Li-ion Batteries Research Articles

Effect analysis on the low-temperature preheating performance of a novel micro-combustor air preheater for the cold start of the Li-ion battery packs

In this work, a micro-combustor (MC) air preheater as the heat source is developed. This novel air preheater has a compact size and outputs hot air with a wide range of temperatures with high temperature uniformity, which can well meet the preheating needs of Li-ion batteries in cold environments. Numerical studies are carried out to investigate the effects of baffle height, number of fins Nfin, hot air inlet velocity, cold air inlet velocity and combustor inlet velocity on the performance of the air preheater. The heating power of the air preheater can be adjusted by changing combustor inlet velocity Vcombustor, the outlet temperature can be easily adjusted by changing cold air inlet velocity Vcold and hot air inlet velocity Vhot, and the addition of baffles makes the outlet temperature very uniform. The results show that the height of the baffle of 20 mm and 30 mm makes ΔTair not exceed 1.5 K. The air preheater performance is better with fin number 6, and the maximum air temperature of 309.8 K is obtained with fin number and Vhot of 6 and 0.3 m/s respectively. Tair can vary between 287.8 K and 309.8 K when Vcombustor=12 m/s.

Porous activated carbon integrated carbon nitride nanosheets as functionalized separators for the efficient polysulfide entrapment in Li[sbnd]S batteries

Electrification of vehicles, hybrid aircraft and the advancement of portable electronics are exacting the deployment of high energy-dense batteries. The high theoretical capacity of sulfur (1675 mAh g−1), cost-effectiveness and environmental benignity of the lithium‑sulfur batteries (LSBs) are propitious for electrochemical energy storage beyond Li-ion battery technology. In this work, we described a simple, scalable preparation and electrochemical performance of porous activated carbon (PC)-infused graphitic carbon nitride (GCN) nanosheets with various ratios (PC@GCN 11, PC@GCN 12 and PC@GCN 21) as a polysulfide anchoring functionalized separator for LSBs. The high specific area (822 m2/g), hetero porosity, conductive carbon framework, surface functionalities and enriched N-doping of the PC@GCN synergistically induce mitigation of polysulfides via chemical and physical adsorption pathways in LSBs. The PC@GCN 21 modified separator demonstrates a high initial discharge capacity of 1389 mAh g−1 at a 0.1C rate and exhibits better capacity retention over 500 cycles at a 1C rate (655 mAh g−1) with sulfur loading of 3.8 mg/cm2 accompanied by high coulombic efficiency (94 %). The assembled cell with high S-loading (5.12 mg/cm2) shows a high initial discharge capacity of 712 mAh g−1 at 0.1C rate conditions. High Li-ion transference number (0.714), stable shuttle current, minimal coulombic efficiency loss (0.84 %), low shuttle factor and negligible self-discharge behaviour support the superior performance of the PC@GCN 21 coated cells. This report demonstrates that combining the high surface area, non-polar porous carbon with polar graphitic carbon nitride is a practical approach for designing metal-free functionalized separators for energy-dense LSBs.

Recent advances in polyaniline/graphene nanocomposites for supercapacitor applications: Synthesis, properties, and future directions

Electrochemical capacitors or supercapacitors have attracted the attention of researchers and industries in the recent past because of the differences in the features and potential applications in comparison to the Li-ion batteries. Supercapacitors have been one of the most investigated applications in literature based on graphene-related materials. This review aims to provide the most recent advancement on the use of graphene and polyaniline (PANI) nanocomposite towards enhancing the supercapacitor properties. The synthesis methods of the graphene and PANI nanocomposite, the characteristics of the nanocomposite and its utilization in supercapacitors are discussed. Graphene and PANI are both well-known materials that possess fascinating physical and electrochemical characteristics, and in the last several years, they have been investigated for numerous applications by many researchers. Together with such advantages as enhanced physical and electrochemical characteristics, mechanical strength, and density, composites of both materials can be a potent material for supercapacitor usage.The preparation methods of graphene, PANI, and its composites described by the authors of the research article include in-situ polymerization, chemical vapor deposition, and hydrothermal-assisted polymerization. These characterization techniques include SEM, TEM, FTIR, XRD, DSC, and TGA to determine other properties of the nanocomposite which shows enhanced properties of graphene and PANI. The electrochemical properties of the nanocomposites are evaluated through cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD) and the achieved values indicate high specific capacitance, cycling stability, and charge-discharge abilities. These outcomes demonstrate the excellent applicability of PANI/graphene nanocomposites as high-performance supercapacitors and encourage the confidence in the effectiveness of the study. Several factors affecting properties of the nanocomposites have been reported in the previous studies, and it is clear from this study how various properties and their relation affects the overall performance of the nanocomposite. Altogether, PANI/graphene nanocomposites have the potential to be used as next-generation supercapacitors, which is still unexplored fully to meet the demands to enhance the high-performance energy storage devices.

