Search

Zn anodes suffer from poor reversibility and stability owing to nonuniform dendrite growth and self-corrosion. Here, 1-ethyl-3-methylimidazolium acetate (EMImAc) is introduced to reconstruct interfacial electrical double layer with simultaneously manipulating the solvation environment and the adsorption situation on Zn anode. The acetate anions with high nucleophilicity can effectively alter the solvation shell around Zn 2+ ions and immobilize the H 2 O molecules, thus weakening water activity and alleviating water-related parasitic reactions. Concomitantly, both the imidazolium cation and acetate anion are inclined to gather on Zn anode surface for constructing an electrostatic shielding layer, and meanwhile the chemisorbed acetate anions also contribute to accelerate the Zn(H 2 O) 6 2+ desolvation process. Such a synergistic effect enables uniform electric field distribution and facilitates Zn ion flux, which mitigates the random diffusion of Zn 2+ and finally promotes the dendrite-free deposition. As a result, the Zn/Zn symmetric cells with EMImAc-integrated aqueous electrolyte realize an excellent cycling lifespan of 7000 h (0.5 mA cm -2 /0.25 mAh cm -2 ) and high Zn utilization of 61.3 % (15 mA cm -2 /20 mAh cm -2 ). Furthermore, the effective of EMImAc additive is demonstrated in Zn/V 2 O 5 cells. This work offers insights into the ionic liquid-integrated aqueous electrolytes to enhance the interface stability of Zn anode for rechargeable zinc batteries., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Inc. All rights reserved.)

The irreversibility and low utilization of Zn anode stemming from the corrosion and dendrite growth have largely limited the commercialization of aqueous zinc batteries. Here, a carbonyl-rich polymer interphase of zinc polyacrylate (ZPAA) is spontaneously in-situ constructed on Zn anode to address the above-mentioned dilemmas. The ZPAA interlayer enables fast transport kinetics of Zn 2+ and tailors the interfacial electric field for realizing the uniform Zn deposition due to superior zincophilicity, high Zn 2+ transference number and inherent ion-diffusion channel. Importantly, acting as a buffer interphase with strong adhesion and isolation of electrolytes, this functional layer effectively protects the Zn electrode against the water-induced erosion and passivation. Remarkably, the ZPAA@Zn electrode realizes an enhanced Coulombic efficiency of 99.71 % within 2200 cycles, delivers an ultra-long cycling stability over 7660 h (>319 days, 1 mA cm -2 ) and 2460 h (5 mA cm -2 ) with lower voltage hysteresis. Also, the ZPAA@Zn/MnO 2 full cell maintains a high capacity of 114 mAh/g after 2000 cycles, much better that of untreated Zn/MnO 2 cell (25 mAh/g). This concept of in-situ fabricating ion-sieve-like polymer interphase provides a facile approach to stabilize Zn anode and further paves a way for high-performance aqueous batteries., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Inc. All rights reserved.)

Zn anodes suffer from the formation of uncontrolled dendrites aggravated by the uneven electric field and the insulating by-product accumulation in aqueous zinc-ion batteries (AZIBs). Here, an effective strategy implemented by 1-butyl-3-methylimidazolium hydrogen sulfate (BMIHSO 4 ) additive is proposed to synergistically tune the crystallographic orientation of zinc deposition and suppress the formation of zinc hydroxide sulfate for enhancing the reversibility on Zn anode surface. As a competing cation, BMI + is proved to preferably adsorb on Zn-electrode compared with H 2 O molecules, which shields the "tip effect" and inhibits the Zn-deposition agglomerations to inducing the horizontal growth along Zn (002) crystallographic texture. Simultaneously, the protonated BMIHSO 4 additives could remove the detrimental OH - in real-time to fundamentally eliminate the accumulation of 6Zn(OH) 2 ·ZnSO 4 ·4H 2 O and Zn 4 SO 4 (OH) 6 ·H 2 O on Zn anode surface. Consequently, Zn anode exhibits an ultra-long cycling stability of one year (8762 h) at 0.2 mA cm -2 /0.2 mAh cm -2 , 3600 h at 2 mA cm -2 /2 mAh cm -2 with a high plating cumulative capacity of 3.6 Ah cm -2 , and a high average Coulombic efficiency of 99.6 % throughout 1000 cycles. This work of regulating Zn deposition texture combined with eliminating notorious by-products could offer a desirable way for stabilizing the Zn-anode/electrolyte interface in AZIBs., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Inc. All rights reserved.)

