High-capacity dilithium hydroquinone cathode material for lithium-ion batteries.

Lithiated organic cathode materials show great promise for practical applications in lithium-ion batteries owing to their Li-reservoir characteristics. However, the reported lithiated organic cathode materials still suffer from strict synthesis conditions and low capacity. Here we report a thermal intermolecular rearrangement method without organic solvents to prepare dilithium hydroquinone (Li2Q), which delivers a high capacity of 323 mAh g-1 with an average discharge voltage of 2.8 V. The reversible conversion between orthorhombic Li2Q and monoclinic benzoquinone during charge/discharge processes is revealed by in situ X-ray diffraction. Theoretical calculations show that the unique Li-O channels in Li2Q are beneficial for Li+ ion diffusion. In situ ultraviolet-visible spectra demonstrate that the dissolution issue of Li2Q electrodes during charge/discharge processes can be handled by separator modification, resulting in enhanced cycling stability. This work sheds light on the synthesis and battery application of high-capacity lithiated organic cathode materials.

Sustainable Aqueous Batteries Based on Bipolar Dissociation of Aluminum Hydroxyacetate Electrolyte.

Rechargeable aqueous batteries are potential systems for large-scale energy storage due to their high safety and low cost. However, developing aqueous batteries with high sustainability, affordability, and reversibility is urgent and challenging. Here we report an amphoteric aluminum hydroxyacetate (AlAc(OH)2) electrolyte with the ability of bipolar ionization of H+ and OH-, which facilitates the redox reactions at both the anthraquinone (AQ) anode and nickel hydroxide (Ni(OH)2) cathode. The bipolar ionization ability of the AlAc(OH)2(H2O)3 solvation structure results from the strong polarization ability of Al3+ and OH-. The H+/OH- dissociation ability with a dissociation constant of 5.0/3.0 is stronger than that of water (14.0), which boosts the simultaneous stable redox reactions of electrodes. Specifically, H+ uptake prevents the AQ anode from the formation of an ionic bond, suppressing the electrode dissolution, whereas OH- provides the local alkaline environment for the stable conversion reaction of the Ni(OH)2 cathode. The AQ anode in the designed AQ||Ni(OH)2 battery delivers a discharge capacity of 243.9 mAh g-1 and a capacity retention of 78.2% after 300 cycles with high reversibility. Moreover, a pouch cell with a discharge capacity of 0.90 Ah was assembled, exhibiting an energy density of 44.7 Wh kg-1 based on the total mass of the battery. This work significantly widens the types of aqueous batteries and represents a design philosophy of bipolar electrolytes and distinct electrochemical reactions with H+ and OH-.

Lattice Strained Induced Spin Regulation in Co-N/S Coordination-Framework Enhanced Oxygen Reduction Reaction.

Oxygen reduction reaction (ORR) is the bottleneck of metal-air batteries and fuel cells. Strain regulation can change the geometry and adjust the surface charge distribution of catalysts, which is a powerful strategy to optimize the ORR activity. The introduction of controlled strain to the material is still difficult to achieve. Herein, we present a temperature-pressure-induced strategy to achieve the controlled lattice strain for metal coordination polymers. Through the systematic study of the strain effect on ORR performance, the relationship between geometric and electronic effects is further understood and confirmed. The strained Co-DABDT (DABDT=2,5-diaminobenzene-1,4-dithiol) with 2 % lattice compression exhibits a superior half-wave potential of 0.81 V. Theoretical analysis reveals that the lattice strain changes spin-charge densities around S atoms for Co-DABDT, and then regulates the hydrogen bond interaction with intermediates to promote the ORR catalytic process. This work helps to understand the catalytic mechanism from the atomic level.

Reliable Organic Carbonyl Electrode Materials Enabled by Electrolyte and Interfacial Chemistry Regulation.

