High Working Voltage Research Articles

A high‐capacity dual‐ion full battery based on nitrogen‐doped carbon nanosphere anode and concentrated electrolyte

AbstractDual‐ion batteries (DIBs) are often criticized for their low discharge capacity and poor cyclic capability despite their inherent high working voltage, low manufacturing cost, and environmental friendliness. To solve these shortcomings, many attempts and efforts have been devoted, but all ended in unsatisfactory results. Herein, a hierarchical porous carbon nanosphere anode with ultrahigh nitrogen doping is developed, which exhibits fast ion transport kinetics and excellent Li+ storage capability. Moreover, employing a concentrated electrolyte is expected to bring a series of advantages such as stable SEI for facilitating ion transmission, enhanced cycling performance, high specific capacity, and operation voltage. These advantages endow the assembled full DIBs with excellent performance as a super‐high specific discharge capacity of 351 mAh g−1 and can be cycled stably for 1300 cycles with Coulombic efficiency (CE) remaining at 99.5%; a high operating voltage range of 4.95–3.63 V and low self‐discharge rate of 2.46% h−1 with stable fast charging‐slow discharging performance. Through electrochemical measurements and physical characterizations, the possible working mechanism of the proof‐of‐concept full battery and the structural variations of electrodes during cycling are investigated. The design strategy of novel battery system in this work will promote the development of high‐performance DIBs.

Inch‐Size Single Crystals of Lead‐Free Chiral Perovskites with Bulk Photovoltaic Effect for Stable Self‐Driven X‐Ray Detection

AbstractLead halide perovskites have made great advance in direct X‐ray detection, however the presence of toxic lead and the requirement of high working voltages severely limit their applicability and operational stability. Thus, exploring “green” lead‐free hybrid perovskites capable of detecting X‐rays at zero bias is crucial but remains toughly challenging. Here, utilizing chiral R/S‐1‐phenylpropylamine (R/S‐PPA) cations, a pair of 0D chiral‐polar perovskites, (R/S‐PPA)2BiI5 (1R/1S) are constructed. Their intrinsic spontaneous electric polarization induces a large bulk photovoltage of 0.63 V, which acts as a driving force to separate and transport photogenerated carriers, thus endowing them with the capability of self‐driven detection. Consequently, self‐driven X‐ray detectors with a low detection limit of 270 nGy s−1 are successfully constructed based on high‐quality, inch‐sized single crystals of 1R. Notably, they show suppressed baseline drift under the self‐driven mode, exhibiting superior operational stability. This study realizes self‐driven X‐ray detection in a single‐phase lead‐free hybrid perovskite by exploiting the intrinsic bulk photovoltaic effect, which sheds light on future explorations of lead‐free hybrid perovskites toward “green” self‐driven radiation detectors with high performance.

Bifunctional urea surface-modified high voltage LiNi0.5Mn1.5O4 cathode for enhanced electrochemical performance

Spinel LiNi0.5Mn1.5O4 (LNMO) cathode material has high specific energy density due to its high working voltage (4.7 V vs. Li/Li+). However, high voltage inevitably brings instability of the surface and interface layer properties and ultimately electrolyte decomposition and irreversible side reactions, which incurs structural degradation, capacity decline, and poor kinetics. Herein, a simple and novel surface modification strategy is proposed to obtain a bifunctional modification cathode material with carbon–nitrogen nanocoating and surface disorder phase transition, which is prepared through gas–solid heat treatment of pristine material and urea in a closed reactor. The surface disordered phase transition introduces favorable oxygen vacancies and synchronously constructs the fast diffusion channel of lithium ions, while the carbon–nitrogen nanocoating effectively alleviates the impedance growth of the electrode/electrolyte interface. Therefore, the surface modified U-LMNO exhibits an initial discharge capacity of 130.1 mAh g−1 at 0.2 C and a capacity retention rate of 95.1% after 200 cycles at 1 C, significantly superior to pristine P-LMNO. These results highlight the essentiality of high-voltage LNMO cathode material surface interface design and facilitate the development and commercialization of high-energy-density LNMO-based lithium-ion batteries.

