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Keywords = Li-metal electrode

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18 pages, 5066 KiB  
Article
Influence of Pulse Duration on Cutting-Edge Quality and Electrochemical Performance of Lithium Metal Anodes
by Lars O. Schmidt, Houssin Wehbe, Sven Hartwig and Maja W. Kandula
Batteries 2025, 11(8), 286; https://doi.org/10.3390/batteries11080286 - 26 Jul 2025
Viewed by 311
Abstract
Lithium metal is a promising anode material for next-generation batteries due to its high specific capacity and low density. However, conventional mechanical processing methods are unsuitable due to lithium’s high reactivity and adhesion. Laser cutting offers a non-contact alternative, but photothermal effects can [...] Read more.
Lithium metal is a promising anode material for next-generation batteries due to its high specific capacity and low density. However, conventional mechanical processing methods are unsuitable due to lithium’s high reactivity and adhesion. Laser cutting offers a non-contact alternative, but photothermal effects can negatively impact the cutting quality and electrochemical performance. This study investigates the influence of pulse duration on the cutting-edge characteristics and electrochemical behavior of laser-cut 20 µm lithium metal on 10 µm copper foils using nanosecond and picosecond laser systems. It was demonstrated that shorter pulse durations significantly reduce the heat-affected zone (HAZ), resulting in improved cutting quality. Electrochemical tests in symmetric Li|Li cells revealed that laser-cut electrodes exhibit enhanced cycling stability compared with mechanically separated anodes, despite the presence of localized dead lithium “reservoirs”. While the overall pulse duration did not show a direct impact on ionic resistance, the characteristics of the cutting edge, particularly the extent of the HAZ, were found to influence the electrochemical performance. Full article
(This article belongs to the Section Battery Processing, Manufacturing and Recycling)
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18 pages, 6225 KiB  
Article
Copper Slag Cathodes for Eco-Friendly Hydrogen Generation: Corrosion and Electrochemical Insights for Saline Water Splitting
by Susana I. Leiva-Guajardo, Manuel Fuentes Maya, Luis Cáceres, Víctor M. Jimenez-Arevalo, Álvaro Soliz, Norman Toro, José Ángel Cobos Murcia, Victor E. Reyes Cruz, Mauricio Morel, Edward Fuentealba and Felipe M. Galleguillos Madrid
Materials 2025, 18(13), 3092; https://doi.org/10.3390/ma18133092 - 30 Jun 2025
Viewed by 467
Abstract
The increasing demand for sustainable energy and clean water has prompted the exploration of alternative solutions to reduce reliance on fossil fuels. In this context, hydrogen production through water electrolysis powered by solar energy presents a promising pathway toward a zero-carbon footprint. This [...] Read more.
The increasing demand for sustainable energy and clean water has prompted the exploration of alternative solutions to reduce reliance on fossil fuels. In this context, hydrogen production through water electrolysis powered by solar energy presents a promising pathway toward a zero-carbon footprint. This study investigates the potential of copper slag, an abundant industrial waste, as a low-cost electrocatalyst for the hydrogen evolution reaction (HER) in contact with saline water such as 0.5 M NaCl and seawater, comparing the electrochemical response when in contact with geothermal water from El Tatio (Atacama Desert). The physicochemical characterisation of copper slag was performed using XRD, Raman, and SEM-EDS to determine its surface properties. Electrochemical evaluations were conducted in 0.5 M NaCl and natural seawater using polarisation techniques to assess the corrosion behaviour and catalytic efficiency of the copper slag electrodes. The results indicate that copper slag exhibits high stability and promising HER kinetics, particularly in seawater, where its mesoporous structure facilitates efficient charge transfer processes. The key novelty of this manuscript lies in the direct revalorisation of untreated copper slag as a functional electrode for HER in real seawater and geothermal water, avoiding the use of expensive noble metals and aligning with circular economy principles. This innovative combination of recycled material and natural saline electrolyte enhances both the technical and economic viability of electrolysis, while reducing environmental impact and promoting green hydrogen production in coastal regions with high solar potential. This research contributes to the value of industrial waste, offering a viable pathway for advancing sustainable hydrogen technologies in real-world environments. Full article
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29 pages, 4963 KiB  
Review
Protective Layer and Current Collector Design for Interface Stabilization in Lithium-Metal Batteries
by Dayoung Kim, Cheolhwan Song and Oh B. Chae
Batteries 2025, 11(6), 220; https://doi.org/10.3390/batteries11060220 - 5 Jun 2025
Viewed by 1238
Abstract
Recent advancements in lithium-metal-based battery technology have garnered significant attention, driven by the increasing demand for high-energy storage devices such as electric vehicles (EVs). Lithium (Li) metal has long been considered an ideal negative electrode due to its high theoretical specific capacity (3860 [...] Read more.
