Metallic lithium anodes are highly promising for revolutionizing current rechargeable batteries because of their ultrahigh energy density. However, the application of lithium metal batteries is ...considerably impeded by lithium dendrite growth. Here, a biomacromolecule matrix obtained from the natural membrane of eggshell is introduced to control lithium growth and the mechanism is motivated by how living organisms regulate the orientation of inorganic crystals in biomineralization. Specifically, cryo-electron microscopy is utilized to probe the structure of lithium at the atomic level. The dendrites growing along the preferred < 111 > crystallographic orientation are greatly suppressed in the presence of the biomacromolecule. Furthermore, the naturally soluble chemical species in the biomacromolecules can participate in the formation of solid electrolyte interphase upon cycling, thus effectively homogenizing the lithium deposition. The lithium anodes employing bioinspired design exhibit enhanced cycling capability. This work sheds light on identifying substantial challenges in lithium anodes for developing advanced batteries.
High energy density and low cost make lithium-sulfur (Li-S) batteries famous in the field of energy storage systems. However, the advancement of Li-S batteries is evidently hindered by the notorious ...shuttle effect and other issues that occur in sulfur cathodes during cycles. Among various strategies applied in Li-S batteries, using biomass-derived materials is more promising due to their outstanding advantages including strong physical and chemical adsorptions as well as abundant sources, low cost, and environmental friendliness. This review summarizes the recent progress of biomass-derived materials in Li-S batteries. By focusing on the aspects of carbon hosts, separator materials, bio-polymer binders, and all-solid-state electrolytes, the authors aim to shed light on the rational design and utilization of biomass-derived materials in Li-S batteries with high energy density and long cycle lifespan. Perspectives regarding future research opportunities in biomass-derived materials for Li-S batteries are also discussed.
This review summarizes recent progress of biomass-derived materials in Li-S batteries. These materials are promising due to their advantages including strong physical and chemical adsorption, high abundance, low cost, and environmental friendliness.
The application of solid polymer electrolytes (SPEs) is still inherently limited by the unstable lithium (Li)/electrolyte interface, despite the advantages of security, flexibility, and workability ...of SPEs. Herein, the Li/electrolyte interface is modified by introducing Li2S additive to harvest stable all‐solid‐state lithium metal batteries (LMBs). Cryo‐transmission electron microscopy (cryo‐TEM) results demonstrate a mosaic interface between poly(ethylene oxide) (PEO) electrolytes and Li metal anodes, in which abundant crystalline grains of Li, Li2O, LiOH, and Li2CO3 are randomly distributed. Besides, cryo‐TEM visualization, combined with molecular dynamics simulations, reveals that the introduction of Li2S accelerates the decomposition of N(CF3SO2)2− and consequently promotes the formation of abundant LiF nanocrystals in the Li/PEO interface. The generated LiF is further verified to inhibit the breakage of CO bonds in the polymer chains and prevents the continuous interface reaction between Li and PEO. Therefore, the all‐solid‐state LMBs with the LiF‐enriched interface exhibit improved cycling capability and stability in a cell configuration with an ultralong lifespan over 1800 h. This work is believed to open up a new avenue for rational design of high‐performance all‐solid‐state LMBs.
Based on the atomic visualization of the lithium (Li)/poly(ethylene oxide) (PEO) interface through cryo‐transmission electron microscopy, Li2S additive is revealed to promote the decomposition of LiN(CF3SO2)2 (LiTFSI) to generate uniform LiF nanocrystals in situ, rendering uniform Li deposition and preventing PEO bond cleavage. This optimized interface is promising for PEO‐electrolyte‐based Li metal batteries with significantly improved cycling lifespan.
Lithium-sulfur batteries have attracted attention due to their six-fold specific energy compared with conventional lithium-ion batteries. Dissolution of lithium polysulfides, volume expansion of ...sulfur and uncontrollable deposition of lithium sulfide are three of the main challenges for this technology. State-of-the-art sulfur cathodes based on metal-oxide nanostructures can suppress the shuttle-effect and enable controlled lithium sulfide deposition. However, a clear mechanistic understanding and corresponding selection criteria for the oxides are still lacking. Herein, various nonconductive metal-oxide nanoparticle-decorated carbon flakes are synthesized via a facile biotemplating method. The cathodes based on magnesium oxide, cerium oxide and lanthanum oxide show enhanced cycling performance. Adsorption experiments and theoretical calculations reveal that polysulfide capture by the oxides is via monolayered chemisorption. Moreover, we show that better surface diffusion leads to higher deposition efficiency of sulfide species on electrodes. Hence, oxide selection is proposed to balance optimization between sulfide-adsorption and diffusion on the oxides.
Lithium metal-based battery is considered one of the best energy storage systems due to its high theoretical capacity and lowest anode potential of all. However, dendritic growth and virtually ...relative infinity volume change during long-term cycling often lead to severe safety hazards and catastrophic failure. Here, a stable lithium–scaffold composite electrode is developed by lithium melt infusion into a 3D porous carbon matrix with “lithiophilic” coating. Lithium is uniformly entrapped on the matrix surface and in the 3D structure. The resulting composite electrode possesses a high conductive surface area and excellent structural stability upon galvanostatic cycling. We showed stable cycling of this composite electrode with small Li plating/stripping overpotential (<90 mV) at a high current density of 3 mA/cm² over 80 cycles.
