Large Areal Capacitance Research Articles

Quasi-Homogeneous Bromine Phase in Zinc-Bromine Batteries with Advanced Energy Efficiency and Energy Density

Abstract Regarding energy density, kinetics, and reversibility, the zinc-bromine batteries (ZBBs) exhibit advantages comparable to the conventional metal hydride nickel batteries as aqueous systems. However, the development of ZBBs has been impeded by two critical challenges: the self-discharge of Br-Br species cross-over and the short circuit caused by zinc dendrites. Achieving high energy density necessitates a large areal capacity electrode and tight battery assembly, which introduces additional hurdles. Addressing these challenges, we have successfully implemented a novel quasi-homogeneous bromine phase. Our optimized approach has realized ZBBs with a remarkable energy efficiency (EE) of 92.7% based on an areal capacity of 12 mA h cm-2 in a period duration of 13 h, an energy density of whole battery (EDB) of 80 W h L-1 with average EE of 92.5% for an extended cycle life of approximately 500 cycles, and a maximum EDB of 186 W h L-1 without pre-added zinc metal. This innovative work holds practical significance for developing ZBBs and providing insights and solutions to critical challenges.

Cation Adsorption Engineering Enables Dual Stabilizations for Fast‐Charging Zn─I2 Batteries

AbstractAqueous zinc‐iodine (Zn─I2) battery is a promising energy storage system due to its inherent safety, high theoretical capacity, sustainability, and cost‐effectiveness. However, the shuttle effect of polyiodide severely affects the stable loading of active iodine and even accelerates the corrosion of the Zn anode, thus impeding its further advancement. Herein, a unique trimethylsulfonium cation (TMS+) with strong adsorption is proposed to stabilize both the iodine cathode and Zn anode. Benefiting from the robust interaction between TMS+ and polyiodide, the electrolyte can effectively immobilize large‐capacity iodine in the form of oily precipitate, thus avoiding the shuttle effect of polyiodide and the Zn corrosion. Additionally, TMS+ can be preferentially adsorbed on various Zn facets, inducing an electrostatic shielding effect to inhibit Zn dendrite growth. Consequently, Zn anode can be stably cycled over 3400 h at 5 mA cm−2/5 mAh cm−2, and a large areal capacity of 2.71 mAh cm−2 as well as long‐life stability over 6400 cycles is achieved for Zn─I2 battery. Furthermore, cation adsorption engineering is practically utilized in pouch cells, realizing superior fast‐charging stability over 790 cycles. This electrolyte modification with dual stabilizations is anticipated to be applied to other metal‐iodine batteries as a cost‐effective, facile, and safe strategy.

Minimizing Undesired Side Reactions Induced by Nanoscale Conductive Carbon Enables Stable Cycling of Semi-Solid Li-Ion Full Batteries.

Semi-solid lithium-ion batteries (SSLIBs) based on "slurry-like" electrodes hold great promise to enable low-cost and sustainable energy storage. However, the development of the SSLIBs has long been hindered by the lack of high-performance anodes. Here the origin of low initial Coulombic efficiency (iCE, typically <60%) is elucidated in the graphite-based semi-solid anodes (in the non-flowing mode) and develop rational strategies to minimize the irreversible capacity loss. It is discovered that Ketjen black (KB), a nanoscale conductive additive widely used in SSLIB research, induces severe electrolyte decomposition during battery charge due to its large surface area and abundant surface defects. High iCEs up to 92% are achieved for the semi-solid graphite anodes by replacing KB with other low surface-area, low-defect conductive additives. A semi-solid full battery (LiFePO4 vs graphite, in the non-flowing mode) is further demonstrated with stable cycle performance over 100 cycles at a large areal capacity of 6 mAh cm-2 and a pouch-type semi-solid full cell that remains functional even when it is mechanically abused. This work demystifies the SSLIBs and provides useful physical insights to further improve their performance and durability.

