Engineering π-Electron Bridge Enables Low-Potential 2D Redox Polymer Anodes for High-Voltage Aqueous All-Organic Batteries.

Here, we propose a novel π-electron bridge engineering strategy to explore a class of dioxin-bridged 2D redox covalent organic polymer (RCOP) as trade-off-breaking anodes for high-voltage aqueous all-organic batteries (AAOBs). By establishing a tunable RCOP platform, we perform theoretical study to scrutinize how bridge units between active sites affect the electrode potential and redox activity for the first time. We discover that compared to common pyrazine bridge, the weakened conjugation and strong electron donor character of the proposed dioxin bridge can induce elevated LUMO level and enriched π-electron populations in active sites, heralding a low electrode potential and enhanced redox activity. Besides, nonaromaticity induced molecular flexibility of dioxin bridge mitigates intermolecular stacking for sufficient active site exposure and charge carrier uptake. To experimentally corroborate this, a new dioxin-bridged RCOP (D-HATN) and its pyrazine-bridged analogue (P-HATN) are synthesized for proof-of-concept demonstration. Hence, D-HATN displays excellent compatibility with Na+/Zn2+/NH4+/H3O+ and obviously lower redox potentials in various electrolytes compared to P-HATN, while affording rapid Grotthuss-type proton conduction and unprecedented durability in acid. Thus,  the D-HATN-involved all-organic proton battery delivers an average output voltage of 0.75 V, which can be further elevated to 1.63 V with alkaline-acidic hybrid electrolyte design, affording markedly-increased specific energy.

Unveiling Organic Electrode Materials in Aqueous Zinc-Ion Batteries: From Structural Design to Electrochemical Performance.

Aqueous zinc-ion batteries (AZIBs) are one of the most compelling alternatives of lithium-ion batteries due to their inherent safety and economics viability. In response to the growing demand for green and sustainable energy storage solutions, organic electrodes with the scalability from inexpensive starting materials and potential for biodegradation after use have become a prominent choice for AZIBs. Despite gratifying progresses of organic molecules with electrochemical performance in AZIBs, the research is still in infancy and hampered by certain issues due to the underlying complex electrochemistry. Strategies for designing organic electrode materials for AZIBs with high specific capacity and long cycling life are discussed in detail in this review. Specifically, we put emphasis on the unique electrochemistry of different redox-active structures to provide in-depth understanding of their working mechanisms. In addition, we highlight the importance of molecular size/dimension regarding their profound impact on electrochemical performances. Finally, challenges and perspectives are discussed from the developing point of view for future AZIBs. We hope to provide a valuable evaluation on organic electrode materials for AZIBs in our context and give inspiration for the rational design of high-performance AZIBs.

Non-Metal Ion Storage in Zinc-Organic Batteries.

Zinc-organic batteries (ZOBs) are receiving widespread attention as up-and-coming energy-storage systems due to their sustainability, operational safety and low cost. Charge carrier is one of the critical factors affecting the redox kinetics and electrochemical performances of ZOBs. Compared with conventional large-sized and sluggish Zn2+ storage, non-metallic charge carriers with small hydrated size and light weight show accelerated interfacial dehydration and fast reaction kinetics, enabling superior electrochemical metrics for ZOBs. Thus, it is valuable and ongoing works to build better ZOBs with non-metallic ion storage. In this review, versatile non-metallic cationic (H+, NH4 +) and anionic (Cl-, OH-, CF3SO3 -, SO4 2-) charge carriers of ZOBs are first categorized with a brief comparison of their respective physicochemical properties and chemical interactions with redox-active organic materials. Furthermore, this work highlights the implementation effectiveness of non-metallic ions in ZOBs, giving insights into the impact of ion types on the metrics (capacity, rate capability, operation voltage, and cycle life) of organic cathodes. Finally, the challenges and perspectives of non-metal-ion-based ZOBs are outlined to guild the future development of next-generation energy communities.

High Sodium Ion Storage by Multifunctional Covalent Organic Frameworks for Sustainable Sodium Batteries.