Upcycling of Spent LiCoO2 Cathode to Lithium Dual‐Ion Battery Anode

AbstractOwing to the paradigm shift of the automobile industry toward the electrification of vehicles, the aftermath of batteries that power these devices at the end of their lives has to be addressed strenuously. Since upcycling strategies are hardly in the limelight, this paper focuses on giving a second life to LiCoO2 cathode as a dual‐ion battery (DIB) anode. Among many possible recovery approaches explored for cobalt, a microwave‐assisted green leaching method comprising mild leaching agents is chosen for this work. Cobalt is recovered as cobalt oxalate and converted to cobalt/cobalt oxide nanospheres embedded in a porous graphitic carbon matrix (Co3O4/Co@C). Due to the high working voltage, excellent safety, and environmental friendliness, DIBs are being considered as a replacement for lithium‐ion batteries in specific sectors. In an unconventional approach, the derived Co3O4/Co@C is effectively employed as an anode material for dual‐ion batteries. The half‐cell demonstrates a high discharge capacity of 550 mAh g−1 at 0.1 A g−1. A full‐cell DIB fabricated using Co3O4/Co@C, derived from upcycled LiCoO2 as an anode and graphite as a cathode, shows an appreciable capacity and remarkable cycling stability. This sustainable approach for upcycling exhausted LIBs can pave the way to improve the circular economy of batteries.

Dual Role of Bis(borate) Additive in Electrode/Electrolyte Interface Layer Construction for High-Voltage NCM 523 Cathode

Increasing the working voltage of a layered oxide cathode is an efficient way to lift the energy density of lithium-ion batteries. However, uncontrollable side reactions and excessive electrolyte decomposition take place at high voltage. Bulk cathode structure degradation and formation of a high working voltage induce excessive growth of the solid-electrolyte interface (SEI) layer and overconsumption of the electrolyte. Construction of a high-voltage stable SEI layer is crucial to enhance the electrochemical performance. In this work, trimethylene borate (TMEB) as a borate ester additive is used to improve the cycled stability of NCM523 cells at 4.5 V charging-cutoff voltage. On one hand, TMEB can be preferentially decomposed during cycling and participate in the film formation process on the surfaces of both anode and cathode. On the other hand, TMEB can tune the solvation sheath by expelling the carbonate solvent molecules out of the solvation sheath to suppress decomposition of the electrolyte. The cells cycled with the 0.5 wt % TMEB-containing electrolyte exhibit improved cycling stability after 200 cycles with the capacity retention of 90.9% indicating TMEB to be an effective additive to improve the lithium-ion batteries at higher charging-cutoff voltage.

When audience takes stage: Pseudo-localized-high-concentration electrolyte with lithium nitrate as the only salt enables lithium metal batteries with excellent temperature and cathode adaptability

A new concept for pseudo-localized-high-concentration electrolytes (PLHCE) is developed using cheap and less corrosive lithium nitrate as the single lithium salt to improve the electrochemical performance of the lithium metal batteries with excellent temperature and cathode adaptability. Unlike conventional localized high-concentration electrolytes, a small number of the diluent molecules involved in the solvation structure by lithium nitrate and triethyl phosphate (TEP) promote the formation of an organic-inorganic composite solid electrolyte interface (SEI) layer. A good balance is achieved in terms of the mechanical properties of the SEI layer. A high coulombic efficiency of more than 98% for the Li||Cu cell and 1000 h of long-term cycling for the Li||Li cell is exhibited. Assisted with the PLHCE strategy, the Li||LFP cells display excellent performance at both room and high temperatures, and the Li||NCM523 cells with a high working voltage exhibit good electrochemical stability as well. Moreover, alternative solvents are selected as the pseudo-diluents, which proves the general applicability of the PLHCE approach. This work provides an innovative concept to use the solubility difference to manipulate the solvation structure, which paves a new but simple way to design advanced electrolytes for lithium secondary batteries.

Achieving Fast and Reversible Sulfur Redox by Proper Interaction of Electrolyte in Potassium Batteries

Potassium–sulfur batteries have potential for low-cost and high-energy density energy storage. However, it is a challenge to find suitable electrolytes affording liquid environment for intermediate sulfur species to convert at high voltages. In this study, a series of ether/potassium salt systems were systematically studied to investigate the electrochemical stability and function of the electrolytes in sulfur electrochemistry by using in situ ultraviolet–visible and Fourier-transform infrared spectroscopies. Interactions of soluble polysulfides with the electrolyte were critical to the electrochemical performance. Under optimized conditions, the bis(trifluoromethanesulfonyl)imide anion demonstrated moderate interaction and reversible solvation/desolvation of polysulfides. Polar carboxyl groups in poly(acrylic acid) were effective for binding polysulfide in electrodes, enabling reversible sulfur conversions at high working voltages and improved initial Coulombic efficiency. This enhanced battery performance was achieved even using a conventional carbon host with a high sulfur loading of ∼69 wt %, i.e., ∼49 wt % in the cathode.