A low-cost electrode based on Mg-Co double hydroxide for high energy density structural supercapacitors in civil engineering

In the field of construction, structural supercapacitors (SSCs) have been widely noticed due to their simultaneous functions of load-bearing and energy storage. Unfortunately, the currently available electrodes for SSCs are still aimed at application scenarios such as electronics and electric vehicles, and while their performance is good, they are not applicable to the construction sector, which is massive in scale and extremely cost-sensitive industry. Herein, after trade-off between cost and electrochemical performance, a novel low-cost 3D nanomaterial was designed through a facile approach aimed at increasing the areal energy density of SSCs. By growing Mg-Co double hydroxide nanomaterials directly on nickel foam, we achieved a large areal capacitance of 2577 mF/cm2 at 5 mA/cm2 (1136.7 F/g at 2.2 A/g). It also exhibits good cycling stability with a capacitance retention of 82.4 % after 10,000 cycles. In addition, SSCs using magnesium-cobalt double hydroxides achieves a high energy density of 285.6 μWh/cm3 at a power density of 6.31 mW/cm3, which is superior to previously reported structural devices. This demonstrates that Mg-Co double hydroxide electrode has good suitability with SSCs and effectively improves the areal energy density of SSCs. Our proposed method also provides a faster and more reliable pathway for low-cost electrode preparation in SSCs, which may lead to the development of a new generation of SSCs.

3D oxidation-resistant MXene electrode supported by softened wood toward high-performance flexible supercapacitors

With the rapid evolution of emerging electronics, MXene materials hold great potential in developing high-performance electrodes for energy storage devices. However, MXenes usually suffer from severe self-stacking, mechanical fragility and susceptibility to oxidation, greatly limiting their further applications. Herein, a simple yet potent strategy is proposed to solve the above challenges by constructing a 3D porous and oxidation-resistant MXene-ascorbic acid/flexible wood electrode (MVFW). FW is employed as a soft and porous framework to solve the self-stacking and mechanical fragility problems of MXenes, ensuring the continuously conductive pathways and rapid ion transport. Ascorbic acid (VC) is introduced to further inhibit the restacking of MXenes and protect them against oxidation, improving the accessibility of active sites/ions and oxidation-resistant stability (capacitance retention of 70 % even after 2 months) of the electrode. Such electrode possesses an intrinsic flexibility with remarkable tensile strength (0.66 MPa) and toughness (0.96 MJ m−3), excellent electrical conductivity (5.4 S cm−1), large areal capacitance (1301 mF cm−2 at 5 mA cm−2) and high rate performance (75 %). The symmetric flexible supercapacitor demonstrates a notable energy density (13.9 μWh cm−2 at 139.7 μW cm−2) and favorable stability after 10,000 cycles or under bending at various angles (30°, 90° and 120°). This study opens up a promising path for the development of flexible, porous and oxidation-resistant MXene electrodes for next-generation wearable energy devices.

Electrodeposition of Graphene/Polypyrrole Electrode for Flexible Supercapacitor with Large Areal Capacitance

Electrodeposition of Graphene/Polypyrrole Electrode for Flexible Supercapacitor with Large Areal Capacitance

Efficient gradient heating-up approach for rapid growth of high-quality amorphous ZrO2 dielectric films

High-k oxide dielectric films are indispensable for low-power-consumption oxide thin-film transistors (TFTs) applied in advanced and portable electronics. However, high-quality oxide dielectric films prepared by solution process typically require sophisticated processes and long thermal annealing time, severely limiting both the throughput manufacturing and cost-effectiveness. In this study, the influence of different heating-up methods on the surface morphology and dielectric properties was systematically investigated. Gradient heating-up method could not only substantially improve the surface morphology and quality of high-k ZrO2 films but also efficiently shorten the annealing time. The gradient heating-up process was further designed on the basis of thermal behavior of the xerogel-like precursor, which successfully realize the preparation of high-quality ZrO2 films with an annealing time of 5 min (i.e. the efficiency of thermal treatment increased by about 89%). The ZrO2 film presented excellent dielectric properties, including a low leakage current density of ∼10−8 A cm−2 (at 2 MV cm−1 ), a large areal capacitance of 169 nF cm−2 and a high dielectric constant of 20.41 (1 MHz). Furthermore, InSnZnO TFT based on the ZrO2 gate dielectrics shows an acceptable device performances, such as a high carrier mobility of 2.82 cm2 V−1 s, a high on/off current ratio of ∼105 and a low subthreshold swing of 0.19 V decade −1 at a low operation voltage of 5 V. This work provide a highly promising approach to fabricate high-quality solution-processed high-k oxide dielectric films employed for large-scale and low-power-consumption electronics.

Multifunctional Heterostructured Fe3O4-FeTe@MCM Electrocatalyst Enabling High-Performance Practical Lithium-Sulfur Batteries Via Built-in Electric Field.