Artificial Electron Channels Enable Contact Prelithiation of Li-Ion Battery Anodes with Ultrahigh Li-Source Utilization.

Contact prelithiation is widely used for compensating the initial capacity loss of lithium-ion batteries (LIBs). However, the low Li-source utilization suffering from the deteriorated contact interfaces results in cycling degeneration. Herein, Li-Ag alloy-based artificial electron channels (AECs) are established in Li source/graphite anode contact interfaces to promote Li-source conversion. Due to the shielding effect of the Li-Ag alloy (50 at. % Li) on Li-ion diffusion, the dry-state corrosion of contact interfaces is restricted. The unblocked electronic conduction across the AEC-involved interface not only facilitates the Li source conversion but also accelerates the prelithiation kinetics during the wet-state process, resulting in an ultrahigh Li-source utilization (90.7%). Thereby, implementing AEC-assisted prelithiation in a LiNi0.5Co0.2Mn0.3O2 pouch cell yields a 35.8% increase in energy density and stable cycling over 600 cycles. This finding affords significant insights into the construction of an efficient prelithiation technology toward the development of high-energy LIBs.

Biomass-based three-dimensional network porous carbon anodes derived from discontinuous activation for high performance Li-ion batteries

An approach of discontinuous activation and frozon-dry pretreatment toward a three-dimensional network porous carbon was proposed by using apple as the carbon source. The porous carbon, characterized by its high surface area and abundant porosity, was optimized through the manipulation of temperature and activator quantities during the activation process. The sample obtained by first calcining at 500 °C and then at 800 °C shows ultra-high rate electrochemical performance of over 900 mA h g−1 after 100 cycles and over 500 mA h g−1 after 500 cycles under the condition of charging and discharging current density of 0.2 A g−1 due to the high porosity. It is ascribed to the unique porous structure that can make the electrolyte and lithium ion transport and path short on the surface and inside the electrode material, further enhance its fast transport ability. The described approach represents an innovative and potentially impactful method for producing porous carbon electrodes with excellent electrochemical performance, particularly in the context of high-rate capability lithium-ion batteries.

Hydrothermal overprinting of the Li-rich strata deposited in the Mesoproterozoic Wumishan Formation, Hebei Province, North China

Lithium (Li), as a strategic critical metal, plays a pivotal role in the emerging energy landscape, particularly in the context of Li-ion batteries driving the new energy economy. Recently, Li-rich strata (with Li2O > 0.3 wt%) have been discovered in the Mesoproterozoic Wumishan Formation in Hebei Province, North China, suggesting a prospective Li reservoir. This study investigates these Li-rich strata using geochemical and in-situ micro-analytical techniques to explore the occurrence of Li and the formation mechanism of Li-host minerals, aiming for a comprehensive understanding of the supernormal enrichment of Li. The Li-rich samples are predominantly composed of dolomite and quartz, followed by clay minerals such as illite, interstratified illite–smectite (I/S), and chlorite, with minor amounts of K-feldspar, albite, biotite, calcite, baryte, fluorite and fluorapatite. In-situ analysis and 7Li NMR spectroscopy reveal that Li predominantly occupies the octahedral sites within the structures of authigenic illite and I/S, while its absence in clastic illite, clastic chlorite, unaltered K-feldspar, and dolomite. The presence of veined minerals (e.g., fluorite, baryte, and calcite) and a strong positive correlation between Li and F imply that post-depositional hydrothermal fluids have significantly contributed to the formation of Li-host minerals. The paragenesis of these minerals suggests that Li-bearing illite has formed through the hydrothermal alteration of K-feldspar. These Li-bearing illites subsequently transformed into Li-bearing I/S, consisting of illite-rich I/S and smectite-rich I/S, under continuous hydrothermal alteration. Lithium could have been leached from the surrounding carbonate rock and tuff through water–rock interaction and subsequently enriched by post-depositional hydrothermal fluids in specific regions, leading to mineralization. These findings provide valuable insights for targeting exploration of this promising Li resource.

