Energy & Environmental Materials最新文献

Sulfide-based inorganic solid electrolytes are promising materials for high-performance safe solid-state batteries. The high ion conductivity, mechanical characteristics, and good processability of sulfide-based inorganic solid electrolytes are desirable properties for realizing high-performance safe solid-state batteries by replacing conventional liquid electrolytes. However, the low chemical and electrochemical stability of sulfide-based inorganic solid electrolytes hinder the commercialization of sulfide-based safe solid-state batteries. Particularly, the instability of sulfide-based inorganic solid electrolytes is intensified in the cathode, comprising various materials. In this study, carbonate-based ionic conductive polymers are introduced to the cathode to protect cathode materials and suppress the reactivity of sulfide electrolytes. Several instruments, including electrochemical spectroscopy, X-ray photoelectron spectroscopy, and scanning electron microscopy, confirm the chemical and electrochemical stability of the polymer electrolytes in contact with sulfide-based inorganic solid electrolytes. Sulfide-based solid-state cells show stable electrochemical performance over 100 cycles when the ionic conductive polymers were applied to the cathode.

A commentary on pressure-induced pre-lithiation towards Si anodes in all-solid-state Li-ion batteries (ASSLIBs) using sulfide electrolytes (SEs) is presented. First, feasible pre-lithiation technologies for Si anodes in SE-based ASSLIBs especially the significant pressure-induced pre-lithiation strategies are briefly reviewed. Then, a recent achievement by Meng et al. in this field is elaborated in detail. Finally, the significance of Meng's work is discussed.

The relation between the structure of the silver network electrodes and the properties of Cu(In,Ga)Se₂ (CIGS) solar cells is systemically investigated. The Ag network electrode is deposited onto an Al:ZnO (AZO) thin film, employing a self-forming cracked template. Precise control over the cracked template's structure is achieved through careful adjustment of temperature and humidity. The Ag network electrodes with different coverage areas and network densities are systemically applied to the CIGS solar cells. It is revealed that predominant fill factor (FF) is influenced by the figure of merit of transparent conducting electrodes, rather than sheet resistance, particularly when the coverage area falls within the range of 1.3–5%. Furthermore, a higher network density corresponds to an enhanced FF when the coverage areas of the Ag networks are similar. When utilizing a thinner AZO film, CIGS solar cells with a surface area of 1.0609 cm² exhibit a notable performance improvement, with efficiency increasing from 10.48% to 11.63%. This enhancement is primarily attributed to the increase in FF from 45% to 65%. These findings underscore the considerable potential for reducing the thickness of the transparent conductive oxide (TCO) in CIGS modules with implications for practical applications in photovoltaic technology.

Epoxy resin, characterized by prominent mechanical and electric-insulation properties, is the preferred material for packaging power electronic devices. Unfortunately, the efficient recycling and reuse of epoxy materials with thermally cross-linked molecular structures has become a daunting challenge. Here, we propose an economical and operable recycling strategy to regenerate waste epoxy resin into a high-performance material. Different particle size of waste epoxy micro-spheres (100–600 μm) with core-shell structure is obtained through simple mechanical crushing and boron nitride surface treatment. By using smattering epoxy monomer as an adhesive, an eco-friendly composite material with a “brick-wall structure” can be formed. The continuous boron nitride pathway with efficient thermal conductivity endows eco-friendly composite materials with a preeminent thermal conductivity of 3.71 W m⁻¹ K⁻¹ at a low content of 8.5 vol% h-BN, superior to pure epoxy resin (0.21 W m⁻¹ K⁻¹). The composite, after secondary recycling and reuse, still maintains a thermal conductivity of 2.12 W m⁻¹ K⁻¹ and has mechanical and insulation properties comparable to the new epoxy resin (energy storage modulus of 2326.3 MPa and breakdown strength of 40.18 kV mm⁻¹). This strategy expands the sustainable application prospects of thermosetting polymers, offering extremely high economic and environmental value.