Recent advancements in lithium-metal-based battery technology have garnered significant attention, driven by the increasing demand for high-energy storage devices such as electric vehicles (EVs). Lithium (Li) metal has long been considered an ideal negative electrode due to its high theoretical specific capacity (3860 mAh g−1) and low redox potential. However, the commercialization of Li-metal batteries (LMBs) faces significant challenges, primarily related to the safety and cyclability of the negative electrodes. The formation of lithium dendrites and uneven solid electrolyte interphases, along with volumetric expansion during cycling, severely hinder the commercial viability of LMBs. Among the various strategies developed to overcome these challenges, the introduction of artificial protective layers and the structural engineering of current collectors have emerged as highly promising approaches. These techniques are critical for regulating Li deposition behavior, mitigating dendrite growth, and enhancing interfacial and mechanical stability. This review summarizes the current state of Li-negative electrodes and introduces methods of enhancing their performance using a protective layer and current collector design. Full article
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13 pages, 4213 KiB  
Article
Carbon Nanotubes-Doped Metal Oxides and Metal Sulfides Heterostructure Achieves 3D Morphology Deposition of Li2S and Stable Long-Cycle Lithium–Sulfur Batteries
by Yu-Lin Luo, Hai Huang, Cheng-Wei Zhu, Wen-Qi Lv, Ye Zeng, Gui-Fang Li, Xiao-Hong Fan, Ding-Rong Deng and Qi-Hui Wu
Inorganics 2025, 13(6), 181; https://doi.org/10.3390/inorganics13060181 - 1 Jun 2025
Viewed by 562
Abstract
The “shuttle effect” caused by the shuttling of soluble long-chain polysulfides between the anode and cathode electrodes has persistently hindered lithium–sulfur batteries (LSBs) from achieving stable and high-capacity performance. Numerous materials have been explored to mitigate the adverse effects of this phenomenon, among [...] Read more.
The “shuttle effect” caused by the shuttling of soluble long-chain polysulfides between the anode and cathode electrodes has persistently hindered lithium–sulfur batteries (LSBs) from achieving stable and high-capacity performance. Numerous materials have been explored to mitigate the adverse effects of this phenomenon, among which metal oxides and metal sulfides are regarded as promising solutions due to their strong adsorption capability toward lithium polysulfides (LiPSs). However, the poor electrical conductivity of the metal oxides and sulfides, coupled with their inherent morphological limitations, makes it challenging to sustainably suppress LiPS shuttling. In this study, we designed a heterostructured catalyst composed of a metal oxide–metal sulfide heterostructure integrated with carbon nanotubes (CNTs). This design addresses the low conductivity issue of metal oxides/sulfides while optimizing the material’s morphology, enabling persistent LiPSs adsorption. Furthermore, the composite successfully facilitates three-dimensional (3D) Li2S deposition. The assembled battery exhibits stable and high-capacity performance, delivering an initial discharge capacity of 622.45 mAh g−1 at 2C and retaining 569.5 mAh g−1 after 350 cycles, demonstrating exceptional cycling stability. Full article
(This article belongs to the Special Issue New Semiconductor Materials for Energy Conversion)
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12 pages, 2446 KiB  
Article
Characterization of Industrial Black Mass from End-of-Life LiFePO4-Graphite Batteries
by Nanna Bjerre-Christensen, Caroline Birksø Eriksen, Kristian Oluf Sylvester-Hvid and Dorthe Bomholdt Ravnsbæk
Batteries 2025, 11(6), 210; https://doi.org/10.3390/batteries11060210 - 26 May 2025
Viewed by 790
Abstract
The use of Li-ion batteries is drastically increasing, especially due to the growing sales of electric vehicles. Simultaneously, there is a shift towards exchanging the traditional Co- and Ni-rich electrode materials with more sustainable alternatives such as LiFePO4. This transition challenges [...] Read more.
