휴대전화기용 아연공기전지 개발

Fast development of portable electronic devices (such as a smart phone, iPad, and Galaxy Note) and electrified vehicles (such as EVs and HEVs) require better and smaller lithium ion batteries as their energy storages. What is needed for the cathode of the lithium ion battery is a material capable of a higher volumetric energy density as well as gravimetric energy density. However, not only the development of cathode material but also the commercialization of high energy density anode material has been limited due to cathode material’s much lower energy density compared to anode material. In this regard, Li-rich material (Li2MnO3-LiMO2, M=Ni, Mn and Co) that has 150 % higher energy density than commercialized LiCoO2 is the unique next generation cathode material to solve the problem of cathode material’s low energy density. In the past decade, many researches have focused on the surface stabilization method of this material to improve its intrinsic problems of poor cycle/ rate capability and such surface treatment methods have been demonstrated in a few examples, including AlF3 coating and spinel heterostructures, yielding noticeable improvements in rate and cycle ability. Although such surface treatments showed improved rate and cycle performances, achieving the high volumetric energy density and long-term cycle life which are more critical factors for the commercialization of Li-rich material still remained unsatisfied. In general, Li-rich material’s reversible capacity is related with its particle size since the Li2MnO3 phase in large Li-rich material, which is a major component to realize high energy density, is not fully activated in low voltage range below 4.6 V. For this reason, many previous papers reported their results with only small primary particle size below 100nm. The high surface area induced by the small particle size increases side reactions with electrolyte resulting poor long-term cycle life as well as lowers the volumetric energy density. Note that Li-rich material’s deteriorations are generated from its surface and continue to affect its cycling capability and the deteriorations can be divided into two mechanisms: one is side reactions with electrolyte, and another is the phase collapse. The side reactions with electrolyte at its high working voltage yield active material attack speiceses such as HF and electrolyte exhaustion causing Li-rich material’s fast discharge capacity decay during cycles. Furthurmore, it is hardly show long-term cycle life with over 200 cycles since the phase transition from layered structure to spinel-like and NiO rock salt is generated on the surface of active material, and followed by expention of this transition into the bulk. For instance, AlF3 coated Li-rich LNCMO has abrupt capacity fade after 100 cycles, although it showed good rate and cycle capability within 100 cycles. Hence, new active material design, rather than simple surface modification methods such as coating or doping, is required to solve above previous limits.The new material design needs to start with a simple question: how to minimize the damages of surface deteriorations such as side reasction with electrolyte and phase trasnsition on bulk material and maximize volumetric energy density. The most effective solution for the question is increasing the primary particle size with the stable activation method, since the volumetric energy density of cathode material is maximized from synthesis of micron secondary particles consisted of primary particles by using co-precipitation method in industry. Here we demonstrate a novel approach for lithium storage, which is a material design of a secondary structure which consists of large flake shaped primary particle (hundred nanometers x mictrometers) with a novel activation method using simple chemical treatment to achieve superior long-term cycle life with high volumetric energy density. In this design, the large primary particle effectively reduced its surface area producing markedly decreased surface instability reaction as well as high tap density. Interstingly, the chemical approach activated only surface Li2MnO3 phase of large primary particle and the very surface activation effectively overcame the activation problem, which is limit of large primary particle have. This novel concept is very meaningful in that it is the first and unique method to achieve cathode material’s high volumetric energy density with long-term cycle life. As a result, this novel designed material affords remarkable battery performance with extremely high cycle retention during 400 cycles and high volumetric energy density ever reported before.

Zinc-air battery (ZAB) with high theoretical energy density and low-cost characteristics has become one of the future candidate energy storage devices for flexible and portable electronic devices. If the application of ZAB in this field is to be promoted, how to improve the performance of solid-state batteries (such as cycle stability, discharge capacity) is the main problem at present. Flexible solid electrolyte plays a vital role in it. In this work, Carboxyl modified cellulose nanofibers (C-CNFs) was prepared by controlling the degree of carboxyl modification, and polyvinyl alcohol (PVA)-based cellulose composite gel polymer electrolyte (GPE) was synthesized. The optimal PVA-based composite GPE was selected to exhibit high ionic conductivity (0.31 S cm−1), excellent water retention and good tensile mechanical strength under environmental conditions. The assembled flexible zinc-air battery (ZAB) exhibits excellent cycle stability, discharge performance and power density. ZAB based on PVA-C-CNFs GPE can work continuously and stably for 50 hours, and at the same time has high cost-effectiveness and safety.

