Storage Mechanism Research Articles

Multi-objective algorithm for hybrid microgrid energy management based on multi-agent system

In the dynamic landscape of renewable energies, microgrid systems emerge as a promising avenue for fostering sustainable local energy generation. However, the effective management of energy resources holds the key to unlocking their full potential. This study assumes the task of creating a multi-objective optimization algorithm for microgrid energy management. At its core, the algorithm places a premium on seamlessly integrating renewable energy sources and orchestrating efficient storage coordination. Leveraging the prowess of a multi-agent system, it allocates and utilizes energy resources. Through the combination of renewable sources, storage mechanisms, and variable loads, the algorithm promotes energy efficiency and ensures a steady power supply. This transformative solution is underscored by the algorithm's remarkable performance in practical simulations and validations across diverse microgrid scenarios, offering a prevue into the future of sustainable energy utilization.

Sputter Deposited Crystalline MoO2 Films as a High-Capacity and Stable Electrode Material for Supercapacitors: Mechanistic/Electrochemical Insights

In this work, we have optimized and fabricated pristine molybdenum dioxide (MoO2) electrodes over the Silicon (Si) substrate and examined the impact of various ion-loaded aqueous electrolytes on their electrochemical behavior. The sputtered electrodes exhibited a high crystalline structure and a very low resistivity. These highly conductive electrodes were tested in three different aqueous electrolytes (acidic, neutral, and alkaline) to establish a relation between the electrode and the nature of the electrolyte to achieve optimal electrochemical performance and cyclability. The electrochemical kinetics showed that the charge storage mechanism was unique for all the electrolytes. The capacitive current was dominant in the neutral electrolyte, whereas it was diffusive dominant in alkaline and 70% capacitive in the acidic electrolyte. Our findings indicated that the MoO2@Si electrode exhibited superior electrochemical activity in an acidic electrolyte. The electrode showed a voltage window of 0.6 V with an areal capacity of 24 mF/cm2 at 0.1 V/s scan rate. Moreover, the electrode also demonstrated excellent cyclability and capacitance retention (∼145%) till 5000 cycles. These results highlighted that the binder-free MoO2@Si electrode showed outstanding electrochemical activity and stability, which makes it suitable for sulfuric acid electrolyte-based energy storage systems.

Molecular heat transport across a time-periodic temperature gradient.

The time-periodic modulation of a temperature gradient can alter the heat transport properties of a physical system. Oscillating thermal gradients give rise to behaviors such as modified thermal conductivity and controllable time-delayed energy storage that are not present in a system with static temperatures. Here, we examine how the heat transport properties of a molecular lattice model are affected by an oscillating temperature gradient. We use analytical analysis and molecular dynamics simulations to investigate the vibrational heat flow in a molecular lattice system consisting of a chain of particles connected to two heat baths at different temperatures, where the temperature difference between baths is oscillating in time. We derive expressions for heat currents in this system using a stochastic energetics framework and a nonequilibrium Green's function approach that is modified to treat the nonstationary average energy fluxes. We find that emergent energy storage, energy release, and thermal conductance mechanisms induced by the temperature oscillations can be controlled by varying the frequency, waveform, and amplitude of the oscillating gradient. The developed theoretical approach provides a general framework to describe how vibrational heat transmission through a molecular lattice is affected by temperature gradient oscillations.

Zn2+-storage mechanism in V6O13 with nanosheets for high-capacity and long-life aqueous zinc-metal batteries.

V6O13 with a nanosheet structure was employed as a cathode material for aqueous zinc metal batteries. V6O13 delivered a high specific capacity of 425 mA h g-1, outstanding rate performance and durable cycling with high capacity retention of 86% after 3000 cycles. Moreover, in situ X-ray diffractometer (XRD), ex situ X-ray photoelectron spectroscopy (XPS) and X-ray absorption near-edge structure (XANES) were employed to ascertain the reaction mechanism of Zn2+ storage.