Rechargeable sodium batteries hold great promise for circumventing the increasing demand for lithium-ion batteries (LIBs) and the limited supply of lithium. However, efficient sodium ion storage remains a great impediment in this field. In this study, we report the designed synthesis of a multifunctional two-dimensional covalent organic framework featuring hexaazatrinaphthalene cores linked by imidazole moieties and demonstrate its effective performance in sodium ion storage. Benzimidazole-linked covalent organic framework (BCOF-1) was synthesized by a condensation reaction between hexaazatrinaphthalenehexamine (HATNHA) and terephthalaldehyde (TA) and exhibited a high theoretical specific capacity of 392 mA h g-1. BCOF-1 crystallizes, forming eclipsed AA stacking and mesoporous hexagonal one-dimensional channels with high surface area (840 m2 g-1), facilitating fast ionic mobility and charge transfer and enabling high-rate capability at high current rates. BCOF-1 exhibits pseudocapacitive-like behavior with a high specific capacity of 387 mA h g-1, an energy density of 302 W h kg-1 at 0.1 C, and a power density of 682 W kg-1 at 5 C. Our results demonstrate that redox-active COFs have the desired structural and electronic merits to advance the use of organic electrodes in sodium-ion storage toward sustainable and efficient batteries.

Spatial Structure Design of Thioether-Linked Naphthoquinone Cathodes for High-Performance Aqueous Zinc-Organic Batteries.

Organic electrode materials (OEMs) have gathered extensive attention for aqueous zinc-ion batteries (AZIBs) due to their structural diversity and molecular designability. However, the reported research mainly focuses on the design of the planar configuration of OEMs and does not take into account the important influence of the spatial structure on the electrochemical properties, which seriously hamper the further performance liberation of OEMs. Herein, this work has designed a series of thioether-linked naphthoquinone-derived isomers with tunable spatial structures and applied them as the cathodes in AZIBs. The incomplete conjugated structure of the elaborately engineered isomers can guarantee the independence of the redox reaction of active groups, which contributes to the full utilization of active sites and high redox reversibility. In addition, the position isomerization of naphthoquinones on the benzene rings changes the zincophilic activity and redox kinetics of the isomers, signifying the importance of spatial structure on the electrochemical performance. As a result, the 2,2'-(1,4-phenylenedithio) bis(1,4-naphthoquinone) (p-PNQ) with the smallest steric hindrance and the most independent redox of active sites exhibits a high specific capacity (279 mAh g-1), an outstanding rate capability (167 mAh g-1 at 100 A g-1), and a long-term cycling lifetime (over 2800 h at 0.05 A g-1).

Selenium-Anchored Chlorine Redox Chemistry in Aqueous Zinc Dual-Ion Batteries.

Chlorine-based batteries with Cl0 to Cl- redox reaction (ClRR) are promising for high-performance energystorage due to their high redox potential and large theoretical capacity. However, the inherent gas-liquid conversion feature of ClRR together with poor Cl fixation can cause Cl2 leakage, reducing battery reversibility. Herein, we utilize a Se-based organic molecule, diphenyl diselenide (di-Ph-Se), as the Cl anchoring agent and realize an atomic level-Cl fixation through chalcogen-halogencoordinating chemistry. The promoted Cl fixation, with two oxidized Cl0 anchoring on a single Ph-Se, and the multivalence conversion of Se contributeto a six-electron conversion process with up to 507 mAh g-1 and an average voltage of 1.51 V, as well as a high energy density of 665 Wh Kg-1 . Based on the superior reversibility of thedeveloped di-Ph-Se electrode with ClRR, a remarkable rate performance (205 mAh g-1 at 5 A g-1 ) and cycling performance (capacity retention of 77.3 % after 500cycles) are achieved. Significantly, the pouch cell delivers a record arealcapacity of up to 6.87 mAh cm-2 and extraordinary self-discharge performance. This chalcogen-halogen coordination chemistry between the Se electrode and Cl provides a new insight for developing reversible and efficientbatteries with halogen redox reactions.

A Dithiin-Linked Covalent Organic Polymer for Ultrahigh Capacity Half-Cell and Symmetric Full-Cell Sodium-Ion Batteries.