The use of Li-ion batteries is drastically increasing, especially due to the growing sales of electric vehicles. Simultaneously, there is a shift towards exchanging the traditional Co- and Ni-rich electrode materials with more sustainable alternatives such as LiFePO4. This transition challenges conventional recycling practices, which typically rely on shredding batteries into a substance known as black mass, which is subsequently processed via hydrometallurgical or pyrometallurgical methods to extract valuable elements. These routes may not be economically viable for future sustainable chemistries with lower contents of high-value metal. Hence, new methods for processing the black mass, allowing, e.g., for physical separation and direct recycling, are direly needed. Such developments require that the black mass is thoroughly understood. In this study, we thoroughly characterize a commercially produced Graphite/LFP black mass sample from real battery waste using a suite of analytical techniques. Our findings reveal detailed chemical, morphological, and structural insights and show that the components in the black mass have different micro-size profiles, which may enable simple size separation. Unfortunately, our analysis also reveals that the employed processing of battery waste into black mass leads to the formation of an unknown Fe-containing compound, which may hamper direct recycling routes. Full article
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17 pages, 5532 KiB  
Article
Effect of Mechanical Pressure on Li Metal Deposition Characteristics and Thermal Stability
by Mengyan Xu, Lin Hao, Yiqiang Zhao and Huiqun Fu
Processes 2025, 13(5), 1599; https://doi.org/10.3390/pr13051599 - 21 May 2025
Viewed by 488
Abstract
Pressure significantly influences lithium (Li) deposition behavior. Although previous studies investigating the influence of pressure on Li deposition have often overlooked the impact of mechanical spacer pressure within the cell, this work specifically focuses on this detail. In this study, we explored the [...] Read more.
Pressure significantly influences lithium (Li) deposition behavior. Although previous studies investigating the influence of pressure on Li deposition have often overlooked the impact of mechanical spacer pressure within the cell, this work specifically focuses on this detail. In this study, we explored the effects of mechanical spacer pressure on the electrochemical properties, deposition morphology, solid–electrolyte interphase (SEI), and thermal stability of Li metal deposition, using spacer pressure as a variable in a small-sized electrode half-cell. The experimental results demonstrate that higher spacer pressure positively enhances Li deposition performance across multiple metrics. However, the beneficial effects of higher spacer pressure decrease with increasing deposition capacity. Specifically, at a low deposition capacity (1 mAh/cm2), a higher spacer pressure facilitates Li metal deposition by promoting SEI stabilization, enabling easier deposition, reducing impedance, and enhancing thermal stability. Conversely, at a high deposition capacity (4 mAh/cm2), the spacer pressure does not significantly improve the aforementioned properties. This study combines the morphology of deposited Li with electrochemical and thermal stability assessments, providing valuable research methods and results for evaluating the effects of external pressure on Li metal deposition. Full article
(This article belongs to the Section Chemical Processes and Systems)
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20 pages, 3813 KiB  
Article
Recycling Positive Electrode Materials of Li-Ion Batteries by Creating a pH Gradient Within Aqueous Sodium Chloride Electrolyser
by Yue Chen and Xiaofei Guan
Processes 2025, 13(5), 1525; https://doi.org/10.3390/pr13051525 - 15 May 2025
Viewed by 676
Abstract
Recycling the positive electrode materials of spent Li-ion batteries is critical for environmental sustainability and resource security. To facilitate the attainment of the goal, this study presents a novel approach for recovering valuable metals from positive electrode materials of spent lithium-ion batteries (LIBs) [...] Read more.