Suppressing the H2–H3 phase transition of LiNi0.90Co0.04Mn0.03Al0.03O2 cathodes via Ta doping towards improved electrochemical performance upon 4.5V

Nowadays, Ni-rich cathodes act as a strong contender for high performance lithium-ion batteries cathodes due to their high capacities. Rapid capacity degradation and poor rate performance at high working voltages hinder their commercialization. This study reports a strategy for Ta5+ doping modification in LiNi0.90Co0.04Mn0.03Al0.03O2 (NCMA) cathode via a solid-state route. This study confirmed that the introduction of strong Ta–O bond is beneficial to degrade H2–H3 phase transition during cycling. Subsequently, the polarization of electrodes and internal resistance have been alleviated since the H2–H3 phase transition of the Ta-doped NCMA cathode is suppressed, which eventually leads to a high cyclability. Moreover, it also confirmed that the diffusion of Li ions has been accelerated since the space of Li layer is enhanced. As a consequence, the Ta-NCMA cathode displays a high initial discharge capacity of 222.6 mA h·g−1 and outperforms the benchmarking cathodes in 100th capacity retention (from 43.7% to 91.8%) between 2.8 and 4.5 V. Besides, compared to pristine NCMA cathodes, the rate capability of Ta5+-doped NCMA cathodes cycling at 5C also increase from 112.2 mA h·g−1 to 167.2 mA h·g−1. Hence, Ta doped Ni-rich cathode should be a potential cathode to realize both high capacity and stability structure.

Nitrogen-Doped Carbon Coated Na3V2(PO4)2F3 Derived from Polyvinylpyrrolidone as a High-Performance Cathode for Sodium-Ion Batteries

Na super ionic conductor (NASICON)-type Na3V2(PO4)2F3 (NVPF) has been regarded as a prospective candidate of cathode materials for sodium-ion batteries due to its excellent structural stability, relatively high capacity and working voltage. However, the poor cyclability and rate capability, resulting from its low intrinsic electronic conductivity, have become a serious obstacle to their practical large-scale application. In this work, N-doped carbon coated NVPF composites (NVPF@NC) were successfully synthesized via a simple sol–gel method, in which low-cost polyvinylpyrrolidone was introduced as a nitrogen source. After high-temperature pyrolysis, a highly conductive N-doped carbon layer was in-situ constructed on the particle surface to enhance the sodium storage performance of NVPF. The optimized NVPF@NC cathode delivered high reversible capacity, excellent rate capability and long-term cycle life compared to pristine NVPF@C. The remarkable electrochemical performance of NVPF@NC cathode benefits from the modification strategy of introducing a heteroatom-doped carbon layer, triggering the formation of extrinsic defects and active sites in the N-doped amorphous carbon layer, which greatly enhances the electrical conductivity and the diffusion rate of sodium ions. This work provides a facile and effective approach for the preparation of N-doped carbon coated NVPF with remarkable sodium storage properties, which could be extended to other electrode materials electrochemical for energy storage.

Synthesis of Fe-doped Mn-based Prussian blue hierarchical architecture for high-performance sodium ion batteries

Sodium manganese hexacyanoferrates (MnHCFs) have great potential as cathode for sodium-ion batteries (SIBs) owing to their large specific capacity, low cost, ecofriendly synthesis and high working voltage. Nevertheless, their cycling stability is limited by Jahn-Teller effect (JT-effect) of Mn3+, phase transitions and Mn2+ dissolution during the charging and discharging processes. Herein, an unconventional solid-liquid two-phase route is developed to fabricate a novel hierarchical nanostructure Na1.02Mn0.57Fe0.43[Fe(CN)6]0.63∙1·39H2O in view of different solubility of raw material Na4Fe(CN)6·10H2O in the mixed solvent of ethanol and water. Benefiting from unique porous hierarchical architecture, good structural stability, high electrical conductivity and fast capacitive behavior, such Fe-doped MnHCF cathode has an outstanding rate capability with large discharging capacity of 127 mAh g−1 at 25 mA g−1 and 71 mAh g−1 at 1200 mA g−1, and an excellent cyclability with 120 mAh g−1 of specific capacity at 100 mA g−1 and 86% of capacity retention over 200 cycles. In particular, the facile and controllable synthesis process of Fe-doped MnHCFs make it accessible for large-scale applications.