ConspectusLithium-ion batteries (LIBs) have achieved great success and dominated the market of portable electronics and electric vehicles owing to their high energy density and long-term cyclability. However, if applying LIBs for large-scale energy storage scenarios, such as regulating the output of electricity generated by sustainable energy in the future age of carbon neutrality, the current electrochemistry of LIBs based on Li-ion interaction/deinteraction between a transition-metal oxide cathode and graphite anode will suffer from problems of scarce natural resources (e.g., Li, Co, and Ni) and high energy consumption/CO2 emission involved in the production of electrodes. Similarly, other commercial batteries such as lead-acid batteries and nickel-metal hydride batteries are also plagued by these issues.In contrast, organic electrode materials, especially carbonyl materials, exhibit advantages of abundant resources, renewability, high capacity, environmental friendliness, and structural designability and have shown great promise for various rechargeable batteries in recent years. However, organic carbonyl electrode materials generally exhibit unsatisfactory cycling stability and rate performance, which are highly dependent on the electrolyte and interfacial chemistry. Appropriate electrolytes and a stable electrode/electrolyte interface would be beneficial for preventing the dissolution of organic carbonyl electrode materials and/or their redox intermediates in electrolytes and promoting fast ion transport between the electrode and electrolyte. In this regard, designing an appropriate electrolyte and constructing a stable electrode/electrolyte interface are the keys to enhancing the comprehensive performance of organic carbonyl electrode materials.In this Account, on the basis of our progress and related works from other groups in the past decade, we afford an overview of understanding the effects of electrolyte and interfacial chemistry on the electrochemical performance of organic carbonyl electrode materials. We will start by briefly introducing the basic properties, working mechanisms, and issues of organic carbonyl electrode materials. Then, the implications of electrolyte and electrode/electrolyte interfacial chemistry on electrochemical performance will be summarized and highlighted through discussing the performance of organic carbonyl electrodes in different types of electrolytes (organic liquid and aqueous and solid-state electrolytes). Meanwhile, the design principles of electrolytes and interfacial chemistry for organic carbonyl electrodes are also discussed. A representative example is that organic carbonyl electrode materials often exhibit better electrochemical performance in ether-based electrolytes than in ester-based electrolytes, which could be mainly attributed to the stable and robust solid electrolyte interphase (SEI) formed on carbonyl electrodes in the ether-based electrolyte. This example demonstrates the importance of investigating the electrode/electrolyte interfacial chemistry of organic carbonyl electrode materials. Finally, future perspectives on designing appropriate electrolytes and understanding electrode/electrolyte interfacial chemistry will also be discussed. It is meaningful to thoroughly reveal the dynamic evolution of the electrode/electrolyte interface during discharge/charge processes and evaluate the compatibility between electrolytes and organic carbonyl electrode materials under practical conditions using limited quantities of electrolytes and high areal-specific-capacity electrodes in the future. This Account could attract more attention to electrolytes and the electrode/electrolyte interfacial chemistry of organic carbonyl electrode materials and finally promote their future commercial applications.

Suppressing Bulk Strain and Surface O2 Release in Li-Rich Cathodes by Just Tuning the Li Content.

Layered oxides represent a prominent class of cathodes employed in lithium-ion batteries. The structural degradation of layered cathodes causes capacity decay during cycling, which is generally induced by anisotropic lattice strain in the bulk of cathode particle and oxygen release at the surface. However, particularly in lithium-rich layered oxides (LLOs) that undergo intense oxygen redox reactions, the challenge of simultaneously addressing bulk and surface issues through a singular modification technique remains arduous. Here a thin (1-nm) and coherent spinel-like phase is constructed on the surface of LLOs particle to suppress bulk strain and surface O2 release by just adjusting the amount of lithium source during synthesis. The spinel-like phase hinders the surface O2 release by accommodating O2 inside the surface layer, while the trapped O2 in the bulk impedes strain evolution by ≈70% at high voltages compared with unmodified LLOs. Consequently, the enhanced structural stability leads to an improved capacity retention of 97.6% and a high Coulombic efficiency of ≈99.5% after 100 cycles at 0.1°C. These findings provide profound mechanistic insights into the functioning of surface structure and offer guidance for synthesizing high-capacity cathodes with superior cyclability.

Reversible Solid-Solid Conversion of Sulfurized Polyacrylonitrile Cathodes in Lithium-Sulfur Batteries by Weakly Solvating Ether Electrolytes.

Despite carbonate electrolytes exhibiting good stability to sulfurized polyacrylonitrile (SPAN), their chemical incompatibility with lithium (Li) metal anode leads to poor electrochemical performance of Li||SPAN full cells. While the SPAN employs conventional ether electrolytes that suffer from the shuttle effect, leading to rapid capacity fading. Here, we tailor a dilute electrolyte based on a low solvating power ether solvent that is both compatible with SPAN and Li metal. Unlike conventional ether electrolytes, the weakly solvating ether electrolyte enables SPAN to undergo reversibly "solid-solid" conversion. It features an anion-rich solvation structure that allows for the formation of a robust cathode electrolyte interphase on the SPAN, effectively blocking the dissolution of polysulfides into the bulk electrolyte and avoiding the shuttle effect. What's more, the unique electrolyte chemistry endowed Li ions with fast electroplating kinetics and induced high reversibility Li deposition/stripping process from 25 °C to -40 °C. Based on tailored electrolyte, Li||SPAN full cells matched with high loading SPAN cathodes (≈3.6 mAh cm-2 ) and 50 µm Li foil can operate stably over a wide range of temperatures. Additionally, Li||SPAN pouch cell under lean electrolyte and 5 % excess Li conditions can continuously operate stably for over a month.