Advanced Structural Engineering Design for Tailored Microporous Structure via Adjustable Graphite Sheet Angle to Enhance Sodium‐Ion Storage in Anthracite‐Based Carbon Anode

AbstractCarbon material has emerged as a highly promising anode for sodium‐ion batteries (SIBs) due to its abundance of resources, cost‐effectiveness, and high carbon yield. This work elaborately designs the precursor structure for the self‐assembly of melamine‐cyanuric acid on the anthracite surface through hydrogen bonding, and successfully constructs N‐doped carbon with tailored microstructure and expanded interlayer spacing. Serving as anode for SIBs, the optimized sample delivers high specific capacity (371.3 mAh g−1 at 0.05 A g−1), superior rate capability (295.8 mAh g−1 at 10.0 A g−1), and excellent ultra‐long cycling performance (the retention of 91.5% after 3000 cycles at 0.5 A g−1). The systematic investigations reveal the enhancement of sodium‐ion storage in the low‐voltage plateau region involving the interlayer intercalation coupled with nanopores filling. It is discovered that the microporous structure formed by the appropriate graphite sheet angle influences the migration and storage of sodium ions. Density functional theory calculations indicate that the adsorption capacity for sodium ion is enhanced and the migration energy barrier perpendicular to the graphite layer is reduced at the appropriate angle of 8°. This study provides novel insights into the sodium‐ion storage mechanism, offering guidance for the better design of anthracite‐based carbon anode with superior performance.

Biomass-Derived Carbon Materials for Advanced Metal-Ion Hybrid Supercapacitors: A Step Towards More Sustainable Energy

Modern research has made the search for high-performance, sustainable, and efficient energy storage technologies a main focus, especially in light of the growing environmental and energy-demanding issues. This review paper focuses on the pivotal role of biomass-derived carbon (BDC) materials in the development of high-performance metal-ion hybrid supercapacitors (MIHSCs), specifically targeting sodium (Na)-, potassium (K)-, aluminium (Al)-, and zinc (Zn)-ion-based systems. Due to their widespread availability, renewable nature, and exceptional physicochemical properties, BDC materials are ideal for supercapacitor electrodes, which perfectly balance environmental sustainability and technological advancement. This paper delves into the synthesis, functionalization, and structural engineering of advanced biomass-based carbon materials, highlighting the strategies to enhance their electrochemical performance. It elaborates on the unique characteristics of these carbons, such as high specific surface area, tuneable porosity, and heteroatom doping, which are pivotal in achieving superior capacitance, energy density, and cycling stability in Na-, K-, Al-, and Zn-ion hybrid supercapacitors. Furthermore, the compatibility of BDCs with metal-ion electrolytes and their role in facilitating ion transport and charge storage mechanisms are critically analysed. Novelty arises from a comprehensive comparison of these carbon materials across metal-ion systems, unveiling the synergistic effects of BDCs’ structural attributes on the performance of each supercapacitor type. This review also casts light on the current challenges, such as scalability, cost-effectiveness, and performance consistency, offering insightful perspectives for future research. This review underscores the transformative potential of BDC materials in MIHSCs and paves the way for next-generation energy storage technologies that are both high-performing and ecologically friendly. It calls for continued innovation and interdisciplinary collaboration to explore these sustainable materials, thereby contributing to advancing green energy technologies.

Boosting potassium and sodium-ion storage performance by in-situ self-assembly of a Co-based π-d conjugated coordination polymer on graphene nanosheets

To obtain anode materials with good electrochemical performances in both potassium ion batteries (PIBs) and sodium-ion batteries (SIBs), a Co-based π-d conjugated coordination polymer (Co-HHTP) is in-situ assembled on graphene (G) nanosheets using a facile one-step solvothermal method. The resulting Co-HHTP/G composite shows improved electrochemical performances over pure Co-HHTP. After 300 cycles of using as an anode of PIBs/SIBs for the first time, the reversible specific capacity of the Co-HHTP/G composite is found to be 381/277 mAh g−1 at 100 mA g−1. After undergoing 500 cycles at 1000 mA g−1, the material's reversible specific capacities remain at 234/164 mAh g−1 for PIBs/SIBs. The improved performances of the Co-HHTP/G composite electrode are due to the incorporation of graphene. This incorporation not only reduces structural stacking and promotes active site utilization, but also increases electrical conductivity and structural stability. According to the ex-situ X-ray photoelectron spectrometer (XPS) spectra, the Co-HHTP/G's energy storage mechanism throughout the process of potassisation/depotassisation is found to be linked to the aromatic rings presented in the organic ligands.