Recycling the positive electrode materials of spent Li-ion batteries is critical for environmental sustainability and resource security. To facilitate the attainment of the goal, this study presents a novel approach for recovering valuable metals from positive electrode materials of spent lithium-ion batteries (LIBs) in an H-shaped cell containing aqueous NaCl electrolyte. The process employs hydrochloric acid that could be derived from the chlorine cycle as the leaching agent. The electrolytic device is engineered to generate a high pH gradient, thereby enhancing the leaching of metal elements and eliminating the requirement for external acid or base addition. This green recycling approach adheres to the principles of a circular economy and provides an environmentally friendly solution for sustainable battery material recycling. Full article
(This article belongs to the Section Environmental and Green Processes)
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8 pages, 2287 KiB  
Communication
Lithiophilic Interlayer with Electrolyte-Reservoir and Dendrite-Buffer for High-Performance Lithium Metal Batteries
by Huasen Shen, Guoning Wu, Tingting Ma, Mengjun Li, Yunan Tian, Si Chen, Shaojun Cai and Zhaohuai Li
Nanomaterials 2025, 15(10), 710; https://doi.org/10.3390/nano15100710 - 9 May 2025
Viewed by 512
Abstract
Uneven local electric fields and limited nucleation sites at the reaction interface can lead to the formation of hazardous lithium (Li) dendrites, posing a significant safety risk and impeding the practical utilization of Li metal anodes (LMAs). Here, we present a method utilizing [...] Read more.
Uneven local electric fields and limited nucleation sites at the reaction interface can lead to the formation of hazardous lithium (Li) dendrites, posing a significant safety risk and impeding the practical utilization of Li metal anodes (LMAs). Here, we present a method utilizing atomic layer deposition (ALD) to create lithiophilic titanium nitride (TiN) sites on carbon nanotubes (CNTs) surfaces, integrated with nanocellulose to form a lithiophilic interlayer (NFCP@TN). This interlayer, which is highly flexible and electrolyte-wettable, functions as a current collector and host material for LMAs. The uniform deposition of Li is facilitated by the synergistic interplay of the lithiophilic active sites TiN, the conductive CNT network, and excellent electrolyte wettability of nanocellulose. As a result, Li preferentially adsorbs on TiN sheaths with lower diffusion barriers, leading to controlled nucleation sites and dendrite-free Li deposition. Furthermore, the well-designed NFCP@TN interlayer exhibits exceptional electrochemical performance and significantly extended cycle life when paired LMA with high areal capacity NCM811 (5.0 mAh cm−2) electrodes. Full article
(This article belongs to the Special Issue Design of Nanomaterials for Electrochemical Devices)
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21 pages, 4601 KiB  
Article
Artificial Interfacial Layers with Zwitterionic Ion Structure Improves Lithium Symmetric Battery Life and Inhibits Dendrite Growth
by Haihua Wang, Wei Yuan, Chaoxian Chen, Rui Cao, Huizhu Niu, Ling Song, Jie Wang and Xinyu Shang
Symmetry 2025, 17(5), 652; https://doi.org/10.3390/sym17050652 - 25 Apr 2025
Viewed by 619
Abstract
Lithium (Li) metal’s exceptional low electrode potential and high specific capacity for next-gen energy storage devices make it a top contender. However, the unregulated and unpredictable proliferation of Li dendrites and the instability of interfaces during repeated Li plating and stripping cycles pose [...] Read more.
Lithium (Li) metal’s exceptional low electrode potential and high specific capacity for next-gen energy storage devices make it a top contender. However, the unregulated and unpredictable proliferation of Li dendrites and the instability of interfaces during repeated Li plating and stripping cycles pose significant challenges to the widespread commercialization of Li metal anodes. We introduce the creation of a hydrogen bond network solid electrolyte interphase (SEI) film that integrates zwitterionic groups, designed to facilitate the stability and longevity of lithium metal batteries (LMBs). Here, we design a PVA/P(SBMA-MBA) hydrogen bond network film (PSM) as an artificial SEI, integrating zwitterions and polyvinyl alcohol (PVA) to synergistically regulate Li⁺ flux. The distinctive zwitterionic effect in the network amplifies the SEI film’s ionic conductivity to 1.14 × 10−4 S cm−1 and attains an impressive Li+ ion transfer number of 0.84. In situ Raman spectroscopy reveals dynamic hydrogen bond reconfiguration under strain, endowing the SEI with self-adaptive mechanical robustness. These properties facilitate a homogeneous Li flux and exceptionally suppress dendritic growth. The advanced Li metal anode may endure over 1200 h at 1 mA cm−2 current density and 1 mAh cm−2 area capacity in a Li|Li symmetric battery. And in full cells paired with LiFePO4 cathodes, 93.8% capacity retention is reached after 300 cycles at 1C. Consequently, this work provides a universal strategy for designing dynamic interphases through molecular dipole engineering, paving the way for safe and durable lithium metal batteries. Full article
(This article belongs to the Section Engineering and Materials)
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18 pages, 3885 KiB  
Article
A Pathway to Circular Economy-Converting Li-Ion Battery Recycling Waste into Graphite/rGO Composite Electrocatalysts for Zinc–Air Batteries
by Reio Praats, Jani Sainio, Milla Vikberg, Lassi Klemettinen, Benjamin P. Wilson, Mari Lundström, Ivar Kruusenberg and Kerli Liivand
Batteries 2025, 11(4), 165; https://doi.org/10.3390/batteries11040165 - 21 Apr 2025
Viewed by 1134
Abstract
Li-ion batteries (LIBs) are one of the most deployed energy storage technologies worldwide, providing power for a wide range of applications—from portable electronic devices to electric vehicles (EVs). The growing demand for LIBs, coupled with a shortage of critical battery materials, has prompted [...] Read more.