Incorporating intermittent renewable energy sources into the power grid will require large amounts of grid-scale energy storage. Electrochemical batteries are a versatile and scalable energy storage option and, hence, Li-ion batteries have been widely adopted to store excess wind and solar energy [1]. Li-ion batteries, however, have a relatively low energy density and serious safety concerns. An alternative electrochemical battery option lies with zinc-air batteries. This technology uses lower cost materials and is overall much safer. Furthermore, zinc-air batteries have a much larger theoretical energy density than Li-ion batteries [2]. The major impediment to wide-scale adoption of zinc-air batteries is the low energy efficiency because of the poor reaction kinetics at the air electrode. Both the charge and discharge reactions at the air electrode are sluggish and require the use of catalysts to obtain practicable performance. However, many catalysts active towards the charge reaction are not active towards the discharge reaction, and vice versa. The development of a catalyst active towards both the charge and discharge reactions, known as a bifunctional catalyst, is therefore a high priority [3]. Furthermore, catalysts employed in zinc-air batteries often show instability, with performance degradation evident after a few cycles. Ultimately, a highly stable bifunctional zinc-air battery catalyst is of the utmost importance.The aim of this work is to develop highly stable bifunctional catalysts for zinc-air batteries using atomic layer deposition (ALD). With ALD, extremely conformal catalyst coatings can be deposited directly on the air electrode of a zinc-air battery. The self-limiting surface reactions of ALD ensure that electrode porosity is maintained while maximizing the total coating surface area [4]. Since ALD operates in the gas phase, catalytic coatings can be deposited deep within the pores of the air electrode. This will help maintain the three-phase boundary necessary for the discharge reaction and ultimately improve the stability of a zinc-air battery [5]. To create a bifunctional catalyst, two ALD processes, one for manganese oxide and another for iron oxide, is combined into one ALD supercycle, depositing a mixed manganese-iron oxide. Since manganese oxide is a well-established discharge catalyst [6], and iron oxide demonstrates activity towards the charge reaction [7], this mixed manganese-iron oxide exhibits bifunctional activity in a zinc-air battery. An optimized supercycle process will be discussed and full-cell battery test results showcased. Specifically, the bifunctional efficiency of a zinc-air battery can be improved by more than 10% by using the mixed manganese-iron oxide catalyst. In addition, the high stability of the manganese-iron oxide catalyst is demonstrated, where bifunctional efficiency can be maintained at over 95% of the initial value over 200 cycles. Materials characterization of the mixed manganese-iron oxide, deposited through ALD, is also included.[1] L. Trahey, F. R. Brushett, N. P. Balsara, G. Ceder, L. Cheng, Y. M. Chiang, N. T. Hahn, B. J. Ingram, S. D. Minteer, J. S. Moore, K. T. Mueller, L. F. Nazar, K. A. Persson, D. J. Siegel, K. Xu, K. R. Zavadil, V. Srinivasan, and G. W. Crabtree, “Energy Storage Emerging: A Perspective from the Joint Center for Energy Storage Research,” Proc. Natl. Acad. Sci. U. S. A., vol. 117, no. 23, pp. 12550–12557, 2020.[2] J. Fu, R. Liang, G. Liu, A. Yu, Z. Bai, L. Yang, and Z. Chen, “Recent Progress in Electrically Rechargeable Zinc – Air Batteries,” Adv. Mater., vol. 31, no. 31, p. 1805230, 2019.[3] E. Davari and D. G. Ivey, “Bifunctional electrocatalysts for Zn – air batteries,” Sustain. Energy Fuels, vol. 2, no. 1, pp. 39–67, 2018.[4] C. Detavernier, J. Dendooven, S. Pulinthanathu Sree, K. F. Ludwig, and J. A. Martens, “Tailoring nanoporous materials by atomic layer deposition,” Chem. Soc. Rev., vol. 40, no. 11, pp. 5242–5253, 2011.[5] M. P. Clark, M. Xiong, K. Cadien, and D. G. Ivey, “High Performance Oxygen Reduction/Evolution Electrodes for Zinc − Air Batteries Prepared by Atomic Layer Deposition of MnOx,” ACS Appl. Energy Mater., vol. 3, no. 1, pp. 603–313, 2020.[6] M. P. Clark, T. Muneshwar, M. Xiong, K. Cadien, and D. G. Ivey, “Saturation Behavior of Atomic Layer Deposition MnOx from Bis(Ethylcyclopentadienyl) Manganese and Water: Saturation Effect on Coverage of Porous Oxygen Reduction Electrodes for Metal-Air Batteries,” ACS Appl. Nano Mater., vol. 2, no. 1, pp. 267–277, 2019.[7] M. Labbe, M. P. Clark, Z. Abedi, A. He, K. Cadien, and D. G. Ivey, “Atomic layer deposition of iron oxide on a porous carbon substrate via ethylferrocene and an oxygen plasma,” Surf. Coatings Technol., vol. 421, p. 127390, 2021.