Sodium ion-batteries (SIBs) are considered as a class of promising alternatives to lithium-ion batteries (LIBs) to overcome their drawbacks of limited sources and safety problems. However, the lack of high-performance electrode materials hinders the wide-range commercialization of SIBs. Comparing to inorganic counterparts, organic electrode materials, which are benefitted from flexibly designable structures, low cost, environmental friendliness, and high theoretical gravimetric capacities, should be a prior choice. Here, a covalent organic polymer (COP) based material (denoted as CityU-9) is designed and synthesized by integrating multiple redox motifs (benzoquinone and thioether), improved conductivity (sulfur induction), and intrinsic insolubility (rigid skeleton). The half-cell SIBs exhibit ultrahigh specific capacity of 1009 mAh g-1 and nearly no capacity drop after 650 cycles. The first all-COP symmetric full-cell shows high specific capacity of 90 mAh g-1 and excellent rate capability. This work can extend the selection of redox-active moieties and provide a rational design strategy of high-performance novel organic electrode materials.

Self-Reinforced Inductive Effect of Symmetric Bipolar Organic Molecule for High-Performance Rechargeable Batteries.

Herein, the self-reinforced inductive effect derived from coexistence of both p- and n-type redox-active motifs in a single organic molecule is presented. Molecular orbital energy levels of each motif are dramatically tuned, which leads to the higher oxidation and the lower reduction potentials. The self-reinforced inductive effect of the symmetric bipolar organic molecule, N,N'-dimethylquinacridone (DMQA), is corroborated, by both experimental and theoretical methods. Furthermore, its redox mechanism and reaction pathway in the Li+ -battery system are scrutinized. DMQA shows excellent capacity retention at the operating voltage of 3.85 and 2.09 V (vs Li+ /Li) when used as the cathode and anode, respectively. Successful operation of DMQA electrodes in a symmetric all-organic battery is also demonstrated. The comprehensive insight into the energy storage capability of the symmetric bipolar organic molecule and its self-reinforced inductive effect is provided. Thus, a new class of organic electrode materials for symmetric all-organic batteries as well as conventional rechargeable batteries can be conceived.

Influence of Backbone on the Performance of Pendant Polymer Electrode Materials in Li-ion Batteries.

Pendant polymers are a promising class of electrode materials due to their synthetic simplicity, derivation from sustainable feedstocks, and potentially benign synthesis. These materials consist of a redox-active pendant tethered to a polymer backbone, which mitigates dissolution during electrode cycling. To date, an extensive number of pendant groups have been studied within the context of metal-ion batteries. However, the choice of the polymer backbone and its impact on the electrode performance have been relatively understudied. In this work, we use a postpolymerization modification approach to synthesize a series of viologen-bearing redox-active pendant polymers with similar molecular weights but three distinct chemical backbones, namely, polyacrylamide, polymethacrylamide, and polystyryl. By evaluating the polymers in lithium-ion batteries, we show that the polymer backbone has a significant influence on electrode performance and behavior. Specifically, the polymethacrylamide displays slower kinetics than the other two polymers, resulting in lower capacities, particularly at high cycling rates. Furthermore, the charge storage mechanism is dependent on the nature of the backbone: the polyacrylamide shows a significant capacitive contribution to charge storage, while the polystyryl does not. The difference in performance between the polymer electrode materials is ascribed to a difference in chain mobility and packing within the electrode films. Overall, this work shows that the fundamental properties of the polymer backbone are critical to the design of high-performance polymer electrodes.

Unveiling the Role of Charge Dilution and Anionic Chemistry in Enabling High-Rate p-Type Polymer Cathodes for Dual-Ion Batteries.

Herein, we introduce a p-type redox conjugated covalent organic polymer (p-PNZ) as a universal and high-rate cathode for diverse dual-ion batteries. By constructing an n-type redox counterpart (n-PNZ) with an analogous reticular structure and redox-site composition, we also attain a comparative platform to probe how the redox-site nature and counterion chemistry affect the rate performance of polymer cathodes. It is disclosed that the charge dilution in p-type redox sites and bulky anions engenders their weak interaction and rapid anion diffusion in electrodes, while the trivial interaction of the solvent with anions facilitates anion desolvation and interfacial charge transfer. Thus, p-PNZ possesses rapid surface-controlled redox kinetics with a high anion diffusion coefficient regardless of its inferior porosity and conductivity relative to n-PNZ. Along with a long cycle life of over 50000 cycles, the p-PNZ-engaged Zn-based dual-ion battery with a dilute electrolyte delivers nearly constant capacities of ∼149 mAh g-1 at various rates of ≤10 A g-1─such an unusual rate capability has rarely been observed previously─and retains ∼99 mAh g-1 at 40 A g-1, surpassing the n-PNZ counterpart and most existing p-type organic cathodes. The p-PNZ cathode can also be applied to build high-rate Li-based batteries, signifying its universality, while the "ready-to-charge" character of p-PNZ enables anode-free dual-ion batteries with a high-rate capability and long lifespan.