The development of capable of simultaneously modulating the sluggish electrochemical kinetics, shuttle effect, and lithium dendrite growth is a promising strategy for the commercialization of lithium-sulfur batteries. Consequently, an elaborate preparation method is employed to create a host material consisting of multi-channel carbon microspheres (MCM) containing highly dispersed heterostructure Fe3O4-FeTe nanoparticles. The Fe3O4-FeTe@MCM exhibitsa spontaneous built-in electric field (BIEF) and possesses both lithophilic and sulfophilic sites, rendering it an appropriate host material for both positive and negative electrodes. Experimental and theoretical results reveal that the existence of spontaneous BIEF leads to interfacial charge redistribution, resulting in moderate polysulfide adsorption which facilitates the transfer of polysulfides and diffusion of electrons at heterogeneous interfaces. Furthermore, the reduced conversion energy barriers enhanced the catalytic activity of Fe3O4-FeTe@MCM for expediting the bidirectional sulfur conversion. Moreover, regulated Li deposition behavior is realized because of its high conductivity and remarkable lithiophilicity. Consequently, the battery exhibited long-term stability for 500 cycles with 0.06% capacity decay per cycle at 5 C, and a large areal capacity of 7.3mAhcm-2 (sulfur loading: 9.73mgcm-2) at 0.1 C. This study provides a novel strategy for the rational fabrication of heterostructure hosts for practical Li-S batteries.

Sustained Release-Driven Interface Engineering Enables Fast Charging Lithium Metal Batteries.

LiNO3 has attracted intensive attention as a promising electrolyte additive to regulate Li deposition behavior as it can form favorable Li3N, LiNxOy species to improve the interfacial stability. However, the inferior solubility in carbonate-based electrolyte restricts its application in high-voltage Li metal batteries. Herein, an artificial composite layer (referred to as PML) composed of LiNO3 and PMMA is rationally designed on Li surface. The PML layer serves as a reservoir for LiNO3 release gradually to the electrolyte during cycling, guaranteeing the stability of SEI layer for uniform Li deposition. The PMMA matrix not only links the nitrogen-containing species for uniform ionic conductivity but also can be coordinated with Li for rapid Li ions migration, resulting in homogenous Li-ion flux and dendrite-free morphology. As a result, stable and dendrite-free plating/stripping behaviors of Li metal anodes are achieved even at an ultrahigh current density of 20mA cm-2 (>570h) and large areal capacity of 10 mAh cm-2 (>1200h). Moreover, the Li||LiFePO4 full cell using PML-Li anode undergoes stable cycling for 2000 cycles with high-capacity retention of 94.8%. This facile strategy will widen the potential application of LiNO3 in carbonate-based electrolyte for practical LMBs.

Stretchable Zn‐Ion Hybrid Capacitor with Hydrogel Encapsulated 3D Interdigital Structure

AbstractTo enhance the areal energy density of current flexible energy storage devices, hybrid capacitors combining the advantages of supercapacitors and batteries are proposed and further enhanced by incorporating the 3D interdigital structure design. However, uneven electric field distribution and hindered ion diffusion kinetics due to the non‐electroactive components in these devices limit the enhancement of areal electrochemical performances when expanding the electrodes longitudinally. Herein, hydrogels with high ionic conductivity and high mechanical stability are designed to accommodate Zn2+‐containing electrolytes and integrated with Ti3C2Tx‐MXene electrodes to assemble flexible Zn‐ion hybrid capacitors (ZIHCs). Fully encapsulated by ionic conductive hydrogels, 3D interdigital electrodes enable omnidirectional ion transport and unimpeded ionic accessibility, facilitating adequate electrode reactions, rapid energy storage, and uniform energy distribution. Hence, the all‐hydrogel‐encapsulated ZIHC achieved a 50‐fold increase in capacitance with a quadrupled electrode thickness, exhibiting a large areal capacitance of 1432 mF cm−2 and an energy density of 389.7 µWh cm−2 without sacrificing power density and rate performance. Finite element simulations further illustrate the uniform distribution of potential, electric field intensity, and energy density in this structure. In addition, the device shows great stability under deformation, excellent adhesion, and underwater workability, demonstrating great promise for next‐generation wearable energy storage devices.

Selective Shielding of the (002) Plane Enabling Vertically Oriented Zinc Plating for Dendrite-Free Zinc Anode.

