the viewpoints concerning the future trends for PTFE-based SF manufacturing methods were also discussed. We hope this work can inspire future research concerning high-quality SF binders and assist in promoting the evolution of the SF manufacturing technology in regards to LIBs.

A Polytetrafluoroethylene-Based Solvent-Free Procedure for the Manufacturing of Lithium-Ion Batteries

Polytetrafluoroethylene (PTFE)-based dry process for lithium-ion batteries is gaining attention as a battery manufacturing scheme can be simplified with drastically reducing environmental damage. However, the electrochemical instability of PTFE in a reducing environment has hampered the realization of the high-performance dry-processed anode. In this study, we present a non-electroconductive and highly ionic-conductive polymer coating on graphite to mitigate the electrochemical degradation of the PTFE binder and minimize the coating resistance. Poly(ethylene oxide) (PEO) and poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE-CFE)) coatings on the anode material effectively inhibit the electron transfer from graphite to PTFE, thereby alleviating the PTFE breakdown. The graphite polymer coatings improved initial Coulombic efficiencies of full cells from 67.2% (bare) to 79.1% (PEO) and 77.8% (P(VDF-TrFE-CFE)) and increased initial discharge capacity from 157.7 mAh g(NCM)-1 (bare) to 185.1 mAh g(NCM)-1 (PEO) and 182.5 mAh g(NCM)-1 (P(VDF-TrFE-CFE)) in the full cells. These outcomes demonstrate that PTFE degradation in the anode can be surmounted by adjusting the electron transfer to the PTFE.

Non-Electroconductive Polymer Coating on Graphite Mitigating Electrochemical Degradation of PTFE for a Dry-Processed Lithium-Ion Battery Anode.

Lithium metal (LM) is a promising anode for next-generation batteries due to its high theoretical capacity and low electrode potential. Nonetheless, side reactions, volume change, and unwanted lithium dendrite growth seriously limit the practical application of LM. Herein, with the aid of a hard template approach, a novel lithiophilic CoF2-carbon hollow sphere (CoF2@C-HS) composite material is successfully prepared via a facile in-situ fluorination and etching strategy. The lithiophilic CoF2 acts as nucleation sites to reduce nucleation overpotential as well as induces the spatial Li deposition and the formation of LiF-rich solid electrolyte interphase (SEI), and the hollow carbon matrix can enhance the electrical conductivity and offer free space for LM deposition. Theoretical simulations reveal that the synergistic effect of lithiophilic CoF2 and hollow carbon matrix homogenizes the electric field distribution and Li+ flux. Benefiting from these advantages, the CoF2@C-HS-modified copper substrate electrode delivers an enhanced Coulombic efficiency (CE) of 93.7% for 280 cycles at 1 mA cm−2 and 1 mA h cm−2. The symmetrical cell using CoF2@C-HS can stably cycle more than 1800 h with a low voltage hysteresis of 11 mV at a current density of 0.5 mA cm−2 and an areal capacity of 0.5 mA h cm−2. Moreover, the Li@CoF2@C-HS composite anode enables more than 300 stable cycles at 1 C with a capacity retention of 95% in LiFePO4-based full cell and 110 stable cycles at 1 C in LiNi0.8Co0.1Mn0.1O2 (NCM811)-based high-voltage full cell. This work might shed a new light on designing lithiophilic hosts to spatially confine LM deposition, realizing dendrite-free LM anodes and the practical applications of LM batteries. 

Lithiophilic CoF2@C hollow spheres towards spatial lithium deposition for stable lithium metal batteries

Dry processing is a promising method for high-performance and low-cost lithium-ion battery manufacturing which uses polytetrafluoroethylene (PTFE) as a binder. However, the electrochemical stability of the PTFE binder in the cathodes and the generated chemistry of the cathode electrolyte interphase (CEI) layers are rarely reported. Herein, the CEI properties and PTFE electrochemical stability are studied via cycling the high-loading dry-processed electrodes in electrolytes with LiPF6 or LiClO4 salt. Using LiClO4 salt can eliminate other possible F sources, allowing the decomposition of PTFE to be studied. The detection of LiF in cells with the LiClO4 salt confirms that PTFE undergoes side reaction(s) in the cathodes. When compared with LiClO4, the CEI layer is much thicker when LiPF6 is used as the electrolyte salt. These results provide insights into the CEI layer and may potentially enlighten the development of binders and electrolytes for the high efficiency and long durability of DP-based LIBs. 

Insights into the Chemistry of the Cathodic Electrolyte Interphase for PTFE-Based Dry-Processed Cathodes.

Natural Fiber-Derived Gas Diffusion Layers for High Performance, Lower Cost Pem Fuel Cells

Ytterbium Ion collection on Graphite Plates

Surface modified reduced graphene oxide (rGO) aerogels were synthesized using the hydrothermal method. Ethylene diamine (EDA) and α-cyclodextrin (CD) were used to functionalize the surface of the graphene oxide layers. The oxygen reduction and surface modification occurred in-situ during the hydrothermal self-assembly process. The chemical functionality and structure of the resulting ethylene diamine modified (rGO-EDA) and cyclodextrin modified (rGO-CD) aerogels as well as of the pristine unmodified rGO aerogel were studied using XPS, SEM, XRD, and SANS techniques. The overall surface composition showed a significant decrease in the oxygen content for all synthesized aerogels. The surface modified aerogels were characterized by a disordered stacking of the assembled rGO layers. The surface functionalities resulted in a broad distribution of the interlayer spacing and introduced structural heterogeneities. Such disordered structures can enable a better adsorption mechanism of the sodium ions. Coin cells based on the synthesized aerogels and sodium metal were assembled and tested at several charge and discharge rates. The correlation between the surface functionality of the rGO, the induced structural heterogeneities due to the disordered stacking, and the electrochemical performance of sodium-ion batteries were investigated. Operando XRD measurements were carried out during the battery cycling to investigate the adsorption or intercalation nature of the sodiation mechanism.

/pdf/reduced-graphene-oxide-aerogels-with-functionalization-3jaarnp8.pdf

Reduced Graphene Oxide Aerogels with Functionalization-Mediated Disordered Stacking for Sodium-Ion Batteries

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Insights into the Chemistry of the Cathodic Electrolyte Interphase for PTFE-Based Dry-Processed Cathodes.

Natural Fiber-Derived Gas Diffusion Layers for High Performance, Lower Cost Pem Fuel Cells

Ytterbium Ion collection on Graphite Plates

Reduced Graphene Oxide Aerogels with Functionalization-Mediated Disordered Stacking for Sodium-Ion Batteries