Li-ion batteries (LIBs) are one of the most deployed energy storage technologies worldwide, providing power for a wide range of applications—from portable electronic devices to electric vehicles (EVs). The growing demand for LIBs, coupled with a shortage of critical battery materials, has prompted the scientific community to seek ways to improve material utilization through the recycling of end-of-life LIBs. While valuable battery metals are already being recycled on an industrial scale, graphite—a material classified as a critical resource—continues to be discarded. In this study, graphite waste recovered from the recycling of LIBs was successfully upcycled into an active graphite/rGO (reduced graphene oxide) composite oxygen electrocatalyst. The precursor graphite for rGO synthesis was also extracted from LIBs. Incorporating rGO into the graphite significantly enhanced the specific surface area and porosity of the resulting composite, facilitating effective doping with residual metals during subsequent nitrogen doping via pyrolysis. These composite catalysts enhanced both the oxygen reduction and oxygen evolution reactions, enabling their use as air electrode catalyst materials in zinc–air batteries (ZABs). The best-performing composite catalyst demonstrated an impressive power density of 100 mW cm−2 and exceptional cycling stability for 137 h. This research further demonstrates the utilization of waste fractions from LIB recycling to drive advancements in energy conversion technologies. Full article
(This article belongs to the Special Issue Two-Dimensional Materials for Battery Applications)
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14 pages, 17658 KiB  
Article
MOF-Derived Hollow Dodecahedral Carbon Structures with Abundant N Sites and Co Nanoparticle-Modified Cu Foil for Dendrite-Free Lithium Metal Battery
by Fei Wang, Huijie Wei, Xinyuan Ren, Junle Zhang, Aiyun Jiang, Yong Liu and Fengzhang Ren
Coatings 2025, 15(4), 490; https://doi.org/10.3390/coatings15040490 - 20 Apr 2025
Viewed by 471
Abstract
In this work, hollow dodecahedral carbon structures with abundant N-doping sites and metal nanoparticles (NC-Co-CNTs) based on MOF-derivative materials were designed and prepared as host materials for lithium metal to ensure uniform lithium deposition on a Cu current collector. NC-Co-CNTs have good electrical [...] Read more.