Bifunctional Interphase with Target-Distributed Desolvation Sites and Directionally Depositional Ion Flux for Sustainable Zinc Anode.

Aqueous zinc batteries (AZBs) feature high safety and low cost, but intricate anodic side reactions and dendrite growth severely restrict their commercialization. Herein, ethylenediaminetetraacetic acid (EDTA) grafted metal organic framework (MOF-E) is proposed as a dually-functional anodic interphase for sustainable Zn anode. Specifically, the target-distributed EDTA serves as an ion-trapped tentacle to accelerate the desolvation and ionic transport by powerful chemical coordination, while the MOFs offer suitable ionic channels to induce oriented deposition. As a result, MOF-E interphase fundamentally suppresses side reactions and guides horizontally arranged Zn deposition with (002) preferred orientations. The Zn|MOF-E@Cu cell exhibits a markedly improved Coulombic efficiency of 99.7 % over 2500 cycles, and the MOF-E@Zn|KVOH (KV12 O30-y ⋅ nH2 O) cell yields a steady circulation of 5000 cycles@90.47 % at 8 A g-1 .

Emerging electrolytes with fluorinated solvents for rechargeable lithium-based batteries.

Electrolytes that can ensure the movement of ions and regulate interfacial chemistries for fast mass and charge transfer are essential in many types of electrochemical energy storage devices. However, in the emerging energy-dense lithium-based batteries, the uncontrollable side-reactions and consumption of the electrolyte result in poor electrochemical performances and severe safety concerns. In this case, fluorination has been demonstrated to be one of the most effective strategies to overcome the above-mentioned issues without significantly contributing to engineering and technical difficulties. Herein, we present a comprehensive overview of the fluorinated solvents that can be employed in lithium-based batteries. Firstly, the basic parameters that dictate the properties of solvents/electrolytes are elaborated, including physical properties, solvation structure, interface chemistry, and safety. Specifically, we focus on the advances and scientific challenges associated with different solvents and the enhancement in their performance after fluorination. Secondly, we discuss the synthetic methods for new fluorinated solvents and their reaction mechanisms in depth. Thirdly, the progress, structure-performance relationship, and applications of fluorinated solvents are reviewed. Subsequently, we provide suggestions on the solvent selection for different battery chemistries. Finally, the existing challenges and further efforts on fluorinated solvents are summarized. The combination of advanced synthesis and characterization approaches with the assistance of machine learning will enable the design of new fluorinated solvents for advanced lithium-based batteries.

Realizing High Capacity and Zero Strain in Layered Oxide Cathodes via Lithium Dual-Site Substitution for Sodium-Ion Batteries.

Sodium-ion batteries have garnered unprecedented attention as an electrochemical energy storage technology, but it remains challenging to design high-energy-density cathode materials with low structural strain during the dynamic (de)sodiation processes. Herein, we report a P2-layered lithium dual-site-substituted Na0.7Li0.03[Mg0.15Li0.07Mn0.75]O2 (NMLMO) cathode material, in which Li ions occupy both transition-metal (TM) and alkali-metal (AM) sites. The combination of theoretical calculations and experimental characterizations reveals that LiTM creates Na-O-Li electronic configurations to boost the capacity derived from the oxygen anionic redox, while LiAM serves as LiO6 prismatic pillars to stabilize the layered structure through suppressing the detrimental phase transitions. As a result, NMLMO delivers a high specific capacity of 266 mAh g-1 and simultaneously exhibits the nearly zero-strain characteristic within a wide voltage range of 1.5-4.6 V. Our findings highlight the effective way of dual-site substitution to break the capacity-stability trade-off in cathode materials for advanced rechargeable batteries.

Hollow Hierarchical Cu2 O-Derived Electrocatalysts Steering CO2 Reduction to Multi-Carbon Chemicals at Low Overpotentials.

