The efficient realization of a closed-loop process is an ultimate goal for reusing spent lithium-ion batteries (LIBs), yet the complicated recycling processes of leaching and purification in an acid atmosphere are totally different compared with the regeneration method of the cathode precursor in alkali solution, inevitably resulting in the redundant consumption of acid/ammonia solutions and increased burden for a green environment. Herein, considering the advantages of selective extraction and similar chemical surroundings for recovery and regeneration, ammonia-leaching has been proposed to achieve short-process closed-loop recycling with effective impurity removal. Particularly, benefiting from the galvanic cell interaction, the sluggish reaction rate and relatively harsh reaction conditions of ammonia-leaching are well addressed.
View Article and Find Full Text PDFLithium (Li) metal batteries hold significant promise in elevating energy density, yet their performance at ultralow temperatures remains constrained by sluggish charge transport kinetics and the formation of unstable interphases. In conventional electrolyte systems, lithium ions are tightly locked in the solvation structure, thereby engendering difficulty in the desolvation process and further exacerbating solvent decomposition. Herein, we propose a new push-pull electrolyte design strategy, utilizing molecular electrostatic potential (ESP) screening to identify 2,2-difluoroethyl trifluoromethanesulfonate (DTF) as an optimal cosolvent.
View Article and Find Full Text PDFDue to the inherent characteristics of traditional graphite anode material, its lithium diffusion kinetic is significantly constrained, easily leading to a noticeable capacity degradation during rapid charge/discharge cycling. Although modifying the graphite by mixing the hard carbon can effectively enhance its fast-charging performance, yet the underlying mechanism of improvement effect and structure design of interface are still needed to further investigate. To address this research gap, hard carbon-coated graphite (HCCG) material has been designed and synthesized through simple interface engineering, which is aimed to explore and elucidate the optimization mechanisms on fast-charging performance from the graphite interface perspective.
View Article and Find Full Text PDFThe application of silicon-based nanomaterials in fast-charging scenarios is hindered by volume expansion during lithiation and side reactions induced by surface effects. Constructing a robust encapsulation structure with high mechanical strength and conductivity is pivotal for optimizing the electrochemical performance of nanostructured silicon anodes. Herein, we propose a multifaceted hierarchical encapsulation structure featuring excellent mechanical strength and high conductivity by sequentially incorporating SiO , hard carbon, and closed-pore carbon layers around silicon quantum dots, thereby enabling stable cycling at high current densities.
View Article and Find Full Text PDFThe elimination of Co from Ni-rich layered cathodes is critical to reduce the production cost and increase the energy density for sustainable development. Herein, a delicate strategy of crystal-facet modulation is designed and explored, which is achieved by simultaneous Al/W-doping into the precursors, while the surface role of the crystal-facet is intensively revealed. Unlike traditional studies on crystal structure growth along a certain direction, this work modulates the crystal-facet at the nanoscale based on the effect of W-doping dynamic migration with surface energy, successfully constructing the core-shell (003)/(104) facet surface.
View Article and Find Full Text PDFLayered silicon (L-Si) anodes are celebrated for their high theoretical capacity but face significant challenges regarding safety and material purity during preparation. This study addresses these challenges by employing NHCl-CaSi as the raw material in a gas-solid de-alloying process, which enhances both safety and purity compared to traditional methods. The L-Si anodes produced demonstrate outstanding electrochemical performance, delivering a high reversible lithium storage capacity of 1497.
View Article and Find Full Text PDFTraditional ethylene carbonate (EC)-based electrolytes constrain the applications of silicon carbon (Si-C) anodes under fast-charging and low-temperature conditions due to sluggish Li migration kinetics and unstable solid electrolyte interphase (SEI). Herein, inspired by the efficient water purification and soil stabilization of aquatic plants, a stable SEI with a 3D desolvation interface is designed with gel polymer electrolyte (GPE), accelerating Li desolvation and migration at the interface and within stable SEI. As demonstrated by theoretical simulations and experiment results, the resulting poly(1,3-dioxolane) (PDOL), prepared by in situ ring-opening polymerization of 1,3-dioxolane (DOL), creates a 3D desolvation area, improving the Li desolvation at the interface and yielding an amorphous GPE with a high Li ionic conductivity (5.