In this work, hollow dodecahedral carbon structures with abundant N-doping sites and metal nanoparticles (NC-Co-CNTs) based on MOF-derivative materials were designed and prepared as host materials for lithium metal to ensure uniform lithium deposition on a Cu current collector. NC-Co-CNTs have good electrical conductivity, which ensures fast electron transport and Li+ transfer. The carbon nanotubes catalytically derived by Co can promote the uniform distribution of Li+ along the hollow dodecahedral carbon surface and deposition inside the cavity, and the larger electronegativity of N-doped sites and lithophilic sites such as Co nanoparticles can effectively adsorb lithium, inducing the Li+ to be deposited in the form of spherical lithium in a dendrite-free state, inhibiting the growth of dendritic lithium and improving the electrochemical performance of the lithium metal battery. Based on the above advantages, the electrodes of NC-Co-CNT-based symmetric cells present superior cycling performance for more than 1100 h with low overpotential at 1 mAh cm−2/1 mAh·cm−2. Even cycling at high current density of 5 mA cm−2 and high deposition parameters of 5 mAh cm−2, it still cycles for up to 800 h at a relatively low overpotential. Full article
(This article belongs to the Special Issue Multilayer Coatings for Nanomaterials: From Synthesis to Applications)
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12 pages, 4129 KiB  
Article
Structural Design of Dry-Processed Lithium-Rich Mn-Based Materials with High Loading for Enhanced Energy Density
by Yujie Ma, Haojin Guo, Tai Yang and Zhifeng Wang
Batteries 2025, 11(4), 146; https://doi.org/10.3390/batteries11040146 - 7 Apr 2025
Cited by 1 | Viewed by 690
Abstract
With the growing demand for electric vehicles and consumer electronics, lithium-ion batteries with a high energy density are urgently needed. Lithium-rich manganese-based materials (LRMs) are known for their high theoretical specific capacity, rapid electron/ion transfer, and high output voltage. Constructing electrodes with a [...] Read more.
With the growing demand for electric vehicles and consumer electronics, lithium-ion batteries with a high energy density are urgently needed. Lithium-rich manganese-based materials (LRMs) are known for their high theoretical specific capacity, rapid electron/ion transfer, and high output voltage. Constructing electrodes with a substantial amount of active materials is a viable method for enhancing the energy density of batteries. In this study, we prepare thick LRM electrodes through a dry process method of binder fibrillation. A point-to-line-to-surface three-dimensional conductive network is designed by carbon agents with various morphologies. This structural design improves conductivity and facilitates efficient ion and electron transport due to close particle contact and tight packing. A high-loading cathode (35 mg cm−2) is fabricated, achieving an impressive areal capacity of up to 7.9 mAh cm−2. Moreover, the pouch cell paired with a lithium metal anode exhibits a remarkable energy density of 949 Wh kg−1. Compared with the cathodes prepared by the wet process, the dry process optimizes the pathways for e/Li+ transport, leading to reduced resistance, superior coulombic efficiency, retention over cycling, and minimized side reaction. Therefore, the novel structural adoption of the dry process represents a promising avenue for driving innovation and pushing the boundaries for enhanced energy density for batteries. Full article
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41 pages, 9104 KiB  
Review
Progress in Modeling and Applications of Solid Electrolyte Interphase Layers for Lithium Metal Anodes
by Zhicong Wei, Weitao Zheng, Yijuan Li and Shaoming Huang
Nanomaterials 2025, 15(7), 554; https://doi.org/10.3390/nano15070554 - 5 Apr 2025
Viewed by 1193
Abstract
The increasing demand for high-specific-energy lithium batteries has stimulated extensive research on the lithium metal anode owing to its high specific capacity and low electrode potential. However, the lithium metal will irreversibly react with the electrolyte during the first cycling process, forming an [...] Read more.
The increasing demand for high-specific-energy lithium batteries has stimulated extensive research on the lithium metal anode owing to its high specific capacity and low electrode potential. However, the lithium metal will irreversibly react with the electrolyte during the first cycling process, forming an uneven and unstable solid electrolyte interphase (SEI) layer, which results in the non-uniform deposition of Li ions and thus the formation of lithium dendrites. This could cause a battery short circuit, resulting in safety hazards such as thermal runaway. In addition, the continuous rupture and repair of the SEIs during the repeated charge/discharge processes will constantly consume the active lithium, which leads to a significant decrease in battery capacity. An effective strategy to address these challenges is to design and construct ideal artificial SEIs on the surface of the lithium metal anode. This review analyzes and summarizes the mathematical modeling of SEI, the functional characteristics of SEIs with different components, and finally discusses the challenges faced by artificial SEIs in practical applications of lithium metal batteries and future development directions. Full article
(This article belongs to the Special Issue 2D Materials for Energy Conversion and Storage)
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14 pages, 5747 KiB  
Article
Controlled Synthesis of Mesoporous Solid Polymer Electrolyte Au(Pt)NiCe/C Membrane Electrode for Electrocatalytic Hydrogenation
by Shaqin Wang, Yunhao Feng, Liangming Duan, Yueming Shang, Huaihang Fan, Ji Liu, Jiahao Han, Xiaoqi Wang and Bin Yang
Micromachines 2025, 16(4), 436; https://doi.org/10.3390/mi16040436 - 3 Apr 2025
Viewed by 521
Abstract
This study presents a structurally tunable Au-based solid polymer electrolyte (SPE) membrane electrode with significantly enhanced performance in organic hydrogenation reactions. Compared to a Pt-based counterpart, the Au-based electrode achieved a 277% increase in cyclohexane yield and a 4.8% reduction in hydrogen evolution [...] Read more.