Dual modification of P2–Na0.67Ni0.33Mn0.67O2 by Co doping and Al1.8Co0.2O3 coating

As promising cathode materials for sodium-ion batteries, P2–Na0.67Ni0.33Mn0.67O2 has the characteristics of high capacity and high working voltage. However, the application is strongly limited because of the rapidly deteriorated electrochemical performances during cycling. Therefore, we present in this study the optimization of the cycling stability of P2–Na0.67Ni0.33Mn0.67O2 through proper Co doping and Al1.8Co0.2O3 surface coating. Without Co doping and Al1.8Co0.2O3 coating, the initial specific discharge capacity of P2–Na0.67Ni0.33Mn0.67O2 in the voltage range of 2–4.3 V is 154.7 mAh·g−1, and the capacity retention rate after 100 cycles is 26.4%. Co doping can improve the cycling stability and rate capability. However, the initial capacity also reduces with the Co doping amount. Furthermore, Al1.8Co0.2O3 coating can improve the cycle stability with a reduced capacity. The coated sample exhibits a retention rate of 84.8% after 100 cycles.

Unveiling the effect of structural water on Zn-ion storage of polyoxovanadate for high-rate and long-life aqueous zinc ion battery

Aqueous zinc-ion batteries (ZIBs) are promising for grid-scale energy storage because of their low cost, high theoretical energy density, and high safety; however, the rational design of advanced cathode materials with stable internal structures and sufficient Zn2+ diffusion channels remains a challenge. To date, most studies have focused on the structural water of electrode materials to improve their electrochemical kinetics without considering its possible negative effects. Herein, we develop the polyoxovanadates of Na6[V10O28]·nH2O with controllable structural water (denoted as NVO-n, n = 18, 2.6 and 0) as cathodes for Zn2+ storage, which provide model objects to study the effects of water molecules on electrochemical properties. Results reveal that an appropriate amount of structural water improves ion transport by shielding the effective charge of Zn2+ ions while reducing the hindrance to the migration of Zn2+ ions, enabling fast Zn2+ storage. Moreover, the NVO-2.6 possesses multi-electron redox ability and high structural stability, which ensures the highly reversible Zn2+ intercalation/de-intercalation at a high working voltage (0.98 V) and small volumetric strain upon cycling. Consequently, the optimized NVO-2.6 delivers a high specific capacity of 228.5 mAh g−1 at 0.1 A g−1 and a long-term cyclability with 89.7% capacity retention after 3000 cycles at 10 A g−1. This study paves a new direction for the design of polyoxovanadate-based cathodes toward high-performance ZIBs.

Size Effect of Electrolyte Ions on the Electric Double-Layer Structure and Supercapacitive Behavior

Finding a viable electrolyte for next-generation supercapacitors is of primary importance for developing supercapacitors with high power and energy densities. Herein, we synthesized a conducting salt, tetramethylphosphonium tetrafluoroborate (TMPBF4), and compared the electrochemical characteristics of supercapacitor devices containing TMPBF4 or 1,1-dimethylpyrrolidinium tetrafluoroborate (DMPBF4). The TMPBF4 salt was selected based on the generally accepted design rule that smaller ions and solvation shells contribute to higher energy and power densities. However, at a low current density (0.1 A g–1), supercapacitors with TMPBF4 in acetonitrile (AN) exhibited a slightly lower capacitance (24.6 ± 0.1 F g–1) than those with DMPBF4 (25.0 ± 0.2 F g–1). Clarification of this behavior using electrochemical and theoretical methods revealed that the total capacitance is influenced by not only the size of the ions but also the degree of cation–anion interactions near the electrodes. By contrast, at a high current density of 10 A g–1, supercapacitors with TMPBF4 showed an 18% increase in capacitance relative to those with DMPBF4. Supercapacitors with TMPBF4 exhibited both high capacitance and a remarkably long cycle life (10,000 cycles) at a high working voltage (3.2 V) and high current density (10 A g–1). Furthermore, supercapacitors utilizing TMPBF4/AN provided a sufficiently fast frequency response for 60 Hz alternating current (ac) line filtering. These insights into the influence of the investigated electrolyte salts on the formation of electric double-layer structures offer design rules for developing electrolytes for supercapacitors.