Zinc metal anodes are gaining popularity in aqueous electrochemical energy storage systems for their high safety, cost-effectiveness, and high capacity. However, the service life of zinc metal anodes is severely constrained by critical challenges, including dendrites, water-induced hydrogen evolution, and passivation. In this study, a protective two-dimensional metal–organic framework interphase is in situ constructed on the zinc anode surface with a novel gel vapor deposition method. The ultrathin interphase layer (~1 μm) is made of layer-stacking 2D nanosheets with angstrom-level pores of around 2.1 Å, which serves as an ion sieve to reject large solvent–ion pairs while homogenizes the transport of partially desolvated zinc ions, contributing to a uniform and highly reversible zinc deposition. With the shielding of the interphase layer, an ultra-stable zinc plating/stripping is achieved in symmetric cells with cycling over 1000 h at 0.5 mA cm⁻² and ~700 h at 1 mA cm⁻², far exceeding that of the bare zinc anodes (250 and 70 h). Furthermore, as a proof-of-concept demonstration, the full cell paired with MnO₂ cathode demonstrates improved rate performances and stable cycling (1200 cycles at 1 A g⁻¹). This work provides fresh insights into interphase design to promote the performance of zinc metal anodes.

The development of cost-effective, highly efficient, and durable electrocatalysts has been a paramount pursuit for advancing the hydrogen evolution reaction (HER). Herein, a simplified synthesis protocol was designed to achieve a self-standing electrode, composed of activated carbon paper embedded with Ru single-atom catalysts and Ru nanoclusters (ACP/Ru_SAC+C) via acid activation, immersion, and high-temperature pyrolysis. Ab initio molecular dynamics (AIMD) calculations are employed to gain a more profound understanding of the impact of acid activation on carbon paper. Furthermore, the coexistence states of the Ru atoms are confirmed via aberration-corrected scanning transmission electron microscopy (AC-STEM), X-ray photoelectron spectroscopy (XPS), and X-ray absorption spectroscopy (XAS). Experimental measurements and theoretical calculations reveal that introducing a Ru single-atom site adjacent to the Ru nanoclusters induces a synergistic effect, tuning the electronic structure and thereby significantly enhancing their catalytic performance. Notably, the ACP/Ru_SAC+C exhibits a remarkable turnover frequency (TOF) of 18 s⁻¹ and an exceptional mass activity (MA) of 2.2 A mg⁻¹, surpassing the performance of conventional Pt electrodes. The self-standing electrode, featuring harmoniously coexisting Ru states, stands out as a prospective choice for advancing HER catalysts, enhancing energy efficiency, productivity, and selectivity.

In challenging operational environments, Lithium-ion batteries (LIBs) inevitably experience mechanical stresses, including impacts and extrusion, which can lead to battery damage, failure, and even the occurrence of fire and explosion incidents. Consequently, it is imperative to investigate the safety performance of LIBs under mechanical loads. This study is grounded in a more realistic coupling scenario consisting of electrochemical cycling and low-velocity impact. We systematically and experimentally uncovered the mechanical, electrochemical, and thermal responses, damage behavior, and corresponding mechanisms under various conditions. Our study demonstrates that higher impact energy results in increased structural stiffness, maximum temperature, and maximum voltage drop. Furthermore, heightened impact energy significantly influences the electrical resistance parameters within the internal resistance. We also examined the effects of State of Charge (SOC) and C-rates. The methodology and experimental findings will offer insights for enhancing the safety design, conducting risk assessments, and enabling the cascading utilization of energy storage systems based on LIBs.