This study presents a structurally tunable Au-based solid polymer electrolyte (SPE) membrane electrode with significantly enhanced performance in organic hydrogenation reactions. Compared to a Pt-based counterpart, the Au-based electrode achieved a 277% increase in cyclohexane yield and a 4.8% reduction in hydrogen evolution during cyclohexene hydrogenation, demonstrating superior catalytic selectivity and energy efficiency. The improved performance is attributed to synergistic optimization of the electrode’s nanostructure and electronic properties. The Au-based electrode exhibited a 215% increase in specific surface area (SSA) relative to its initial state, along with a markedly enhanced electrochemical active surface area (ECSA). These enhancements stem from its mesoporous architecture, lattice contraction, and high density of zero-dimensional defects. X-ray photoelectron spectroscopy (XPS) revealed a negative shift in Au4f binding energy, a positive shift in Ni0 peaks, and an increased concentration of oxygen vacancies (Ov), indicating favorable modulation of the surface electronic structure. This reconstruction promotes H* adsorption and accelerates the hydrogenation reaction, serving as a key mechanism for catalytic enhancement. The core innovation of this work lies in the coordinated engineering of nanoscale structure and surface electronic states, enabling concurrent improvements in reaction rate, selectivity, and energy efficiency. These findings offer valuable guidance for designing noble metal-based membrane electrodes in advanced hydrogen energy conversion and storage systems. Full article
(This article belongs to the Special Issue Revolutionary Advances in 2D and 1D Material Based Electronics)
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21 pages, 5327 KiB  
Article
A Universal Highly Concentrated Electrolyte for Improved Cycling Stability in Li(Ni1-x-yMnxCoy)O2-NMC-Based Batteries
by Jun Ji Nicholas Lim, Yi Cai and Madhavi Srinivasan
Energies 2025, 18(4), 974; https://doi.org/10.3390/en18040974 - 18 Feb 2025
Viewed by 853
Abstract
While 1 M LiPF6 has been widely adopted as the standard electrolyte in current LIBs, its chemical instability has reduced the battery’s cycling stability by, for instance, accelerating the dissolution of transition metals from electrode materials, particularly in high-voltage cathodes. Lithium bis(fluorosulfonyl)imide [...] Read more.
While 1 M LiPF6 has been widely adopted as the standard electrolyte in current LIBs, its chemical instability has reduced the battery’s cycling stability by, for instance, accelerating the dissolution of transition metals from electrode materials, particularly in high-voltage cathodes. Lithium bis(fluorosulfonyl)imide (LiFSI) has emerged as a promising alternative salt for next-generation high-voltage energy-dense LIB electrolytes. However, despite extensive research, the optimal concentration and formulation of LiFSI remain unresolved, with variations typically tested across different Li(Ni1-x-yMnxCoy)O2 (NMC) series cathodes. Herein, 6:4.5:8.3 LiFSI/EC/DMC (in molar ratio) is proposed as a universal electrolyte for high-voltage NMC series cathodes. The 6:4.5:8.3 LiFSI/EC/DMC electrolyte decomposes to form a uniform cathode–electrolyte interface with abundant inorganic species, resulting in a lower interface resistance. By adopting the 6:4.5:8.3 LiFSI/EC/DMC electrolyte, NMC series Li-ion half-cells are all able to stably cycle up to 200 cycles at a cut-off voltage of 4.4 V. Especially for high Ni content (NMC 811) cathode, the capacity retention was improved from 43.6% to 87.5% when charged to 4.4 V at 1C rate. This work provides a feasible universal electrolyte formulation for developing next-generation high-voltage LIBs. Full article
(This article belongs to the Section D: Energy Storage and Application)
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