Highly efficient synthesis of nano LiMn0.90Fe0.10PO4/C composite via mechanochemical activation assisted calcination

Among various lithium-ion batteries cathode materials, olivine-type phosphate LiMnPO4 has the advantages of high working voltage, superior theoretical energy density and high stability, however, its electronic and ionic insulation limit its application. In this work, LiMn0.90Fe0.10PO4/C (LMFP@C) nano composites are prepared via a mechanochemical activation assisted carbothermal reduction method, and the consequence of carbon coating amount on the electrochemical performance of the materials is discussed in detail. The results of physical and chemical properties analysis show that the mechanical liquid activation process can effectively reduce the particle size of the precursor to nanometer scale and make the raw material mixed evenly. The high crystallinity, particle nanometrization and uniform carbon coating enable LMFP@C composites with excellent electrochemical performance even when a small amount of carbon coating is introduced. Under an optimizing coated carbon amount of 2.5 wt%, the material showed ∼4.0 V and ∼3.6 V voltage platforms at 0.1, 0.2, 0.5, 1, and 2C, and released discharge specific capacities of ∼155 mAh·g−1 and ∼140 mAh·g−1 at 0.1 and 1C, respectively. It also shows optimal cycling stability with a capacity retention rate ∼100% after 100 cycles at 2C.

A Novel Energy Harvesting Method for Online Monitoring Sensors in HVdc Overhead Line

Due to the lack of alternating electric fields and alternating magnetic fields in HVdc transmission system, there has been no sustainable and stable energy harvesting method compatible with them up to now, hindering the application of HVdc sensors. In this letter, we proposed a novel dc energy harvesting method using corona current, and an energy harvesting circuit is constituted with space ion flow generated by dc corona. The feasibility of the proposed method is increased by adding an artificial corona electrode and placing the load before the corona electrode. In addition, it can flexibly operate at any position in an HVdc transmission system according to actual demand. Then the output power is further maximized by adopting a capacitor with high working voltages. The detailed measurement results based on the experimental system validate the effectiveness of the proposed method, with a stable output power as high as 10.15 mW in a dc system of 22 kV. A detailed discussion of the overall performance is finally carried out.

Growth characteristics of scanning micro-arc oxidation coating on Ti6Al4V alloy

ABSTRACT In this study, the ceramic coating was prepared on Ti6Al4V alloy by scanning micro-arc oxidation (SMAO). The growth features of SMAO coating were investigated by combining the voltage and discharge variation. The result shows that a higher working voltage is obtained during SMAO treatment owing to additional resistance from the electrolyte column. As the SMAO goes on, the discharge region moves to the electrolyte column edge, exhibiting an annular shape. The current density with Gaussian distribution is observed between the stainless-steel tube (cathode) and titanium substrate (anode), which causes the SMAO coating to show a higher thickness in the middle and lower on both sides. Similar to traditional MAO, the SMAO coating has an enhancement in the thickness, pore size and Si content with increasing oxidation time, but coating degradation occurs in the later stage of SMAO. The SMAO coating mainly consists of amorphous SiO2, rutile and anatase phases.

Ultrafast Charge-Discharge Capable and Long-Life Na3.9 Mn0.95 Zr0.05 V(PO4 )3 /C Cathode Material for Advanced Sodium-Ion Batteries.

Na4 MnV(PO4 )3 /C (NMVP) has been considered an attractive cathode for sodium-ion batteries with higher working voltage and lower cost than Na3 V2 (PO4 )3 /C. However, the poor intrinsic electronic conductivity and Jahn-Teller distortion caused by Mn3+ inhibit its practical application. In this work, the remarkable effects of Zr-substitution on prompting electronic and Na-ion conductivity and also structural stabilization are reported. The optimized Na3.9 Mn0.95 Zr0.05 V(PO4 )3 /C sample shows ultrafast charge-discharge capability with discharge capacities of 108.8, 103.1, 99.1, and 88.0 mAh g-1 at 0.2, 1, 20, and 50 C, respectively, which is the best result for cation substituted NMVP samples reported so far. This sample also shows excellent cycling stability with a capacity retention of 81.2% at 1 C after 500 cycles. XRD analyses confirm the introduction of Zr into the lattice structure which expands the lattice volume and facilitates the Na+ diffusion. First-principle calculation indicates that Zr modification reduces the band gap energy and leads to increased electronic conductivity. In situ XRD analyses confirm the same structure evolution mechanism of the Zr-modified sample as pristine NMVP, however the strong ZrO bond obviously stabilizes the structure framework that ensures long-term cycling stability.