Improving the fast-charging capabilities and energy storage capacity of electric vehicles presents a feasible strategy for mitigating the prevalent concern of range anxiety in the market. Nanostructure electrode materials play a crucial role in this process. However, the current method of preparation is arduous and yields restricted quantities. In view of this, we have devised an innovative approach that provides convenience and efficacy, facilitating the large-scale synthesis of CoS 2 nanoparticles, which exhibited exceptional performance. When the current density was 1000 mA g -1 , the discharging capacity reached 760 mAh g -1 after 400 cycles. Remarkably, even at an increased current density of 5000 mA g -1 , the discharging capacity of CoS 2 remained at 685.5 mAh g -1 . The ultra-high performance could be attributed to the specific surface area, which minimized the diffusion distance of sodium-ions during the charging and discharging processes and mitigated the extent of structural damage. Our straightforward preparation techniques facilitate the mass production and present a novel approach for the development of cost-effective and high-performing anode materials for sodium-ion batteries.

Single-crystalline Ni-rich cathode (SC-NCM) has attracted increasing interest owing to its greater capacity retention in advanced solid-state lithium batteries (SSLBs), while suffers from severe interfacial instability during cycling. Here, via atomic layer deposition, Li 3 PO 4 is introduced to coat SC-NCM (L-NCM), to suppress undesired side reaction and enhance interfacial stability. The dynamic degradation and surface regulation of SC-NCM are investigated inside a working SSLB by in situ atomic force microscopy (AFM). We directly observe the uneven cathode electrolyte interphase (CEI) and surface defects on pristine SC-NCM particle. Remarkably, the formed amorphous LiF-rich CEI on L-NCM maintains its initial structure upon cycling, and thus endows the battery with improved cycling stability and excellent rate capability. Such on-site tracking provides deep insights into surface mechanism and structure-reactivity correlation of SC-NCM, and thus benefits the optimizations of SSLBs., (© 2022 Wiley-VCH GmbH.)

All-carbon graphdiyne (GDY)-based materials have attracted extensive attention owing to their extraordinary structures and outstanding performance in electrochemical energy storage. Straightforward insights into the interfacial evolution at GDY electrode/electrolyte interface could crucially enrich the fundamental comprehensions and inspire targeted regulations. Herein, in situ optical microscopy and atomic force microscopy monitoring of the GDY and N-doped GDY electrodes reveal the interplay between the solid electrolyte interphase (SEI) and Li deposition. The growth and continuous accumulation of the flocculent-like SEI is directly tracked at the surface of GDY electrode. Moreover, the nanoparticle-shaped SEI homogeneously propagates at the interface when N configurations are involved, providing a critical clue for the N-doping effects of stabilizing interfaces and homogenizing Li deposition. This work probes into the dynamic evolution and structure-reactivity correlation in detail, creating effective strategies for GDY-based materials optimization in lithium-ion batteries.

Sulfide-based solid-state electrolytes (SSEs) matched with alloy anodes are considered as promising candidates for application in all-solid-state batteries (ASSBs) to overcome the bottlenecks of the lithium (Li) anode. However, an understanding of the dynamic electrochemical processes on alloy anode in SSE is still elusive. Herein, in situ atomic force microscopy gives insights into the block-formation and stack-accumulation behaviors of Li precipitation on an Li electrode, uncovering the morphological evolution of nanoscale Li deposition/dissolution in ASSBs. Furthermore, two-dimensional Li-indium (In) alloy lamellae and the homogeneous solid electrolyte interphase (SEI) shell on the In electrode reveal the precipitation mechanism microscopically regulated by the alloy anode. The flexible and wrinkle-structure SEI shell further enables the electrode protection and inner Li accommodation upon cycles, elucidating the functional influences of SEI shell on the cycling behaviors. Such on-site tracking of the morphological evolution and dynamic mechanism provide an in-depth understanding and thus benefit the optimizations of alloy-based ASSBs.