View Article and Find Full Text PDFThe instability in the structural integrity caused by interfacial issues is commonly regarded as the primary drawback of Ni-rich layered cathode materials (LiNiCoMnO, where x ≥ 0.8), which must be addressed before their commercial application. Herein, a novel multiple-function surface modification strategy is proposed based on the single crystal structure to in-situ achieve the construction of a coating layer and surface doping with Ce element to enhance the structural stability of the LiNiCoMnO (NCM).
View Article and Find Full Text PDFSingle-crystal Ni-rich cathodes offer promising prospects in mitigating intergranular microcracks and side reaction issues commonly encountered in conventional polycrystalline cathodes. However, the utilization of micrometer-sized single-crystal particles has raised concerns about sluggish Li diffusion kinetics and unfavorable structural degradation, particularly in high Ni content cathodes. Herein, we present an innovative in situ doping strategy to regulate the dominant growth of characteristic planes in the single-crystal precursor, leading to enhanced mechanical properties and effectively tackling the challenges posed by ultrahigh-nickel layered cathodes.
View Article and Find Full Text PDFConstraining the electrochemical reactivity of free solvent molecules is pivotal for developing high-voltage lithium metal batteries, especially for ether solvents with high Li metal compatibility but low oxidation stability ( <4.0 V vs Li/Li). The typical high concentration electrolyte approach relies on nearly saturated Li coordination to ether molecules, which is confronted with severe side reactions under high voltages ( >4.
View Article and Find Full Text PDFAs a mainstream technology for recycling spent lithium-ion batteries, direct regeneration is rapidly developed due to its high efficiency and green characteristics. However, efficient reuse of spent LiNiCoMn O cathode is still a significant challenge, as the rock salt/spinel phase on the surface hinders the Li replenishment and phase transformation to the layered structure. In this work, the fundamental understanding of the repair mechanism is confirmed that the oxidizing atmosphere is the crucial factor that can greatly improve the rate and degree of phase restoration.
View Article and Find Full Text PDFLithium metal batteries (LMBs) offer significant advantages in energy density and output voltage, but they are severely limited by uncontrollable Li dendrite formation resulting from uneven Li behaviors and high reactivity with potential co-solvent plating. Herein, to uniformly enhance the Li behaviors in desolvation and diffusion, the local Li solvation shell structure is optimized by constructing an anion-braking separator, hence dynamically reducing the self-amplifying behavior of dendrites. As a prototypal, two-dimensional lithiated-montmorillonite (LiMMT) is blade-coated on the commercial separator, where abundant -OH groups as Lewis acidic sites and electron acceptors could selectively adsorb corresponding FSI anions, regulating the solvation shell structure and restricting their migration.
View Article and Find Full Text PDFLayered cathode materials for sodium-ion batteries (SIBs) have gained considerable attention as promising candidates owing to their high capacity and potential for industrial scalability. Nonetheless, challenges arise from stress and structural degradation resulting from the deposition of larger ion radius species, leading to diminished cyclic stability and rate performance. In this study, we present a novel and straightforward strategy that combines the synergistic effects of an amorphous aluminum oxide coating and aluminum ion doping.
View Article and Find Full Text PDFCurrently, the recycling of spent lithium-ion batteries (LIBs) has mainly been focused on the extraction of precious metals, such as lithium, cobalt and nickel from cathodes, while the waste graphite anode has been overlooked due to its low-cost production and abundant resources reserve. However, there are enormous potential value and pollution risk in the view of graphite recycling. Thus, we propose an original method to prepare expanded graphite (EG) as new anode material generated from waste graphite in LIBs which integrates the oxidation and purification in one-step.
View Article and Find Full Text PDFChem Commun (Camb)
June 2023
We report the improved kinetic mechanism of a nickel-rich LiNiMnCoAlO cathode. The important role of Co/Al in inhibiting cation disorder to increase the lithium ion diffusion rate is revealed. Impressively, it retains an excellent capacity retention of 76.