The electrochemical reduction of carbon dioxide into multi-carbon products (C2+ ) using renewably generated electricity provides a promising pathway for energy and environmental sustainability. Various oxide-derived copper (OD-Cu) catalysts have been showcased, but still require high overpotential to drive C2+ production owing to sluggish carbon-carbon bond formation and low CO intermediate (*CO) coverage. Here, the dilemma is circumvented by elaborately devising the OD-Cu morphology. First, computational studies propose a hollow and hierarchical OD-Cu microstructure that can generate a core-shell microenvironment to inhibit CO evolution and accelerate *CO dimerization via intermediate confinement and electric field enhancement, thereby boosting C2+ generation. Experimentally, the designed nanoarchitectures are synthesized through a heteroseed-induced approach followed by electrochemical activation. In situ spectroscopic studies further elaborate correlation between *CO dimerization and designed architectures. Remarkably, the hierarchical OD-Cu manifests morphology-dependent selectivity of CO2 reduction, giving a C2+ Faradaic efficiency of 75.6% at a considerably positive potential of -0.55 V versus reversible hydrogen electrode.

High-Efficiency Lithium-Ion Transport in a Porous Coordination Chain-Based Hydrogen-Bonded Framework.

Fast and selective Li+ transport in solid plays a key role for the development of high-performance solid-state electrolytes (SSEs) of lithium metal batteries. Porous compounds with tunable Li+ transport pathways are promising SSEs, but the comprehensive performances in terms of Li+ transport kinetics, electrochemical stability window, and interfacial compatibility are difficult to be achieved simultaneously. Herein, we report a porous coordination chain-based hydrogen-bonded framework (NKU-1000) containing arrayed electronegative sites for Li+ transport, exhibiting a superior Li+ conductivity of 1.13 × 10-3 S cm-1, a high Li+ transfer number of 0.87, and a wide electrochemical window of 5.0 V. The assembled solid-state battery with NKU-1000-based SSE shows a high discharge capacity with 94.4% retention after 500 cycles and can work over a wide temperature range without formation of lithium dendrites, which derives from the linear hopping sites that promote a uniformly high-rate Li+ flux and the flexible structure that can buffer the structural variation during Li+ transport.

Reversible Metal and Ligand Redox Chemistry in Two-Dimensional Iron-Organic Framework for Sustainable Lithium-Ion Batteries.

Metal-organic frameworks (MOFs) are emerging as attractive electrode materials for lithium-ion batteries, owing to their fascinating features of sustainable resources, tunable chemical components, flexible molecular skeletons, and renewability. However, they are faced with a limited number of redox-active sites and unstable molecular frameworks during electrochemical processes. Herein, we design a novel two-dimensional (2D) iron(III)-tetraamino-benzoquinone (Fe-TABQ) with dual redox centers of Fe cations and TABQ ligands for high-capacity and stable lithium storage. It is constructed of square-planar Fe-N2O2 linkages and phenylenediamine building blocks, between which the Fe-TABQ chains are connected by multiple hydrogen bonds, and then featured as an extended π-d-conjugated 2D structure. The redox chemistry of both Fe3+ cations and TABQ anions is revealed to render its remarkable specific capacity of 251.1 mAh g-1. Benefiting from the intrinsic robust Fe-N(O) bonds and reinforced Li-N(O) bonds during cycling, Fe-TABQ delivers high capacity retentions over 95% after 200 cycles at various current densities. This work will enlighten more investigations for the molecular designs of advanced MOF-based electrode materials.

Atomic Ruthenium-Riveted Metal-Organic Framework with Tunable d-Band Modulates Oxygen Redox for Lithium-Oxygen Batteries.

Non-aqueous Li-O2 batteries have aroused considerable attention because of their ultrahigh theoretical energy density, but they are severely hindered by slow cathode reaction kinetics and large overvoltages, which are closely associated with the discharge product of Li2O2. Herein, hexagonal conductive metal-organic framework nanowire arrays of nickel-hexaiminotriphenylene (Ni-HTP) with quadrilateral Ni-N4 units are synthesized to incorporate Ru atoms into its skeleton for NiRu-HTP. The atomically dispersed Ru-N4 sites manifest strong adsorption for the LiO2 intermediate owing to its tunable d-band center, leading to its high local concentration around NiRu-HTP. This favors the formation of film-like Li2O2 on NiRu-HTP with promoted electron transfer and ion diffusion across the cathode-electrolyte interface, facilitating its reversible decomposition during charge. These allow the Li-O2 battery with NiRu-HTP to deliver a remarkably reduced charge/discharge polarization of 0.76 V and excellent cyclability. This work will enrich the design philosophy of electrocatalysts for regulation of kinetic behaviors of oxygen redox.