Uncontrolled growth of Zn dendrites hinders the future development of aqueous Zn-ion batteries. Despite that the (100) plane possesses better zincophilic ability and fast kinetics, dendrites are generally suppressed via (002) plane-oriented Zn deposition in previous reports; the ordered (100) plane-dominant Zn deposition, especially under high current density has not yet been realized. Herein, vertically-oriented Zn plating with preferential growth of (100) plane is reported using disodium lauryl phosphate (DLP) as an electrolyte additive. DLP is preferentially anchored on the Zn (002) crystal plane via the polar phosphate group, then the deposition of Zn atoms on the (002) plane is retarded by the long alkyl chain, finally promoting the preferred growth of the (100) plane. This unique growth pattern results in ultrastable Zn plating/stripping at a super-high current density of 50mA cm-2 , with a cumulative capacity of 8500 mAh cm-2 . The Zn//Zn symmetric cell also cycles steadily for 700h with a large areal capacity of 10 mAh cm-2 at a current density of 10mA cm-2 . This study provides new insights into the realization of dendrite-free Zn anodes by crystal plane modulation.

Spontaneous Built-In Electric Field in C3N4-CoSe2 Modified Multifunctional Separator with Accelerating Sulfur Evolution Kinetics and Li Deposition for Lithium-Sulfur Batteries.

The discovery of the heterostructures that is combining two materials with different properties has brought new opportunities for the development of lithium sulfur batteries (LSBs). Here, C3N4-CoSe2 composite is elaborately designed and used as a functional coating on the LSBs separator. The abundant chemisorption sites of C3N4-CoSe2 form chemical bonding with polysulfides, provides suitable adsorption energy for lithium polysulfides (LiPSs). More importantly, the spontaneously formed internal electric field accelerates the charge flow in the C3N4-CoSe2 interface, thus facilitating the transport of LiPSs and electrons and promotingthe bidirectional conversion of sulfur. Meanwhile, the lithiophilic C3N4-CoSe2 sample with catalytic activity can effectively regulate the uniform distribution of lithium when Li+ penetrates the separator, avoiding the formation of lithium dendrites in the lithium (Li) metal anode. Therefore, LSBs based on C3N4-CoSe2 functionalized membranes exhibit a stable long cycle life at 1C (with capacity decay of 0.0819% per cycle) and a large areal capacity of 10.30mAhcm-2 at 0.1C (sulfur load: 8.26mgcm-2, lean electrolyte 5.4µLmgs -1). Even under high-temperature conditions of 60°C, a capacity retention rate of 81.8% after 100 cycles at 1C current density is maintained.

High capacity and dendrite-free Zn anode enabled by zincophilic 3D Sn-C nanowire framework

Aqueous zinc-ion batteries, due to their safety and low cost, are considered one of the most promising candidates for aqueous zinc-ion battery. However, the rampant dendrite growth of Zn has severely impacted the cycle life of the battery. Herein, we have designed a zincophilic 3D Sn-modified carbon fiber network (Sn-C) as an artificial interface layer framework on the anode surface. This Sn-C nanonetwork can guide the uniform growth of Zn, reducing notorious dendritic growth, and the interlayer growth pattern accommodates the volumetric expansion caused by the large areal capacity deposition. The assembled symmetric batteries have cycled for over 2000 h at 5 mAh cm−2 and 10 mAh cm−2, and even at large areal capacities of 20 mAh cm−2 and 50 mAh cm−2, the batteries have still cycled for over 300 h.

NbN quantum dots anchored hollow carbon nanorods as efficient polysulfide immobilizer and lithium stabilizer for Li-S full batteries

The shuttle effect of lithium polysulfides (LiPSs) and uncontrollable lithium dendrite growth seriously hinder the practical application of lithium-sulfur (Li-S) batteries. To simultaneously address such issues, monodispersed NbN quantum dots anchored on nitrogen-doped hollow carbon nanorods (NbN@NHCR) are elaborately developed as efficient LiPSs immobilizer and Li stabilizer for high-performance Li-S full batteries. Density functional theory (DFT) calculations and experimental characterizations demonstrate that the sulfiphilic and lithiophilic NbN@NHCR hybrid can not only efficiently immobilize the soluble LiPSs and facilitate diffusion-conversion kinetics for alleviating the shuttling effect, but also homogenize the distribution of Li+ ions and regulate uniform Li deposition for suppressing Li-dendrite growth. As a result, the assembled Li-S full batteries (NbN@NHCR-S||NbN@NHCR-Li) deliver excellent long-term cycling stability with a low decay rate of 0.031% per cycle over 1000 cycles at high rate of 2 C. Even at a high S loading of 5.8 mg cm−2 and a low electrolyte/sulfur ratio of 5.2 µL mg−1, a large areal capacity of 6.2 mA h cm−2 can be achieved in Li-S pouch cell at 0.1 C. This study provides a new perspective via designing a dual-functional sulfiphilic and lithiophilic hybrid to address serious issues of the shuttle effect of S cathode and dendrite growth of Li anode.