A Unified Charge Storage Mechanism to Rationalize the Electrochemical Behavior of Quinone-Based Organic Electrodes in Aqueous Rechargeable Batteries.

Due to their eco-sustainability and versatility, organic electrodes are promising candidates for large-scale energy storage in rechargeable aqueous batteries. This is notably the case of aqueous hybrid batteries that pair the low voltage of a zinc anode with the high voltage of a quinone-based (or analogue of quinone-based) organic cathode. However, the mechanisms governing their charge-discharge cycles remain poorly understood and are even a matter of debate and controversy. No consensus exists on the charge carrier in mild aqueous electrolytes, especially when working in an electrolyte containing a multivalent metal cation such as Zn2+. In this study, we comprehensively investigate the electrochemical reactivity of two model quinones, chloranil, and duroquinone, either diluted in solution or incorporated into carbon-based composite electrodes. We demonstrate that a common nine-member square scheme proton-coupled electron transfer mechanism allows us to fully describe and rationalize their electrochemical behavior in relation to the pH and chemical composition of the aqueous electrolyte. Additionally, we highlight the crucial role played by the pKas associated with the reduced states of quinones in determining the nature of the charge carrier that compensates for the negative charges reversibly injected in the active material. Finally, contrary to the widely reported findings for Zn/organic batteries, we unequivocally establish that the predominant solid-state charge carriers in Zn2+-based mild aqueous electrolytes are not multivalent Zn2+ cations but rather protons supplied by the weakly acidic hexaaqua metal ions (i.e., [Zn(H2O)6]2+]).

Achieving Exceptional Volumetric Desalination Capacity Using Compact MoS2 Nanolaminates.

Capacitive deionization (CDI) has emerged as a promising technology for freshwater recovery from low-salinity brackish water. It is still inapplicable in specific scenarios (e.g., households, islands, or offshore platforms) due to too low volumetric adsorption capacities. In this study, we report a high-density semi-metallic molybdenum disulfide (1T'-MoS2) electrode with compact architecture obtained by restacking of exfoliated nanosheets, which achieved high capacitance up to ∼277.5 F cm-3 under an ultrahigh scan rate of 1000mV s-1 with a lower charge-transfer resistance and nearly ten-fold higher electrochemical active surface area than the 2H-MoS2 electrode. Furthermore, 1T'-MoS2 electrode demonstrates exceptional volumetric desalination capacity of 65.1 mgNaCl cm-3 in CDI experiments. Ex-situ X-ray diffraction (XRD) reveal that the cation storage mechanism with the dynamic expansion of 1T'-MoS2 interlayer to accommodate cations such as Na+, K+, Ca2+, and Mg2+, which in turn enhances the capacity. Theoretical analysis unveils that 1T' phase is thermodynamically preferable over 2H phase, the ion hydration and channel confinement also play critical role in enhancing ion adsorption. Overall, this work provides a new method to design compact two-dimensional layered nanolaminates with high volumetric performance for CDI desalination. This article is protected by copyright. All rights reserved.

Application of deep learning through group method of data handling for interfacial tension prediction in brine/CO2 systems: MgCl2 and CaCl2 aqueous solutions

Capillary/residual CO2 trapping is one of the main mechanisms of CO2 storage in underground formations. Therefore, it is required to estimate the brine/CO2 interfacial tension under different conditions. Although many methods have been proposed so far, the error of estimation is still high. This paper proposes a novel deep learning method to estimate the brine/CO2 interfacial tension at various temperatures, pressures, and salinities. The proposed method is a neural network with the Group Method of Data Handling (GMDH) learning method. The GMDH has the advantage of handling the structural and parametric optimization of the network automatically. The proposed method is tested on an experimental dataset of brine/CO2 interfacial tension with CalCl2 and MgCl2 salts. The results of the proposed method were compared with four of the best performing methods in the literature. The Average Absolute Percentage Error (AAPE) of the method on the training, testing and all data was 1.3 %, 2.95 %, 1.73 %, respectively, while the best method from the literature could reach an AAPE of 8.16 % on all data. Therefore, the proposed method performs far better than the existing methods. Also, a sensitivity analysis was done to determine the most influential inputs to estimate the output. The contribution of this work is to show the applicability of the GMDH method to construct more optimal data-driven models to estimate the brine/CO2 interfacial tension. Also, the utilized dataset is collected under a wide range of pressure, temperature and salinity conditions that increases the generality of the model.