Compared with conventional liquid batteries, all‐solid‐state batteries (ASSBs) show great promise for enabling higher safety in electric vehicles without compromising operational durability and ...range. As a key component of ASSBs, solid‐state electrolytes (SSEs) need high ionic conductivity and favorable interfacial compatibility between electrodes and SSEs. In the recent decade, numerous efforts have been devoted to SSE advancement and fruitful achievements have been made, particularly regarding metal anode‐oriented SSEs with high energy density. This review focuses on the historical process of SSEs employed in ASSBs. The new understanding and origins for the enhanced ionic conductivity and mechanical properties of SSEs are first summarized. As to the cathode/SSE interface, its decomposition mechanism and modification strategies are analyzed. As to the interfacial issues of SSEs with anodes, the mechanisms of dendrite formation and penetration into the SSEs are discussed in detail. Additionally, assisted by a library of big data sources, contributions are systematically highlighted from different countries, institutions, and corresponding authors to significantly advance SSE progress, and certain insights are provided into the underlying relationships between various items in a collective manner. Finally, current challenges and potential strategies are identified for the future development of SSEs in ASSBs.
By illustrating the correlation between performance improvement/failure of solid state electrolytes (SSEs) and microscale material design, this review aims to provide a comprehensive evolution view and an iterative historical perspective of the SSEs over the past 10 years.
2D transition metal carbides, carbonitrides, and nitrides known as MXenes possess high electrical conductivity, large redox active surface area, rich surface chemistry, and tunable structures. ...Benefiting from these exceptional chemical and physical properties, the applications of MXenes for electrochemical energy storage and conversion have attracted increasing research interests around the world. Notably, the electrochemical performances of MXenes are directly dependent on their synthesis conditions, interfacial chemistries and structural configurations. In this review, we summarize the synthesis techniques of MXenes, as well as the recent advances in the interfacial structure design of MXene‐based nanomaterials for electrochemical energy storage and conversion applications. Additionally, we provide an in‐depth discussion on the relationship between interfacial structure and electrochemical performance from the perspectives of energy storage and electrocatalysis mechanisms. Finally, the challenges and insights for the future research of interfacial structure design of MXenes are outlined.
In this review, we summarize the synthesis techniques of MXenes, as well as the recent advances in the interfacial structure design of MXene‐based nanomaterials for electrochemical energy storage and conversion applications. Additionally, we provide an in‐depth discussion on the relationship between interfacial structure and electrochemical performance from the perspectives of energy storage and electrocatalysis mechanisms. Finally, the challenges and perspectives for the future research of interfacial structure design of MXenes are outlined.
High‐performance rechargeable all‐solid‐state lithium metal batteries with high energy density and enhanced safety are attractive for applications like portable electronic devices and electric ...vehicles. Among the various solid electrolytes, argyrodite Li6PS5Cl with high ionic conductivity and easy processability is of great interest. However, the low interface compatibility between sulfide solid electrolytes and high capacity cathodes like nickel‐rich layered oxides requires many thorny issues to be resolved, such as the space charge layer (SCL) and interfacial reactions. In this work, in situ electrochemical impedance spectroscopy and in situ Raman spectroscopy measurements are performed to monitor the detailed interface evolutions in a LiNi0.8Co0.1Mn0.1O2 (NCM)/Li6PS5Cl/Li cell. Combining with ex situ characterizations including scanning electron microscopy and X‐ray photoelectron spectroscopy, the evolution of the SCL and the chemical bond vibration at NCM/Li6PS5Cl interface during the early cycles is elaborated. It is found that the Li+ ion migration, which varies with the potential change, is a very significant cause of these interface behaviors. For the long‐term cycling, the SCL, interfacial reactions, lithium dendrites, and chemo‐mechanical failure have an integrated effect on interfaces, further deteriorating the interfacial structure and electrochemical performance. This research provides a new insight on intra and intercycle interfacial evolution of solid‐state batteries.
Several in situ and ex situ measurements are used to monitor the interfacial evolutions in a LiNi0.8Co0.1Mn0.1O2 (NCM)/Li6PS5Cl/Li cell. The detailed interfacial evolution shows very different behavior between inter and intracycles. The evolution of the space charge layer and the chemical bond vibration at NCM/Li6PS5Cl interface play key roles during the early cycles.
Lithium metal is the most attractive anode material due to its extremely high specific capacity, minimum potential, and low density. However, uncontrollable growth of lithium dendrite results in ...severe safety and cycling stability concerns, which hinders the application in next generation secondary batteries. In this paper, a new and facile method imposing a magnetic field to lithium metal anodes is proposed. That is, the lithium ions suffering Lorentz force due to the electromagnetic fields are put into spiral motion causing magnetohydrodynamics (MHD) effect. This MHD effect can effectively promote mass transfer and uniform distribution of lithium ions to suppress the dendrite growth as well as obtain uniform and compact lithium deposition. The results show that the lithium metal electrodes within the magnetic field exhibit excellent cycling and rate performance in a symmetrical battery. Additionally, full batteries using limited lithium metal as anodes and commercial LiFePO4 as cathodes show improved performance within the magnetic field. In summary, a new and facile strategy of suppressing lithium dendrites using the MHD effect by imposing a magnetic field is proposed, which may be generalized to other advanced alkali metal batteries.
An novel external strategy of imposing a magnetic field to lithium metal anodes is presented. The generated Lorentz force due to the electromagnetic fields is used to promote mass transfer and uniform distribution of lithium ions. This magnetohydrodynamics effect can effectively suppress the dendrite growth as well as obtain uniform and compact lithium deposition with the remarkable performance.
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