Halogenated Zn2+ Solvation Structure for Reversible Zn Metal Batteries.

Rechargeable aqueous Zn metal batteries have become promising candidates for large-scale electrochemical energy storage owing to their high safety and affordable low cost. However, Zn metal anode suffers from dendritic growth and hydrogen evolution reaction (HER), deteriorating the electrochemical performance. Here, we demonstrate that these challenges can be conquered by introducing a halogen ion into the Zn2+ solvation structure. By designing an electrolyte composed of zinc acetate and ammonium halide, the electron-donating anion I- can coordinate with Zn2+ and transform the traditional Zn(H2O)62+ to ZnI(H2O)5+, in which I- could transfer electrons into H2O and thus suppress HER. The dynamic electrostatic shielding layer formed by concomitant NH4+ can restrict the dendritic growth. As a result, the halogenated electrolyte achieves a high initial coulombic efficiency (CE) of 99.3% in the Zn plating/stripping process and remains at an average of ∼99.8% with uniform Zn deposition. Moreover, Zn-I batteries are constructed by using dissociative I- as the cathode and carbon felt-polyaniline as the conductive and adsorptive layer, exhibiting an average CE of 98.6% without capacity decay after 300 cycles. This work provides insights into the halogenated Zn2+ solvation structure and offers a general electrolyte design strategy for achieving a highly reversible Zn metal anode and batteries.

Optimize Lithium Deposition at Low Temperature by Weakly Solvating Power Solvent.

For lithium (Li) metal batteries, the decrease in operating temperature brings severe safety issues by more disordered Li deposition. Here, we demonstrate that the solvating power of solvent is closely related to the reversibility of the Li deposition/stripping process under low-temperature conditions. The electrolyte with weakly solvating power solvent shows lower desolvation energy, allowing for a uniform Li deposition morphology, as well as a high deposition/stripping efficiency (97.87 % at -40 °C). Based on a weakly solvating electrolyte, we further built a full cell by coupling the Li metal anode with a sulfurized polyacrylonitrile electrode at a low anode-to-cathode capacity ratio for steady cycling at -40 °C. Our results clarified the relationship between solvating power of solvent and Li deposition behavior at low temperatures.

Designing Quinone-Based Anodes with Rapid Kinetics for Rechargeable Proton Batteries.

Quinone compounds, which are capable of accommodating proton (H+ ), are emerging electrodes in aqueous batteries. However, the storage mechanism of proton in quinone compounds is less known and the energy/power density of quinone-based proton battery is still limited. Here we design a series of quinone anodes and study their electrochemical properties in acidic electrolyte, in which tetramethylquinone (TMBQ) delivers a high capacity of 300 mAh g-1 with an extremely low polarization of 20 mV at 1 C, and maintains over 50 % theoretical capacity in less than 16 seconds. The fast kinetics of TMBQ is attributed to the continuous H+ migration channel, high H+ diffusion coefficient (10-6  cm2 s-1 ), and low H+ migration energy barrier (0.26 eV). When coupling with MnO2 cathode, the battery shows a long lifespan of 4000 cycles with a capacity retention of 77 % at 5 C. This study reveals the proton transport in quinone-electrodes and offers new insights to design advanced aqueous batteries.

Tuning Interphase Chemistry to Stabilize High-Voltage LiCoO2 Cathode Material via Spinel Coating.

Cathode electrolyte interphases (CEIs) are critical to the cycling stability of high-voltage cathodes for batteries, yet their formation mechanism and properties remain elusive. Here we report that the compositions of CEIs are largely controlled by abundant species in the inner Helmholtz layer (IHL) and can be tuned from material aspects. The IHL of LiCoO2 (LCO) was found to alter after charging, with a solvent-rich environment that results in fragile organic-rich CEIs. By passivated spinel Li4 Mn5 O12 coating, we achieve an anion-rich IHL after charging, thus enabling robust LiF-rich CEIs. In situ microscopy reveals that LiF-rich CEIs maintain mechanical integrity at 500 °C, in sharp contrast to organic-rich CEIs which undergo severe expansion and subsequent voids/cracks in the cathode. As a result, the spinel-coated LCO exhibits a high specific capacity of 194 mAh g-1 at 0.05 C and a capacity retention of 83 % after 300 cycles at 0.5 C. Our work sheds new light on modulating CEIs for advanced lithium-ion batteries.