Electrochemically Induced Crystalline‐to‐Amorphous Transition of Dinuclear Polyoxovanadate for High‐Rate Lithium‐Ion Batteries

AbstractPolyoxometalates are intriguing high‐capacity anode materials for alkali‐metal‐ion storage due to their multi‐electron redox capabilities and flexible structure. However, their poor electrical conductivity and high working voltage severely restrict their practical application. Herein, the dinuclear polyoxovanadate Sr2V2O7·H2O with unusually high electrical conductivity is reported as a promising anode material for lithium‐ion batteries. During the initial lithiation process, the Sr2V2O7·H2O anode experiences an electrochemically induced crystalline‐to‐amorphous transition. The resulting amorphous structure provides high redox activity and fast reaction kinetics via reversible V4.9+/V2.8+ redox couple through the intercalation mechanism. Furthermore, when coupled with the LiFePO4 cathode, the strong VO bonds of the amorphous anode provide excellent structural stability, with the full‐cell capable of performing >12 000 cycles with a capacity retention of 72%. Another advantage of Sr2xV2O7‐δ·yH2O (0.5 ≤ x ≤ 1.0) is its composition adjustability, which enables delicately regulating the Sr vacancy content without destroying the structure. The defect Sr2xV2O7‐δ·yH2O (x = 0.5) electrodes show significantly improved specific capacity and rate capability without sacrificing other key properties, delivering a high specific capacity of 479 mAh g‐1 at 0.1 mA cm‐2 and 41.9% of its capacity in 2 min. Overall, the preliminary study points the way forward for the facile preparation of high‐quality polyoxometalates for advanced energy storage applications and beyond.

Hydroxylation strategy unlocking multi-redox reaction of manganese hexacyanoferrate for aqueous zinc-ion battery

Prussian blue analogues (PBAs), as one of the most promising cathodes due to their open framework and high working voltage (∼1.75 V vs Zn/Zn2+) for rechargeable aqueous zinc ion batteries (RAZIBs), commonly suffer from poor reversible capacity owing to single redox center. Here, a hydroxylation strategy is proposed for activating inactive redox pair of Mn(II)/Mn(III) in manganese hexacyanoferrate (MnHCF) to supply extra capacity. As a result, OH − rich MnHCF cathode renders a high discharge capacity of 136.1 mAh/g (at 100 mA g−1) and a considerable energy density of 228.8 Wh kg−1 benefiting from the unlocked multi-redox reaction, which is much better than the OH − poor MnHCF (58.3 mAh/g and 52.6 Wh kg−1, respectively). Furthermore, the abundant hydroxyl in OH-rich MnHCF can continuously activate the multi-redox centers to provide high capacity in the subsequent cycles. Density functional theory (DFT) calculation reveals that abundant hydroxyl functional group favors to capture Zn2+ on the sites near Mn atoms, thereby facilitating the activation of Mn-redox reaction. This study offers new opportunities for exploiting cathodes with both high working voltage and discharge capacity for RAZIBs.

Interface Engineering of Zinc Electrode for Rechargeable Alkaline Zinc-Based Batteries.

Rechargeable aqueous zinc-based batteries have gained considerable interest because of their advantages of high theoretical capacity, being eco-friendly, and cost effectiveness. In particular, zinc-based batteries with alkaline electrolyte show great promise due to their high working voltage. However, there remain great challenges for the commercialization of the rechargeable alkaline zinc-based batteries, which are mainly impeded by the limited reversibility of the zinc electrode. The critical problems refer to the dendrites growth, electrode passivation, shape change, and side reactions, affecting discharge capacity, columbic efficiency, and cycling stability of the battery. All the issues are highly associated with the interfacial properties, including both electrons and ions transport behavior at the electrode interface. Herein, this work concentrates on the fundamental electrochemistry of the challenges in the zinc electrode and the design strategies for developing high-performance zinc electrodes with regard to optimizing the interfaces between host and active materials as well as electrode and electrolyte. In addition, potential directions for the investigation of electrodes and electrolytes for high-performance zinc-based batteries are presented, aiming at promoting the development of rechargeable alkaline zinc-based batteries.