Comprehensive Insights into Potassium‐Ion Capacitors: Mechanisms, Materials, Devices and Future Perspectives

AbstractAlkali metal‐ion capacitors integrate two electrodes from both batteries and supercapacitors (SCs), combining the advantages of large capacity, high‐rate performance, and long cycle life. Potassium (K) has similar properties to sodium (Na) and lithium (Li), however, the abundance of K in the crust is the same with Na, and much higher than Li. Due to the fast kinetics and low self‐discharge of Potassium‐ion capacitors (PICs), PICs attract more interest from researchers in the field of electrochemical energy storage. The current dilemma is that the research on PICs is more inherited from sodium‐ion capacitors (SICs) and lithium‐ion capacitors (LICs). Despite advancements in electrode materials, there is still a lack of profound understanding of the intrinsic issues and key challenges of PICs. In order to provide a detailed and systematic analysis of the development of PICs, in this review, special attention is given on the following Accordingly, full eight key sections: i) development history, ii) defining equations, iii) energy storage mechanism, iv) device configuration, v) electrode materials, vi) electrolyte design, vii) key technologies, and viii) future perspectives. This review provides an intensive theoretical foundation for the development of PICs and is able to pave the path for the practical application of PICs.

Facile Galvanic Replacement Construction of Bi@C Nanosheets Array as Binder‐Free Anodes for Superior Sodium‐Ion Batteries

AbstractBismuth (Bi) possesses an ultrahigh theoretical volume capacity (3800 mAh cm−3) and low embedding potential stimulated considerable attention as anodes for sodium‐ion batteries (SIBs). However, its practical application is still hampered by the huge volume variation during the charge/discharge process. To settle this issue, Bi@C nanosheet arrays (Bi@C‐NSA) are fabricated on copper foam via a facile galvanic replacement followed by in situ polymerization of dopamine and an annealing procedure. The carbon‐coated nanosheet array structure not only accommodates the volume expansion during cycling and maintains electrode stability, but also facilitates rapid electron/ion transport. Due to the unique structural design, this Bi@C‐NSA exhibits an impressive capacity of 315.72 mAh g−1 after 1500 cycles under 1 A g−1. Furthermore, a series of in situ/ex situ techniques reveal that this Bi@C‐NSA possesses superior reaction kinetics and undergoes a typical alloying/dealloying storage mechanism. Furthermore, Bi@C‐NSA also achieves commendable reversible capacity and cycling stability in a wide temperature range (0 °C–60 °C). Notably, the assembled Na3V2(PO4)3//Bi@C‐NSA full cell demonstrates a capacity of 325 mAh g−1 after 50 cycles at 0.05 A g−1, which promises for practical applications. This galvanic replacement strategy spearheads a way to prepare nanoarray electrodes and will accelerate the development of sodium‐ion batteries.

Outstanding Lithium Storage Performance of a Copper‐Coordinated Metal‐Covalent Organic Framework as Anode Material for Lithium‐Ion Batteries

Metal‐covalent organic frameworks (MCOF) as a bridge between covalent organic framework (COF) and metal organic framework (MOF) possess the characteristics of open metal sites, structure stability, crystallinity, tunability as well as porosity, but still in its infancy. In this work, a covalent organic framework DT‐COF with a keto‐enamine structure synthesized from the condensation of 3,3′‐dihydroxybiphenyl diamine (DHBD) and triformylphloroglucinol (TFP) was coordinated with Cu2+ by a simple post‐modification method to a obtain a copper‐coordinated metal‐covalent organic framework of Cu‐DT COF. The isomerization from a keto‐enamine structure of DT‐COF to a enol‐imine structure of Cu‐DT COF is induced due to the coordination interaction of Cu2+. The structure change of Cu‐DT COF induces the change of the electron distribution in the Cu‐DT COF, which greatly promotes the activation and deep Li‐storage behavior of the COF skeleton. As anode material for lithium‐ion batteries (LIBs), Cu‐DT COF exhibits greatly improved electrochemical performance, retaining the specific capacities of 760 mAh g−1 after 200 cycles and 505 mAh g−1 after 500 cycles at a current density of 0.5 A g−1. The preliminary lithium storage mechanism studies indicate that Cu2+ is also involved in the lithium storage process. A possible mechanism for Cu‐DT COF was proposed on the basis of FT‐IR, XPS, EPR characterization and electrochemical analysis. This work enlightens a novel strategy to improve the energy storage performance of COF and promotes the application of COF and MCOF in LIBs.