Metal-ligand redox in layered oxide cathodes for Li-ion batteries

Metal-ligand redox in layered oxide cathodes for Li-ion batteries

Enhanced structural stability of Si electrode employing TiNi/Si pillars with oriented Li diffusion pathway

As the anode materials of Li-ion batteries, pillar-shaped TiNi/Si particles fabricated by employing electrochemical etching of (100) Si wafers and TiNi alloy coating, were investigated for their structural and electrochemical properties. The most suitable porous wafer for producing Si pillars was obtained at a current density of 2.5 mA/cm2 during etching. The deposited TiNi alloy film consisted of a crystallized austenitic (B2) phase capable of inducing phase transformation through annealing at 500°C. Particularly, by coating with the inactive materials, only the (100) plane of single crystalline Si was exposed during the initial charging process to restrict Li ion movement exclusively along the <100>Si direction. The TiNi/Si electrode exhibited a lower capacity compared to the Si electrode but demonstrated improved cycling performance. It showed a charge capacity of 1110 mAh/g at 0.1 C with an initial efficiency of 77 % and maintained a capacity retention of 49 % (543 mAh/g) up to 100 cycles. After the initial cycle, Si electrodes exposed to various lithium insertion directions exhibited severe structural damage such as cracking and particle pulverization, whereas TiNi/Si electrodes demonstrated enhanced structural stability due to surface coating and restricted reaction pathway.

Wet-Chemical Synthesis of a Protective Coating on NCM111 Cathode: The Quantified Effects of Washing, Sintering and Coating

LiNixCoyMn1-x-yO2 (NCM) cathodes, especially with high Ni content, are widely expected to keep advancing the energy density of Li-ion batteries. However, ensuring a good cycle life remains a key challenge. Applying inert protective coatings on the surface of NCMs is a common route for mitigating surface-based degradation. In this study a sustainable ethanol-based wet-chemical coating method for covering the material with Al2O3 is developed and demonstrated on NCM111. The effect of the synthesis procedure is carefully evaluated to distinguish the benefits of the protective coating from the contributions of re-sintering and removal of surface contaminants, all taking place during the synthesis of the coated material. We show that while the cycling stability is significantly improved by the material regeneration alone (65% vs 79% state-of-health after 500 charge-discharge cycles at voltage range 2.7–4.3 V vs Li/Li+), the Al2O3-coated material displays further cycle life gains, maintaining 88% of initial capacity after 500 charge-discharge cycles. This work thus demonstrates both a sustainable wet-chemical coating method and the importance of establishing a proper baseline for characterization of inert protective coatings in general. The importance of both gains further prominence with the transition to inherently less stable higher Ni content NCMs.

Visualizing and Quantifying Electronic Accessibility in Composite Battery Electrodes using Electrochemical Fluorescent Microscopy

Electronic connections between active material particles and the conductive carbon binder domain govern high-energy commercial Li-ion batteries' rate capability and lifetime (LIB). This work develops an in situ electrochemical fluorescent microscopy (EFM) technique that maps fluorescence intensity to these local electronic connections. Specifically, rapid redox kinetics of an electrofluorophore translates to reaction distributions limited by the electronic accessibility of battery electrode regions and individual active material particles. This technique can visualize hot spots, dead zones, and isolated particles on the electrode surface. EFM characterization of a series of LiNi0.33Mn0.33Co0.33O2 electrodes across processing parameters finds a significant negative correlation between the number of disconnected active particles and the rate capability. This low-cost technique provides quantitative mesoscale characterization of commercial LIB electrodes with fast throughput (<60 s) to facilitate rapid research and development and provide manufacturing quality control.