High-Areal Capacity, High-Rate Lithium Metal Anodes Enabled by Nitrogen-Doped Graphene Mesh.

Hosts hold great prospects for addressing the dendrite growth and volume expansion of the Li metal anode, but Li dendrites are still observable under the conditions of high deposition capacity and/or high current density. Herein, a nitrogen-doped graphene mesh (NGM) is developed, which possesses a conductive and lithiophilic scaffold for efficient Li deposition. The abundant nanopores in NGM can not only provide sufficient room for Li deposition, but also speed up Li ion transport to achieve a high-rate capability. Moreover, the evenly distributed N dopants on the NGM can guide the uniform nucleation of Li so that to inhibit dendrite growth. As a result, the composite NGM@Li anode shows satisfactory electrochemical performances for Li-S batteries, including a high capacity of 600 mAh g-1 after 300 cycles at 1 C and a rate capacity of 438 mAh g-1 at 3 C. This work provides a new avenue for the fabrication of graphene-based hosts with large areal capacity and high-rate capability for Li metal batteries.

Improved capacitive performance of polypyrrole-based composite hydrogel for flexible self-powered sensing system

Developing all-gel supercapacitors with high capacitance and stretchability remains a challenge. Herein, high mass of electroactive anthraquinonemonosulfonate(AQS)-doped polypyrrole (PPy) nanoparticles templated by poly(vinyl alcohol) (PVA) have been loaded into poly(acrylic acid) (PAA) hydrogel. The extra energy storage of AQS significantly enhances the electrochemical performance of the obtained PPy-AQS-PVA/PAA hydrogel electrodes. As a result, the assembled symmetrical supercapacitor can deliver a large areal specific capacitance of 392.5 mF/cm2, a high energy density of 34.89 μWh/cm2 and an enhanced cycling performance with 118% capacitance retention after 5000 CV cycles. Besides, such a device can work normally under various deformations and at extreme temperatures. Notably, the PPy-AQS-PVA/PAA hydrogels exhibit sustainable sensing capability for strain. When integrated the flexible supercapacitor with the strain sensor, a promising self-powered sensing system can monitor both large and subtle human movements accurately. Therefore, the multifunctional conductive PPy-AQS-PVA/PAA hydrogels have great potential in flexible electronic devices.

Salting-Out Effect Realizing High-Strength and Dendrite-Inhibiting Cellulose Hydrogel Electrolyte for Durable Aqueous Zinc-Ion Batteries.

Aqueous zinc-ion batteries are limited by poor Zn stripping/plating reversibility. Not only can hydrogel electrolytes address this issue, but also they are suitable for constructing flexible batteries. However, there exists a contradiction between the mechanical strength and the ionic conductivity for hydrogel electrolytes. Herein, high-concentration kosmotropic ions are introduced into the cellulose hydrogel electrolyte to take advantage of the salting-out effect. This can significantly improve both the mechanical strength and ionic conductivity. Additionally, the obtained cellulose hydrogel electrolyte (denoted as Con-CMC) has strong adhesion, a wide electrochemical stability window, and good water retaining ability. The Con-CMC is also found to accelerate the desolvation process, improve Zn deposition kinetics, promote Zn deposition along the (002) plane, and suppress parasitic reactions. Accordingly, the Zn/Zn cell with Con-CMC demonstrates dendrite-free behavior with prolonged lifespan and can endure extremely large areal capacity of 25 mAh cm-2. The Con-CMC also enables a large average Coulombic efficiency of 99.54% over 500 cycles for the Zn/Cu cell. Furthermore, the assembled pouch-type Zn/polyaniline full battery provides great rate capability, superior cyclability (even with limited Zn anode excess), a slow self-discharge rate, and outstanding affordability to external forces. Overall, this work extends our knowledge of the rational design of hydrogel electrolytes.