Boosting the Kinetics and Stability of Zn Anodes in Aqueous Electrolytes with Supramolecular Cyclodextrin Additives.

The hydrophobic internal cavity and hydrophilic external surface of cyclodextrins (CDs) render promising electrochemical applications. Here, we report a comparative and mechanistic study on the use of CD molecules (α-, ß-, and γ-CD) as electrolyte additives for rechargeable Zn batteries. The addition of α-CD in aqueous ZnSO4 solution reduces nucleation overpotential and activation energy of Zn plating and suppresses H2 generation. Computational, spectroscopic, and electrochemical studies reveal that α-CD preferentially adsorbs in parallel on the Zn surface via secondary hydroxyl groups, suppressing water-induced side reactions of hydrogen evolution and hydroxide sulfate formation. Additionally, the hydrophilic exterior surface of α-CD with intense electron density simultaneously facilitates Zn2+ deposition and alleviates Zn dendrite formation. A formulated 3 M ZnSO4 + 10 mM α-CD electrolyte enables homogenous Zn plating/stripping (average Coulombic efficiency ∼ 99.90%) at 1 mA cm-2 in Zn|Cu cells and a considerable capacity retention of 84.20% after 800 cycles in Zn|V2O5 full batteries. This study provides insight into the use of supramolecular macrocycles to modulate and enhance the interface stability and kinetics of metallic anodes for aqueous battery chemistry.

High-performance all-solid-state electrolyte for sodium batteries enabled by the interaction between the anion in salt and Na3SbS4.

All-solid-state sodium batteries with poly(ethylene oxide) (PEO)-based electrolytes have shown great promise for large-scale energy storage applications. However, the reported PEO-based electrolytes still suffer from a low Na+ transference number and poor ionic conductivity, which mainly result from the simultaneous migration of Na+ and anions, the high crystallinity of PEO, and the low concentration of free Na+. Here, we report a high-performance PEO-based all-solid-state electrolyte for sodium batteries by introducing Na3SbS4 to interact with the TFSI- anion in the salt and decrease the crystallinity of PEO. The optimal PEO/NaTFSI/Na3SbS4 electrolyte exhibits a remarkably enhanced Na+ transference number (0.49) and a high ionic conductivity of 1.33 × 10-4 S cm-1 at 45 °C. Moreover, we found that the electrolyte can largely alleviate Na+ depletion near the electrode surface in symmetric cells and, thus, contributes to stable and dendrite-free Na plating/stripping for 500 h. Furthermore, all-solid-state Na batteries with a 3,4,9,10-perylenetetracarboxylic dianhydride cathode exhibit a high capacity retention of 84% after 200 cycles and superior rate performance (up to 10C). Our work develops an effective way to realize a high-performance all-solid-state electrolyte for sodium batteries.

Quinone Electrodes for Alkali-Acid Hybrid Batteries.

Aqueous batteries are promising candidates for large-scale energy storage but face either limited energy density (lead-acid batteries), cost/resource concerns (Ni-MH batteries), or safety issues due to metal dendrite growth at high current densities (zinc batteries). We report that through designing electrochemical redox couples, quinones as intrinsic dendrite-free and sustainable anode materials demonstrate the theoretical energy density of 374 W h kg-1 coupling with affordable Mn2+/MnO2 redox reactions on the cathode side. Due to the fast K-ion diffusion in the electrolyte, low K-ion desolvation energy at the interface, and fast quinone/phenol reaction, the optimized poly(1,4-anthraquinone) in the KOH electrolyte shows specific capacities of 295 mA h g-1 at 300 C-rate and 225 mA h g-1 at 240 mA cm-2. Further constructed practical aqueous batteries exhibit an output voltage of 2 V in alkali-acid hybrid electrolyte systems with exceptional electrochemical kinetics, which can release/store over 95% of the theoretical capacity in less than 40 s (25 000 mA g-1). The scaled Ah level aqueous battery with the upgradation of interfacial chemistry on the electrode current collector exhibits an overall energy density of 92 W h kg-1, exceeding commercial aqueous lead-acid and Ni-MH batteries. The rapid response, intrinsic dendrite-free existence, and cost efficiency of quinone electrodes provide promising application interests for regulating the output of the electricity grid generated by intermittent solar and wind energy.