Manufacturing lithium-ion anodes from silicon recovered from end-of-life solar panels

With the rapid growth of solar energy, the recycling or re-use of used solar panels has become a key issue. Recycling high-value photovoltaic silicon from solar cells is an important step towards achieving “carbon neutrality.” In this paper, an efficient and high-value recycling strategy is employed to convert recycled silicon from discarded solar cells into lithium-ion anode materials. In this case, the recycled PV silicon is etched with hydrofluoric acid (HF) to create a porous silicon structure. This structure is designed to withstand the expansion stress of the electrodes. After surface modification with citric acid and carbon nanotubes to enhance the electrical conductivity of the recycled silicon and buffer the electrode from stress expansion during lithium storage and release, lithium difluorooxalate borate was added to pre-treat the surface of the recycled photovoltaic silicon through heat treatment. This process creates a robust and fast lithium-ion conductive interface enriched with LiF, Li2C2O4, LiBO2, and Li2B4O7. Density Functional Theory (DFT) calculations were performed to investigate the electronic structure of the synthesized materials, revealing their remarkable electronic conductivity and atomic bonding characteristics. When used as an anode for Li-ion batteries, W-pSi@C/CNTs exhibited high initial coulombic efficiency with stable cycling, demonstrating a capacity of 2040 mAh/g at 0.2 A/g for 200 cycles. In addition, this high-value recycling will help promote the development of renewable energy in an economically and environmentally sustainable manner.

Ion solvation modulating via Imidazolidinyl urea additive for stable Zn2+ deposition

The development of energy conversion and storage equipment is a necessary guarantee for social development, and aqueous Zn-ion batteries have become a promising alternative to Li-ion batteries due to its high safety, environmental friendliness, and low cost. However, aqueous Zn-ion batteries suffer from the dendrite growth and parasitic reactions, which hinder the wide application of the batteries. In this paper, imidazolidinyl urea (IDU) is added to aqueous electrolytes because of the special structural properties of IDU. The effects of IDU as an additive on battery stability are elucidated through theoretical modelling, calculations, and experimental validation. Firstly, the effect of concentration on the ion transport properties of the electrolyte was obtained by modelling and calculating the Zn2+ diffusion coefficient and ionic conductivity of electrolytes with different concentrations of IDU added. In addition, the optimal IDU addition concentration was achieved by verification of cycling experiments in Zn symmetric cells. Moreover, it was confirmed using in situ deposition experiments that the addition of IDU could participate in the coordination of Zn2+ into the solvated layer of Zn2+, thereby accelerating the desolvation process of Zn2+, and further improving the uneven deposition of Zn on the negative electrode surface and the growth of dendrites. Finally, it was verified that the IDU addition could enhance the cycle life and stability of the battery, maintaining an efficiency of about 95% and a specific capacity of discharge of 90 mAh·g-1 after more than 1000 cycles in a full cell assembled from Zn flakes and improved iodine electrodes.

Supplying active lithium to single-crystal Li(Ni0.90Co0.05Mn0.05)0.98Ta0.02O2 with Li2MnO3 coating served as cathode for Li-ion batteries

Ni-rich layered oxide with Ni molar content larger than 90% was regarded as an extremely promising candidate for cathode material applied in lithium-ion batteries owing to the significant discharging capacity and low cost. Nevertheless, rigorous cycling attenuation resulted from the crystal structure collapse and unstable particles interface deeply restrained the commercial application. In the work, LiNi0.90Co0.05Mn0.05O2 was modified by Ta5+ doping and Li2MnO3 covering, which was aimed to enhance the structure stability, defend the electrolyte attacking and promote Li+ migration during cycling. The material characterization demonstrated the cathodes after Ta5+ doping delivered the larger cell lattice parameters and higher cation ordering, which was helpful to improve the rate property and discharge capacity at low temperature. The Li2MnO3 layer was tightly adhered on the outside of LiNi0.90Co0.05Mn0.05O2, which could effectively relieve the electrolyte attacking and sustain the particle morphology integrity. As a result, 2wt.% Li2MnO3 coated Li(Ni0.90Co0.05Mn0.05)0.98Ta0.02O2 exhibited the outstanding discharge capacity of 150.2 mAh g−1 at 10.0 large current density and 140.6 mAh g−1 at -30 °C as well as the remarkable capacity retention of 93.1% after 300 cycles. Meanwhile, the pouch full batteries obtained by 2wt.% Li2MnO3 coated Li(Ni0.90Co0.05Mn0.05)0.98Ta0.02O2 also showed the more stable storage capability, cyclic property in comparison with bare LiNi0.90Co0.05Mn0.05O2.