Modulation of Radical Intermediates in Rechargeable Organic Batteries.

Organic materials have been considered as promising electrodes for next-generation rechargeable batteries in view of their sustainability, structural flexibility, and potential recyclability. The radical intermediates generated during the redox process of organic electrodes have profound effect on the reversible capacity, operation voltage, rate performance, and cycling stability. However, the radicals are highly reactive and have very short lifetime during the redox of organic materials. Great efforts have been devoted to capturing and investigating the radical intermediates in organic electrodes. Herein, this review summarizes the importance, history, structures, and working principles of organic radicals in rechargeable batteries. More importantly, challenges and strategies to track and regulate the radicals in organic batteries are highlighted. Finally, further perspectives of organic radicals are proposed for the development of next-generation high-performance rechargeable organic batteries.

Modified Viologen- and Carbonylpyridinium-Based Electrodes for Organic Batteries.

Efficient electrochemical energy storage has been identified as one of the most pressing needs for a sustainable energy economy. Inorganic battery materials have traditionally been the center of attention, with the current state-of-the-art device being the lithium-ion battery. Recent pursuits have led to organic materials for their beneficial chemistry and properties, but suitable materials for organic batteries are still few and far between. This Spotlight on Applications highlights two intriguing pyridinium-based organic materials, modified viologens and carbonylpyridiniums, that have both been successfully employed in electrode materials for solid-state Li-ion-type organic batteries (LOBs). We first provide an overview of the inherent electronic properties of each building block and how they can effectively be modified while maintaining or enhancing their desirable electrochemical properties for practical applications. We then describe a range of different material designs for a battery context and their application in various organic device settings, with some examples showing competitive performance with traditional Li-ion batteries.

In Situ Electrochemical Activation of Hydroxyl Polymer Cathode for High-Performance Aqueous Zinc-Organic Batteries.

The slow reaction kinetics and structural instability of organic electrode materials limit the further performance improvement of aqueous zinc-organic batteries. Herein, we have synthesized a Z-folded hydroxyl polymer polytetrafluorohydroquinone (PTFHQ) with inert hydroxyl groups that could be partially oxidized to the active carbonyl groups through the in situ activation process and then undertake the storage/release of Zn2+ . In the activated PTFHQ, the hydroxyl groups and S atoms enlarge the electronegativity region near the electrochemically active carbonyl groups, enhancing their electrochemical activity. Simultaneously, the residual hydroxyl groups could act as hydrophilic groups to enhance the electrolyte wettability while ensuring the stability of the polymer chain in the electrolyte. Also, the Z-folded structure of PTFHQ plays an important role in reversible binding with Zn2+ and fast ion diffusion. All these benefits make the activated PTFHQ exhibit a high specific capacity of 215 mAh g-1 at 0.1 A g-1 , over 3400 stable cycles with a capacity retention of 92 %, and an outstanding rate capability of 196 mAh g-1 at 20 A g-1 .

All-Graphene Quantum Dot-Derived Battery: Regulating Redox Activity Through Localized Subdomains.

In the quest for materials sustainability for grid-scale applications, graphene quantum dot (GQD), prepared via eco-efficient processes, is one of the promising graphitic-organic matters that have the potential to provide greener solutions for replacing metal-based battery electrodes. However, the utilization of GQDs as electroactive materials has been limited; their redox behaviors associated with the electronic bandgap property from the sp2 carbon subdomains, surrounded by functional groups, are yet to be understood. Here, the experimental realization of a subdomained GQD-based anode with stable cyclability over 1000 cycles, combined with theoretical calculations, enables a better understanding of the decisive impact of controlled redox site distributions on battery performance. The GQDs are further employed in cathode as a platform for full utilization of inherent electrochemical activity of bio-inspired redox-active organic motifs, phenoxazine. Using the GQD-derived anode and cathode, an all-GQD battery achieves a high energy density of 290 Wh kgcathode -1 (160 Wh kgcathode+anode -1 ), demonstrating an effective way to improve reaction reversibility and energy density of sustainable, metal-free batteries.