Unique Octupolar 2D‐Polymer Frameworks as Mixed Conductors and Metal‐Free Catalysts for Dual‐Promoted Li and S Electrochemistry: Multi‐regulation Role of Ethoxylation Chemistry

Here, we for the first time introduce ethoxylation chemistry to develop a new octupolar cyano‐vinylene‐linked 2D polymer framework (Cyano‐OCF‐EO) capable of acting as efficient mixed electron/ion conductors and metal‐free sulfur evolution catalysts for dual‐promoted Li and S electrochemistry. Our strategy creates a unique interconnected network of strongly‐coupled donor 3‐(acceptor‐core) octupoles in Cyano‐OCF‐EO, affording enhanced intramolecular charge transfer, substantial active sites and crowded open channels. This enables Cyano‐OCF‐EO as a new versatile separator modifier, which endows the modified separator with superior catalytic activity for sulfur conversion and rapid Li ion conduction with the high Li+ transference number up to 0.94. Thus, the incorporation of Cyano‐OCF‐EO can concurrently regulate sulfur redox reactions and Li‐ion flux in Li‐S cells, attaining boosted bidirectional redox kinetics, inhibited polysulfide shuttle and dendrite‐free Li anodes. The Cyano‐OCF‐EO‐involved Li‐S cell is endowed with excellent overall electrochemical performance especially large areal capacity of 7.5 mAh cm–2 at high sulfur loading of 8.7 mg cm–2. Mechanistic studies unveil the dominant multi‐promoting effect of the triethoxylation on electron and ion conduction, polysulfide adsorption and catalytic conversion as well as previously‐unexplored ‐CN/C‐O dual‐site synergistic effect for enhanced polysulfide adsorption and reduced energy barrier toward Li2S conversion.

Ultra-thick, dense dual-encapsulated Sb anode architecture with conductively elastic networks promises potassium-ion batteries with high areal and volumetric capacities

Ultra-thick, dense alloy-type anodes are promising for achieving large areal and volumetric performance in potassium-ion batteries (PIBs), but severe volume expansion as well as sluggish ion and electron diffusion kinetics heavily impede their widespread application. Herein, we design highly dense (3.1 ​g ​cm−3) Ti3C2Tx MXene and graphene dual-encapsulated nano-Sb monolith architectures (HD-Sb@Ti3C2Tx-G) with high-conductivity elastic networks (1560 ​S ​m−1) and compact dually encapsulated structures, which exhibit a large volumetric capacity of 1780.2 ​mAh cm−3 (gravimetric capacity: 565.0 ​mAh g−1), a long-term stable lifespan of 500 cycles with 82% retention, and a large areal capacity of 8.6 ​mAh cm−2 (loading: 31 ​mg ​cm−2) in PIBs. Using ex-situ SEM, in-situ TEM, kinetic investigations, and theoretical calculations, we reveal that the excellent areal and volumetric performance mechanism stems from the three dimensional (3D) high-conductivity elastic networks and the dual-encapsulated Sb architecture of Ti3C2Tx and graphene; these effectively mitigate against volume expansion and the pulverization of Sb, offering good electrolyte penetration and rapid ionic/electronic transmission. Ti3C2Tx also decreases the K+ diffusion energy barrier, and the ultra-thick compact electrode ensures volumetric and areal performance. These findings provide a feasible strategy for fabricating ultra-thick, dense alloy-type electrodes to achieve high areal and volumetric capacity energy storage via highly-dense, dual-encapsulated architectures with conductive elastic networks.

In Situ Synthesis Method of Approaching High Surface Capacity Sulfur and the Role of Cobalt Sulfide as Lithium–Sulfur Battery Materials

Lithium–sulfur batteries (Li–S) are potentially applicable in electrification and the replacement of fossil fuels due to the high energy density and the economy of sulfur. However, effectively an insulator, sulfur is known to suffer from inert electrochemical and poor conductivity. By synthetically incorporating conductive, low‐dimensional carbonaceous composites acting as both containment hosts and catalysts to active materials, this work entails an effective and straightforward materials engineering approach in fundamentally remodeling active materials utilization and activation. This synthetic‐based approach highlights direct processing capabilities than traditional thermal infusion processes without compromising performance and addresses the low activation, poor conductivity as well as alleviating side reactions due to polysulfide species. Motivated by recent efforts in excellent catalytic properties of cobalt sulfide (CoS)‐based materials, in this work, high‐performance CoS‐based carbonaceous composites are designed and employed, alleviating side reactions. These sulfide‐based catalysts are further elucidated in their role in facilitating charge/discharge of active materials, and assessed on practical polysulfide and side reaction alleviation with respect to various discharge/charge states. Proof‐of‐concept devices demonstrate the following performance highlights: 1) high‐performance stability, 2) strong polysulfide adsorption capability and kinetic characteristics, 3) large and workable areal capacity, and active materials loading.