The practical application of lithium (Li) metal anodes in high-capacity batteries is impeded by the formation of hazardous Li dendrites. To address this challenge, this research presents a novel methodology that combines laser ablation and heat treatment to precisely induce controlled grain growth within laser-structured grooves on copper (Cu) current collectors. Specifically, this approach enhances the prevalence of Cu (100) facets within the grooves, effectively lowering the overpotential for Li nucleation and promoting preferential Li deposition. Unlike approaches that modify the entire surface of collectors, our work focuses on selectively enhancing lithiophilicity within the grooves to mitigate the formation of Li dendrites and exhibit exceptional performance metrics. The half-cell with these collectors maintains a remarkable Coulombic efficiency of 97.42% over 350 cycles at 1 mA cm⁻². The symmetric cell can cycle stably for 1600 h at 0.5 mA cm⁻². Furthermore, when integrated with LiFePO₄ cathodes, the full-cell configuration demonstrates outstanding capacity retention of 92.39% after 400 cycles at a 1C discharge rate. This study introduces a novel technique for fabricating selective lithiophilic three-dimensional (3D) Cu current collectors, thereby enhancing the performance of Li metal batteries. The insights gained from this approach hold promise for enhancing the performance of all laser-processed 3D Cu current collectors by enabling precise lithiophilic modifications within complex structures.

High-capacity nickel-rich layered oxides are promising cathode materials for high-energy-density lithium batteries. However, the poor structural stability and severe side reactions at the electrode/electrolyte interface result in unsatisfactory cycle performance. Herein, the thin layer of two-dimensional (2D) graphitic carbon-nitride (g-C₃N₄) is uniformly coated on the LiNi_0.8Co_0.1Mn_0.1O₂ (denoted as NCM811@CN) using a facile chemical vaporization-assisted synthesis method. As an ideal protective layer, the g-C₃N₄ layer effectively avoids direct contact between the NCM811 cathode and the electrolyte, preventing harmful side reactions and inhibiting secondary crystal cracking. Moreover, the unique nanopore structure and abundant nitrogen vacancy edges in g-C₃N₄ facilitate the adsorption and diffusion of lithium ions, which enhances the lithium deintercalation/intercalation kinetics of the NCM811 cathode. As a result, the NCM811@CN-3wt% cathode exhibits 161.3 mAh g⁻¹ and capacity retention of 84.6% at 0.5 C and 55 °C after 400 cycles and 95.7 mAh g⁻¹ at 10 C, which is greatly superior to the uncoated NCM811 (i.e. 129.3 mAh g⁻¹ and capacity retention of 67.4% at 0.5 C and 55 °C after 220 cycles and 28.8 mAh g⁻¹ at 10 C). The improved cycle performance of the NCM811@CN-3wt% cathode is also applicable to solid–liquid-hybrid cells composed of PVDF:LLZTO electrolyte membranes, which show 163.8 mAh g⁻¹ and the capacity retention of 88.1% at 0.1 C and 30 °C after 200 cycles and 95.3 mAh g⁻¹ at 1 C.

All-solid-state lithium metal batteries (ASSLMBs) featuring sulfide solid electrolytes (SEs) are recognized as the most promising next-generation energy storage technology because of their exceptional safety and much-improved energy density. However, lithium dendrite growth in sulfide SEs and their poor air stability have posed significant obstacles to the advancement of sulfide-based ASSLMBs. Here, a thin layer (approximately 5 nm) of g-C₃N₄ is coated on the surface of a sulfide SE (Li₆PS₅Cl), which not only lowers the electronic conductivity of Li₆PS₅Cl but also achieves remarkable interface stability by facilitating the in situ formation of ion-conductive Li₃N at the Li/Li₆PS₅Cl interface. Additionally, the g-C₃N₄ coating on the surface can substantially reduce the formation of H₂S when Li₆PS₅Cl is exposed to humid air. As a result, Li–Li symmetrical cells using g-C₃N₄-coated Li₆PS₅Cl stably cycle for 1000 h with a current density of 0.2 mA cm⁻². ASSLMBs paired with LiNbO₃-coated LiNi_0.6Mn_0.2Co_0.2O₂ exhibit a capacity of 132.8 mAh g⁻¹ at 0.1 C and a high-capacity retention of 99.1% after 200 cycles. Furthermore, g-C₃N₄-coated Li₆PS₅Cl effectively mitigates the self-discharge behavior observed in ASSLMBs. This surface-coating approach for sulfide solid electrolytes opens the door to the practical implementation of sulfide-based ASSLMBs.