Two Birds One Stone: Graphene Assisted Reaction Kinetics and Ionic Conductivity in Phthalocyanine-Based Covalent Organic Framework Anodes for Lithium-ion Batteries.

This work reports a covalent organic framework composite structure (PMDA-NiPc-G), incorporating multiple-active carbonyls and graphene on the basis of the combination of phthalocyanine (NiPc(NH2 )4 ) containing a large π-conjugated system and pyromellitic dianhydride (PMDA) as the anode of lithium-ion batteries. Meanwhile, graphene is used as a dispersion medium to reduce the accumulation of bulk covalent organic frameworks (COFs) to obtain COFs with small-volume and few-layers, shortening the ion migration path and improving the diffusion rate of lithium ions in the two dimensional (2D) grid layered structure. PMDA-NiPc-G showed a lithium-ion diffusion coefficient (DLi + ) of 3.04 × 10-10 cm2 s-1 which is 3.6 times to that of its bulk form (0.84 × 10-10 cm2 s-1 ). Remarkably, this enables a large reversible capacity of 1290 mAh g-1 can be achieved after 300 cycles and almost no capacity fading in the next 300 cycles at 100 mA g-1 . At a high areal capacity loading of ≈3 mAh cm-2 , full batteries assembled with LiNi0.8 Co0.1 Mn0.1 O2 (NCM-811) and LiFePO4 (LFP) cathodes showed 60.2% and 74.7% capacity retention at 1 C for 200 cycles. Astonishingly, the PMDA-NiPc-G/NCM-811 full battery exhibits ≈100% capacity retention after cycling at 0.2 C. Aided by the analysis of kinetic behavior of lithium storage and theoretical calculations, the capacity-enhancing mechanism and lithium storage mechanism of covalent organic frameworks are revealed. This work may lead to more research on designable, multifunctional COFs for electrochemical energy storage.

Aqueous Organic Batteries Using the Proton as a Charge Carrier.

Benefiting from the merits of low cost, nonflammability, and high operational safety, aqueous rechargeable batteries have emerged as promising candidates for large-scale energy-storage applications. Among various metal-ion/non-metallic charge carriers, the proton (H+ ) as a charge carrier possesses numerous unique properties such as fast proton diffusion dynamics, a low molar mass, and a small hydrated ion radius, which endow aqueous proton batteries (APBs) with a salient rate capability, a long-term life span, and an excellent low-temperature electrochemical performance. In addition, redox-active organic molecules, with the advantages of structural diversity, rich proton-storage sites, and abundant resources, are considered attractive electrode materials for APBs. However, the charge-storage and transport mechanisms of organic electrodes in APBs are still in their infancy. Therefore, finding suitable electrode materials and uncovering the H+ -storage mechanisms are significant for the application of organic materials in APBs. Herein, the latest research progress on organic materials, such as small molecules and polymers for APBs, is reviewed. Furthermore, a comprehensive summary and evaluation of APBs employing organic electrodes as anode and/or cathode is provided, especially regarding their low-temperature and high-power performances, along with systematic discussions for guiding the rational design and the construction of APBs based on organic electrodes.

A Sulfur Heterocyclic Quinone Cathode Towards High-Rate and Long-Cycle Aqueous Zn-Organic Batteries.

Organic materials have attracted much attention in aqueous zinc-ion batteries (AZIBs) due to their sustainability and structure-designable, but their further development is hindered by the high solubility, poor conductivity, and low utilization of active groups, resulting in poor cycling stability, terrible rate capability, and low capacity. In order to solve these three major obstacles, a novel organic host, benzo[b]naphtho[2',3':5,6][1,4]dithiino[2,3-i]thianthrene-5,7,9,14,16,18-hexone (BNDTH), with abundant electroactive groups and stable extended π-conjugated structure is synthesized and composited with reduced graphene oxide (RGO) through a solvent exchange composition method to act as the cathode material for AZIBs. The well-designed BNDTH/RGO composite exhibits a high capacity of 296 mAh g-1 (nearly a full utilization of the active groups), superior rate capability of 120 mAh g-1 , and a long lifetime of 58 000 cycles with a capacity retention of 65% at 10 A g-1 . Such excellent performance can be attributed to the ingenious structural design of the active molecule, as well as the unique solvent exchange composition strategy that enables effective dispersion of excess charge on the active molecule during discharge/charge process. This work provides important insights for the rational design of organic cathode materials and has significant guidance for realizing ideal high performance in AZIBs.