Interfacial bonding enhances MXene/Sb2Se3 composites toward cyclic stability and fast aluminum storage

Metal-chalcogenides have been extensively studied as electrode materials for rechargeable ion batteries due to their high theoretical specific capacity and high abundance. Although promising, these materials face challenges related to slow electrochemical kinetics, pronounced structural distortions, and severe shuttle effects. These issues have seriously hindered the practical application of metal-chalcogenides in ion batteries. This work presents a novel approach to form interfacial binding bonds and in situ generation of antimony selenide (Sb2Se3) on MXene by electrostatic adsorption. This innovative strategy enhances the reversible capacity and cycling stability of Sb2Se3 and effectively improves the electrochemical kinetics and shuttle effect. Ex-situ characterization elucidates the distinctive energy storage mechanism of the Ti3C2/Sb2Se3 cathode and the inhibitory effect of MXene on the dissolution of reaction intermediates into the electrolyte. Additionally, the improvement in charge transfer and ion diffusion due to the introduction of MXene was validated through density functional theory calculations. This work offers new insights into enhancing the stability of metal-chalcogenides and understanding the energy storage mechanism of antimony-based selenides in ion batteries.

Rapid fabrication of binder free nickel cobalt oxide electrodes with dendritic nanostructure for electrochemical energy storage applications

A rapid and facile technique to synthesize nickel cobalt oxide electrodes by photothermal treatment of mixed organometallic precursor solution is reported. Using short and intense pulses of light from a xenon flash lamp, spray coated films are converted into porous nickel cobalt oxide electrodes with dendritic nanostructure. The electrode films fabricated in a few seconds show excellent energy storage properties as supercapacitor electrodes. Specific capacitance of up to 116 Fg−1 and capacitance retention of up to 75 % were observed in samples with low mass loading. Analysis of the cyclic voltammetry (CV) curves shows that capacitance is the dominating charge storage mechanism in these films. To study the effect of varying the mass loading in electrodes, double and triple layered electrodes were also studied. In films with high mass loading, the specific capacitance of the films decreased but areal capacitance continued to increase. A high areal capacitance of up to 243 mFcm−2 is observed in films with high mass loading. CV curve analysis of high mass loading electrodes further shows that in films with higher mass loading, the charge storage mechanism is a mix of capacitance and diffusion processes. The contribution of diffusion increased with increase in the mass loading of the electrodes. This study sheds light into the mechanism of charge storage in electrodes prepared by large-scale-amenable single step process of photonic curing which could be utilized to fabricate electrodes in industrial scale.

Insights into pseudocapacitive mechanism of aqueous ammonium-ion supercapacitors with exceptional energy density and cyclability