Quantification of solvent-mediated host-ion interaction in graphite intercalation compounds for extreme-condition Li-ion batteries

Achieving simultaneous fast-charging capabilities and low-temperature adaptability in graphite-based lithium-ion batteries (LIBs) with an acceptable cycle life remains challenging. Herein, an ether-based electrolyte with temperature-adaptive Li+ solvation structure is designed for graphite, and stable Li+/solvent co-intercalation has been achieved at subzero. As revealed by in-situ variable temperature (−20 ℃) X-ray diffraction (XRD), the poor compatibility of graphite in ether-based electrolyte at 25 ℃ is mainly due to the continuous electrolyte decomposition and the in-plane rearrangement below 0.5 V. Former results in a significant irreversible capacity, while latter maintains graphite in a prolonged state of extreme expansion, ultimately leading to its exfoliation and failure. In contrast, low temperature triggers the rearrangement of Li+ solvation structure with stronger Li+/solvent binding energy and shorter Li+–O bond length, which is conducive for reversible Li+/solvent co-intercalation and reducing the time of graphite in an extreme expansion state. In addition, the co-intercalation of solvents minimizes the interaction between Li-ions and host graphite, endowing graphite with fast diffusion kinetics. As expected, the graphite anode delivers about 84% of the capacity at room temperature at −20 ℃. Moreover, within 6 min, about 83%, 73%, and 43% of the capacity could be charged at 25, −20, and −40 ℃, respectively.

A diffuse interface model for electro-chemo-mechanical systems

Electro-chemo-mechanics plays a critical role in the performance and longevity of energy storage systems, such as lithium-ion batteries and hydrogen energy storage. These systems involve multi-material composites comprising both liquid and solid phases, with their behavior influenced by processes in the bulk phases and at their interfaces.Traditional multi-phase theoretical and numerical models often adopt a discrete representation of material interfaces, introducing discontinuities in the problem’s fields. The numerical implementation is carried out using special interface elements, a methodology that requires conformal meshes and is not always supported by open-source computing platforms.This paper introduces a novel modeling framework that employs a diffuse representation of material interfaces, inspired by the phase-field method. From a modeling perspective, this approach allows for the consistent coupling of bulk and interface electro-chemo-mechanical processes, adhering to thermodynamic principles. Numerically, the proposed model is particularly suited for simulating real material microstructures using regular meshes, facilitating advanced numerical implementations.The methodology is detailed for a generic multi-material electro-chemo-mechanical system and applied specifically to Li-ion batteries. Numerical examples demonstrate the model’s effectiveness in simulating coupled interface processes without resorting to interface elements. This work provides a significant advancement in the simulation of electro-chemo-mechanical systems, offering a robust tool for studying the complex interplay of bulk and interface processes.

Influence of 3D Structural Design on the Electrochemical Performance of Aluminum Metal as Negative Electrode for Li-Ion Batteries.

Aluminum (Al) is one of the most promising active materials for producing next-generation negative electrodes for lithium (Li)-ion batteries. It features low density, high specific capacity, and low working potential, making it ideal for producing energy-dense cells. However, this material loses its electrochemical activity within 100 cycles, making it practically unusable. Several claims in the literature support the idea that a dual degradation mechanism is at play. First, the slow diffusion of Li in the Al matrix causes the electrochemical reactions to be partly irreversible, making the initial capacity of the cell drop. Second, the stress caused by cycling make the active material pulverize and lose activity. Recent work shows that shortening the diffusion path of Li by 3D structuring is an effective way to mitigate the first capacity loss mechanism, while alloying Al with other elements effectively mitigates the second one. In this work, we demonstrate that the benefits of 3D structuring and alloying are cumulative and that a mesh made of an Al-magnesium alloy performs better than both a pure Al foil and a foil of an Al-Mg alloy.

Aspects of Spodumene Lithium Extraction Techniques

Lithium (Li), a leading cathode material in rechargeable Li-ion batteries, is vital to modern energy storage technology, establishing it as one of the most impactful and strategical elements. Given the surge in the electric car market, it is crucial to improve lithium recovery from its rich mineral deposits using the most effective extraction technique. In recent years, both industry and academia have shown significant interest in Li recovery from various Li-bearing minerals. Of these, only extraction from spodumene has established a reliable industrial production of Li salts. The current approaches for cracking of the naturally occurring, stable α-spodumene structure into a more open structure—β-spodumene—involve the so-called decrepitation process that takes place at extreme temperatures of ~1100 °C. This conversion is necessary, as β-spodumene is more susceptible to chemical attacks facilitating Li extraction. In the last several decades, many techniques have been demonstrated and patented to process hard-rock mineral spodumene. The objective of this review is to present a thorough analysis of significant findings and the enhancement of process flowsheets over time that can be useful for both research endeavors and industrial process improvements. The review focuses on the following techniques: acid methods, alkali methods, carbonate roasting/autoclaving methods, sulfuric acid roasting/autoclaving methods, chlorinating methods, and mechanochemical activation. Recently, microwaves (MWs), as an energy source, have been employed to transform α-spodumene into β-spodumene. Considering its energy-efficient and short-duration aspects, the review discusses the interaction mechanism of MWs with solids, MW-assisted decrepitation, and Li extraction efficiencies. Finally, the merits and/or disadvantages, challenges, and prospects of the processes are summarized.