A High-Rate and Long-Life Aqueous Rechargeable Mg-Ion Battery Based on an Organic Anode Integrating Diimide and Triazine.

Aqueous Mg-ion batteries (MIBs) lack reliable anode materials. This study concerns the design and synthesis of a new anode material - a π-conjugate of 3D-poly(3,4,9,10-perylenetracarboxylic diimide-1,3,5-triazine-2,4,6-triamine) [3D-P(PDI-T)] - for aqueous MIBs. The increased aromatic structure inhibits solubility in aqueous electrolytes, enhancing its structural stability. The 3D-P(PDI-T) anode exhibits several notable characteristics, including an extremely high rate capacity of 358 mAh g-1 at 0.05 A g-1 , A 3D-P(PDI-T)‖Mg2 MnO4 full cell exhibits a reversible capacity of 148 mAh g-1 and a long cycle life of 5000 cycles at 0.5 A g-1 . The charge storage mechanism reveals a synergistic interaction of Mg2+ and H+ cations with C-N/C=O groups. The assembled 3D-P(PDI-T)‖Mg2 MnO4 full cell exhibits a capacity retention of around 95 % after 5000 cycles at 0.5 A g-1 . This 3D-P(PDI-T) anode sustained its framework structure during the charge-discharge cycling of Mg-ion batteries. The reported results provide a strong basis for a cutting-edge molecular engineering technique to afford improved organic materials that facilitate efficient charge-storage behavior of aqueous Mg-ion batteries.

Design and Synthesis of a π-Conjugated N-Heteroaromatic Material for Aqueous Zinc-Organic Batteries with Ultrahigh Rate and Extremely Long Life.

Electroactive organic materials with tailored functional groups are of great importance for aqueous Zn-organic batteries due to their green and renewable nature. Herein, a completely new N-heteroaromatic material, hexaazatrinaphthalene-phenazine (HATN-PNZ) is designed and synthesized, by an acid-catalyzed condensation reaction, and its use as an ultrahigh performance cathode for Zn-ion batteries demonstrated. Compared with phenazine monomer, it is revealed that the π-conjugated structure of N-heteroaromatics can effectively increase electron delocalization, thereby improving its electrical conductivity. Furthermore, the enlarged aromatic structure noticeably suppresses its dissolution in aqueous electrolytes, thus enabling high structural stability. As expected, the HATN-PNZ cathode delivers a large reversible capacity of 257 mAh g-1 at 5 A g-1 , ultrahigh rate capability of 144 mAh g-1 at 100 A g-1 , and an extremely long cycle life of 45 000 cycles at 50 A g-1 . Investigation of the charge-storage mechanism demonstrates the synergistic coordination of both Zn2+ and H+ cations with the phenanthroline groups, with Zn2+ first followed by H+ , accompanying the reversible formation of zinc hydroxide sulfate hydrate. This work provides a molecular-engineering strategy for superior organic materials and adds new insights to understand the charge-storage behavior of aqueous Zn-organic batteries.

Molecular Engineering of Metalloporphyrins for High-Performance Energy Storage: Central Metal Matters.

Porphyrin derivatives represent an emerging class of redox-active materials for sustainable electrochemical energy storage. However, their structure-performance relationship is poorly understood, which confines their rational design and thus limits access to their full potential. To gain such understanding, we here focus on the role of the metal ion within porphyrin molecules. The A2 B2 -type porphyrin 5,15-bis(ethynyl)-10,20-diphenylporphyrin and its first-row transition metal complexes from Co to Zn are used as models to investigate the relationships between structure and electrochemical performance. It turned out that the choice of central metal atom has a profound influence on the practical voltage window and discharge capacity. The results of DFT calculations suggest that the choice of central metal atom triggers the degree of planarity of the porphyrin. Single crystal diffraction studies illustrate the consequences on the intramolecular rearrangement and packing of metalloporphyrins. Besides the direct effect of the metal choice on the undesired solubility, efficient packing and crystallinity are found to dictate the rate capability and the ion diffusion along with the porosity. Such findings open up a vast space of compositions and morphologies to accelerate the practical application of resource-friendly cathode materials to satisfy the rapidly increasing need for efficient electrical energy storage.