Intensive understanding of the surface mechanism of cathode materials, such as structural evolution and chemical and mechanical stability upon charging/discharging, is crucial to design advanced solid-state lithium batteries (SSLBs) of tomorrow. Here, via in situ atomic force microscopy monitoring, we explore the dynamic evolution process at the surface of LiNi 0.5 Co 0.2 Mn 0.3 O 2 cathode particles inside a working SSLB. The dynamic formation process of the cathode interphase layer, with an inorganic-organic hybrid structure, was real-time imaged, as well as the evolution of its mechanical property by in situ scanning of the Derjaguin-Muller-Toporov modulus. Moreover, different components of the cathode interphase layer, such as LiF, Li 2 CO 3 , and specific organic species, were identified in detailat different stages of cycling, which can be directly correlated with the impedance buildup of the battery. In addition, the transition metal migration and the formation of new phases can further exacerbate the degradation of the SSLB. A relatively stable cathode interphase is key to improving the performance of SSLBs. Our findings provide deep insights into the dynamic evolution of surface morphology, chemical components and mechanical properties of the cathode interphase layer, which are pivotal for the performance optimization of SSLBs.

Unstable electrode/solid-state electrolyte interfaces and internal lithium dendrite penetration hamper the applications of solid-state lithium-metal batteries (SSLMBs), and the underlying mechanisms are not well understood. Herein, in situ optical microscopy provides insights into the lithium plating/stripping processes in a gel polymer electrolyte and reveals its dynamic evolution. Spherical lithium deposits evolve into moss-like and branch-shaped lithium dendrites with increasing current densities. Remarkably, the on-site-formed solid electrolyte interphase (SEI) shell on the lithium dendrite is distinctly captured after lithium stripping. Inducing an on-site-formed SEI shell with an enhanced modulus to wrap the lithium precipitation densely and uniformly can regulate dendrite-free behaviors. An in-depth understanding of lithium dendrite evolution and its functional SEI shell will aid in the optimization of SSLMBs., (© 2020 Wiley-VCH GmbH.)

The hybrid nanocomposites of zero-valent iron loaded the activated carbon derived from the corn stalk (ZVI@ACCS) was prepared and used to remove the antibiotics of tetracycline (TC), oxytetracycline (OTC) and chlortetracycline (CTC) from aqueous solution. The adsorption amounts of three antibiotics (103.1 mg g -1 for CTC, 72.9 mg g -1 for OTC and 81.5 mg g -1 for TC) were sensitive to the temperature and independent of pH in the range of 4.2-7.1 at 298 K through the synergistic interactions of the electrostatic attraction, the bridging complexation and the surface complexation. The equilibrium was performed within 20 min at 298 K. The spontaneous (ΔG o <0) and endothermic (ΔH o >0) adsorption of three antibiotics onto the ZVI@ACCS nanocomposites gave a better matching (r 2  > 0.99) with Langmuir and pseudo-second-order models., Competing Interests: Declaration of competing interests The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

Molybdenum disulfide is considered one of the most promising anodes for lithium-ion batteries due to its high specific capacity; however, it suffers from an unstable solid electrolyte interphase. Understanding its structural evolution and reaction mechanism upon charging/discharging is crucial for further improvements in battery performance. Herein, the interfacial processes of solid electrolyte interphase film formation and lithiation/delithiation on ultra-flat monolayer molybdenum disulfide are monitored by in situ atomic force microscopy. The live formation of ultra-thin and dense films can be induced by the use of fluoroethylene carbonate as an additive to effectively protect the anode electrodes. The evolution of the fluoroethylene carbonate-derived solid electrolyte interphase film upon cycling is quantitatively analysed. Furthermore, the formation of wrinkle-structure networks upon lithiation process is distinguished in detailed steps, and accordingly, structure-reactivity correlations are proposed. These quantitative results provide an in-depth understanding of the interfacial mechanism in molybdenum disulfide-based lithium-ion batteries.