Modeling of Li-ion Battery Management System for Unmanned Aerial Vehicles

Nowadays, systems that use more electricity in aircraft are increasing due to harmful gas emissions. This increase has created the need to store electrical energy and accelerated the trend towards battery technologies. Since energy storage in batteries occurs as a result of chemical reactions, problems may occur that will damage the battery group or the entire system. These problems are caused by high current, voltage, and temperature, which affect the reaction rate during battery charging/discharging. A Battery Management System (BMS) is needed to prevent problems and to use the required electrical energy safely. In this study, it is aimed to meet the energy needs of the system in a controlled manner by disabling only the damaged cell in case of problems that may occur in the cells in the battery. For this purpose, a model of an Unmanned Aerial Vehicle (UAV) system been created by adding a BMS block to each cell to control the battery cells. The BMS model is realized based on the cell temperature, the State of Charge (SoC) value of the cell, and the output voltage values of the cell. The UAV system is modeled using MATLAB/Simulink environment. Thanks to the proposed BMS, in case of a problem that may occur in any cell in the battery, that cell will be disabled and the required energy will be met through the remaining cells. It is observed from the results obtained that when the cell parameters become normal, it continues to feed the system again.

Supramolecular-driven construction of multilayered structure by modified hummers method for robust silicon anode

Rational design of nano-structured silicon (Si)-based composites to enhance the structural stability and electrical conductivity is key to developing high-performance lithium-ion batteries. Here, a supramolecular self-assembly strategy is first adopted to prepare Si@rGO composites with multilayered structure through the modified Hummers method. Experimental results demonstrate that Si@SiOx NPs are uniformly distributed in rGO interlayers by supramolecular interaction. In situ Raman results suggest that the multilayer embedded structure can effectively confine the Si NPs and preserve the integrity of the electrode. Theoretical calculations indicate that the imbalanced charge distribution in inner interface shows enhanced dual-interfacial bonding and charge interactions in the Si@SiOx⊂rGO composite, resulting in an interfacial electric-field between Si NPs and rGO for fast ionic and charge migration. The fabricated MSi@SiOx⊂rGO anode with high Si contents (> 60 wt.% Si) exhibits superior Li-ion reaction kinetics (882.4 mAh g−1 at 8 A g−1), durable structural stability (0.031% per cycle capacity attenuation with an average Coulombic efficiency > 99.7%), and low expansion rate. High-mass-loading electrodes show great potential for commercial applications. Full cells assembled with LiCoO2 cathodes also demonstrate outstanding Li-ion storage properties. This work provides insights into the interfacial design of Si@C anodes for advanced Li-ion battery.

Machine learning-based design of electrocatalytic materials towards high-energy lithium||sulfur batteries development

The practical development of Li | |S batteries is hindered by the slow kinetics of polysulfides conversion reactions during cycling. To circumvent this limitation, researchers suggested the use of transition metal-based electrocatalytic materials in the sulfur-based positive electrode. However, the atomic-level interactions among multiple electrocatalytic sites are not fully understood. Here, to improve the understanding of electrocatalytic sites, we propose a multi-view machine-learned framework to evaluate electrocatalyst features using limited datasets and intrinsic factors, such as corrected d orbital properties. Via physicochemical characterizations and theoretical calculations, we demonstrate that orbital coupling among sites induces shifts in band centers and alterations in the spin state, thus influencing interactions with polysulfides and resulting in diverse Li-S bond breaking and lithium migration barriers. Using a carbon-coated Fe/Co electrocatalyst (synthesized using recycled Li-ion battery electrodes as raw materials) at the positive electrode of a Li | |S pouch cell with high sulfur loading and lean electrolyte conditions, we report an initial specific energy of 436 Wh kg−1 (whole mass of the cell) at 67 mA and 25 °C.