View Article and Find Full Text PDFThough numerous framework structures have been constructed to strengthen the reaction kinetics and durability, the inevitable generation of polysulfide dissolution during conversion-process can cause irreparable destruction to ion-channel and crystal structure integrality, which has become a huge obstacle to the application of metal-sulfide in potassium-ion batteries. Herein, the quantum dot structure with catalytic conversion capability is synchronously introduced into the design of FeS anode materials to heighten its K-storage performance. The constructed quantum dot structure anchored by the graphene with space-confinement effect can shorten the ion diffusion path and enlarge the active area, thus accelerating the K-ions transmission kinetics and absorption action, respectively.
View Article and Find Full Text PDFAs a promising high energy density cathode, single-crystal Ni-rich cathode face poor diffusion dynamics, which leads to poor structural evolution, poor cyclic stability and unfavorable rate performance, thus impeding its wider application. Herein, the strategy of synergistic surface modification by ionic conductor coating and trace element doping is delicately designed. The surface protective LiBO layer is wrapped on the single-crystal LiNiCoMnO (NCM83), which can improve the compatibility of cathode/electrolyte with reduced interface resistance.
View Article and Find Full Text PDFChem Commun (Camb)
June 2022
Graphite with an activated edge is carefully designed a controllable solution treatment and sintering process. The simultaneous existence of extra active sites and expanded layers at the edge enable it to exhibit excellent fast-charging performance in a half-cell and full-cell set-up. This work highlights an overall understanding of polarization and the optimum structure for a fast-charging anode.
View Article and Find Full Text PDF2D layered Sn-based materials have attracted enormous attention due to their remarkable performance in sodium-ion batteries. Nevertheless, this promising candidate involves a complex Na -storage process with multistep conversion-alloying reactions, which induces the uneven dispersion of heterogeneous intermediate accompanied by severe agglomeration of metallic Sn , inescapably resulting in poor reaction reversibility with sluggish rate capability and inferior cyclic lifespan. Herein, a delicately layered heterostructure SnSSe/C consisting of defect-rich SnSSe and graphene is designed and successfully achieved via a facile hydrothermal process.
View Article and Find Full Text PDFHigh-capacity Ni-rich layered oxides are promising cathode materials for secondary lithium-based battery systems. However, their structural instability detrimentally affects the battery performance during cell cycling. Here, we report an Al/Zr co-doped single-crystalline LiNiCoMnO (SNCM) cathode material to circumvent the instability issue.
View Article and Find Full Text PDFBackground: To explore the effect of adhesive surface with porcelain sintering and different silane coupling agents on adhesive properties of zirconia ceramics.
Methods: Zirconia blocks (n=72) were randomly divided into two large groups (n=36) according to whether the adhesive surface was treated with sintered porcelain: N (no porcelain sintering), P (porcelain sintering). Then, according to different silane coupling agents, each group was randomly divided into three small groups, six small groups in total (n=12): NN (no porcelain sintering and agent), NM (no porcelain sintering + Monobond-S), NC (no porcelain sintering + Clearfil Repair); PN (porcelain sintering + no agent), PM (porcelain sintering + Monobond-S), PC (porcelain sintering + Clearfil Repair).
Chem Commun (Camb)
March 2022
We report the FeVO porous nanorods on carbon cloth as a novel cathode material for flexible aqueous energy storage. It exhibits excellent electrochemical properties and cycling stability in supercapacitors and zinc-ion batteries. Moreover, this work makes significant progress for developing high-performance electrodes and provides a foundation for future research.
View Article and Find Full Text PDFLithium-ion batteries based on single-crystal LiNi Co Mn O (NCM, 1-x-y ≥ 0.6) cathode materials are gaining increasing attention due to their improved structural stability resulting in superior cycle life compared to batteries based on polycrystalline NCM. However, an in-depth understanding of the less pronounced degradation mechanism of single-crystal NCM is still lacking.
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