Aqueous ammonium-ion (NH4+) supercapacitors (AASCs) have recently garnered increased concerns but are consistently facing the challenge of lower energy density. Herein, a high-performance electrode (CuCo2S4@CP) with pseudocapacitive property has been synthesized and primordially applied to AASCs. The CuCo2S4@CP electrode has an ultrahigh specific capacity of 1512 C g−1 at 1 A g−1 and a distinguished cyclic stability of 87.74 % after 10,000 cycles. When the CuCo2S4@CP electrode is combined with the activated carbon (AC) negative electrode, the CuCo2S4@CP//AC device exhibits a high specific capacity of 547 C g−1 at 1 A g−1, excellent cycle stability (83.28 % at 10 A g−1), high energy density of 74.17 Wh kg−1, and excellent device consistency. In addition, the charge transfer mechanism of CuCo2S4@CP electrode in NH4+electrolyte has been elucidated. The CuCo2S4 surface density functional theory (DFT) elucidates that NH4+ has a minimal contribution to the surface, implying an insertion behavior of NH4+ within the CuCo2S4 lattice. Subsequent ex-situ characterization further confirms the energy storage process, revealing charge transfer to Co atoms following NH4+ insertion into CuCo2S4. The analysis of charge distribution illustrates an energy storage mechanism wherein the hydrogen bond formed between NH4+ and CuCo2S4 serves as the transport channel for charge transfer, facilitating the process of electrons from NH4+ to Co atoms. Therefore, the pseudocapacitive mechanism of CuCo2S4 with NH4+ provides a blueprint for sustainable energy storage with high energy density in aqueous electrolyte.

Layer‑by‑layer assembled binder-free hydrated vanadium oxide-acetylene black electrode for flexible aqueous zinc ion battery

Vanadium oxides are potential positive electrode materials for aqueous zinc ion batteries (ZIBs) owing to their advantages of high theoretical capacity, low cost, and so on. Developments of methods for preparing binder-free vanadium oxide electrodes on a large scale and further investigation of their Zn2+ storage mechanisms are essential for expanding their uses in large-scale energy storage systems and wearable electronics. In this work, binder-free electrodes with hydrated vanadium oxide (V2O5·nH2O, denoted as VOH)-acetylene black (AB) on carbon cloth (VOH-AB/CC) are fabricated by a simple and scalable method which combined low-temperature hydrothermal treatment with layer-by-layer drop/spray-coating process. The AB can greatly improve the electrical conductivity of VOH, thereby enhancing the electrochemical performance. The as-prepared electrode with 20 wt% of AB (VOH-AB2/CC) delivers a high capacity of 280 mA h g−1 at 1 A/g and a good rate capability of 205 mA h g−1 at 4 A/g, which is better than many of the reported binder-free vanadium base electrodes. Besides, excellent cycling performance with 89 % retention rate after 3000 cycles at 4 A/g is achieved on the VOH-AB2/CC electrode. Furthermore, a storage mechanism of Zn2+/H+/H2O insertion accompanied by the formation of basic zinc salt precipitate during the discharging process is proposed by the aid of ex-situ XRD and XPS techniques. Additionally, the flexible Quasi-Solid-State ZIB constructed using VOH-AB/CC as positive electrode can work well at different bending states and two ZIBs connected in series can lighten a light-emitting diode even under bending state. This work provides a low-cost, time-saving, environmental-friendly and scalable method to fabricate binder-free hydrated vanadium oxide electrodes for flexible aqueous ZIBs.

Freestanding Ammonium Vanadate Composite Cathodes with Lattice Self-Regulation and Ion Exchange for Long-Lasting Ca-Ion Batteries.

Calcium-ion batteries (CIBs) have emerged as a promising alternative for electrochemical energy storage. The lack of high-performance cathode materials severely limits the development of CIBs. Vanadium oxides are particularly attractive as cathode materials for CIBs, and preinsertion chemistry is often used to improve their calcium storage performance. However, the room temperature cycling lifespan of vanadium oxides in organic electrolytes still falls short of 1000 cycles. Here, based on preinsertion chemistry, the cycling life of vanadium oxides is further improved by integrated electrode and electrolyte engineering. Utilizing a tailored Ca electrolyte, the constructed freestanding (NH4)2V6O16·1.35H2O@graphene oxide@carbon nanotube (NHVO-H@GO@CNT) composite cathode achieves a 305 mAh g-1 high capacity and 10000 cycles record-long life. Additionally, for the first time, a Ca-ion hybrid capacitor full cell is assembled and delivers a capacity of 62.8 mAh g-1. The calcium storage mechanism of NHVO-H@GO@CNT based on a two-phase reaction and the exchange of NH4 + and Ca2+ during cycling are revealed. The lattice self-regulation of V─O layers is observed and the layered vanadium oxides with Ca2+ pillars formed by ion exchange exhibit higher capacity. This work provides novel strategies to enhance the calcium storage performance of vanadium oxides via integrated structural design of electrodes and electrolyte modification.

Electropolymerization of a Carbonyl-Modified Dihydropyrazine Derivative for Aqueous Zinc Batteries with Ultrahigh Cycling Stability.

The design of aqueous zinc-ion batteries (ZIBs) that have high specific capacity and long-term stability is essential for future large-scale energy storage systems. Cathode materials with extended π-conjugation and abundant active sites are desirable to enhance the charge storage performance and the cycling stability of the aqueous ZIB. Based on this concept, 6,9-dihydropyrazino[2,3-g]quinoxaline-2,3,7,8(1H,4H)-tetrone was chosen as the monomer to be electropolymerized onto carbon cloth (PDHPQ-Tetrone/CC). When used as the cathode material for aqueous ZIBs, an exceptional cycling life (>20,000 cycles) at a current density of 10 A g-1 was achieved, with the specific capacity maintained at 82.8% and with the Coulombic efficiency at around 100% throughout cycling. At the charge-discharge current density of 0.1 A g-1, the ZIB with PDHPQ-Tetrone/CC achieved a high specific capacity of 248 mAh g-1. Kinetic analyses showed that both surface-capacitive-controlled processes and semi-infinite diffusion-controlled processes contribute to the stored charge. The charge storage mechanism was investigated with ex situ characterizations and involves the redox processes of carbonyl/hydroxyl and amino/imino groups coupled with insertion and extraction of both Zn2+ and H+.

Organic Electrode Materials for Energy Storage and Conversion: Mechanism, Characteristics, and Applications.

ConspectusLithium ion batteries (LIBs) with inorganic intercalation compounds as electrode active materials have become an indispensable part of human life. However, the rapid increase in their annual production raises concerns about limited mineral reserves and related environmental issues. Therefore, organic electrode materials (OEMs) for rechargeable batteries have once again come into the focus of researchers because of their design flexibility, sustainability, and environmental compatibility. Compared with conventional inorganic cathode materials for Li ion batteries, OEMs possess some unique characteristics including flexible molecular structure, weak intermolecular interaction, being highly soluble in electrolytes, and moderate electrochemical potentials. These unique characteristics make OEMs suitable for applications in multivalent ion batteries, low-temperature batteries, redox flow batteries, and decoupled water electrolysis. Specifically, the flexible molecular structure and weak intermolecular interaction of OEMs make multivalent ions easily accessible to the redox sites of OEMs and facilitate the desolvation process on the redox site, thus improving the low-temperature performance, while the highly soluble nature enables OEMs as redox couples for aqueous redox flow batteries. Finally, the moderate electrochemical potential and reversible proton storage and release of OEMs make them suitable as redox mediators for water electrolysis. Over the past ten years, although various new OEMs have been developed for Li-organic batteries, Na-organic batteries, Zn-organic batteries, and other battery systems, batteries with OEMs still face many challenges, such as poor cycle stability, inferior energy density, and limited rate capability. Therefore, previous reviews of OEMs mainly focused on organic molecular design for organic batteries or strategies to improve the electrochemical performance of OEMs. A comprehensive review to explore the characteristics of OEMs and establish the correlation between these characteristics and their specific application in energy storage and conversion is still lacking.In this Account, we initially provide an overview of the sustainability and environmental friendliness of OEMs for energy storage and conversion. Subsequently, we summarize the charge storage mechanisms of the different types of OEMs. Thereafter, we explore the characteristics of OEMs in comparison with conventional inorganic intercalation compounds including their structural flexibility, high solubility in the electrolyte, and appropriate electrochemical potential in order to establish the correlations between their characteristics and potential applications. Unlike previous reviews that mainly introduce the electrochemical performance progress of different organic batteries, this Account specifically focuses on some exceptional applications of OEMs corresponding to the characteristics of organic electrode materials in energy storage and conversion, as previously published by our groups. These applications include monovalent ion batteries, multivalent ion batteries, low-temperature batteries, redox flow batteries with soluble OEMs, and decoupled water electrolysis employing organic electrodes as redox mediators. We hope that this Account will make an invaluable contribution to the development of organic electrode materials for next-generation batteries and help to unlock a world of potential energy storage applications.