Rechargeable zinc-air batteries (RZBs) demonstrate significant potential as next-generation batteries as they are non-flammable, resource-abundant, cost-efficient, feasible for ambient air operation, and have remarkable theoretical energy density (1086 Wh kg-1). However, the development of RZBs needs to address many challenges to speed up their commercialization. For example, low round-trip efficiency during cycling is caused by retarded reactivity of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) at the air cathode. An air cathode with deficient electrocatalytic kinetics creates a large voltage gap, especially when the practical charge voltage is > 2.0 V, during the charging and discharging process. Moreover, the cycle life of the RZBs is limited owing to the structural degradation of air cathodes working under high charge voltage. Therefore, it is essential to improve both the round-trip efficiency and structural durability of air cathodes to ensure further development and commercialization of RZBs. For efficient energy generation and storage, photo-enhanced RZBs that combine photochemical and electrochemical energy conversion and storage with the help of solar energy, are a promising research focus. Photo-enhanced RZBs require a photoactive OER/ORR bifunctional cathode that is not merely an electrochemical catalyst but also a photo-active catalyst.In the present study, we developed a photoactive bifunctional air-electrocatalyst with a staggered p-n heterojunction band gap structure, comprising n-type g-C3N4 and p-type copper-doped ZIF-67 (CuZIF-67) composite, to accelerate sluggish OER/ORR processes via a durable structure and stable long-cycle-life performance for photo-enhanced RZBs. g-C3N4/CuZIF-67 has a suitable band gap, which ensures wide-range light absorption in the UV–Vis–NIR region, and stimulates more electrons to participate in ORR/OER electrocatalytic activity. Besides, it has a staggered bandgap structure and a BEF at the p-n junction of the catalyst, which improves electron–hole pairs separation efficiency, lowers overpotential, promotes ORR/OER electrocatalytic activity, and eventually enhances the efficiency of RZBs (the voltage gap was significantly decreased by 14% with simulated solar light irradiation). Moreover, a high concentration of pyrrolic-N groups in the cathode material, resulting in the excellent electrochemical durability of RZBs during charge/discharge cycles. The photo-enhanced RZB based on the g-C3N4/CuZIF-67 bifunctional catalyst exhibits good round-trip efficiency of 60% (2 mA cm-2) with a significantly decreased voltage gap (from 0.92 to 0.81 V) after 1000 cycles, under simulated solar light irradiation. It can be concluded that staggered p-n heterojunction and pyrrolic nitrogen-rich groups play an important role in efficient and durable photo-enhanced Zn-air batteries.

Renewable energy systems and designing economically viable electrochemical energy storage systems is essential to decrease environmental pollution concerns while meeting the growing energy demand. Among the various energy storage devices, rechargeable zinc-air batteries (RZAB) have attracted great attention due to their relatively high specific energy (1218 W.h/kg), and volumetric energy density (6136 W.h/L) cost-effectiveness, and environmental friendliness, comparable to that of lithium–air batteries [1]. However, the sluggish kinetics of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) during the discharge and recharge process of the air cathode on RZAB prevents large-scale application. So far noble metals (Pt, Ru, Ir) and their alloys (Pt-Ru/C) are used as bifuctional oxygen electrocatalysts in commercial rechargeable RZAB, yet they are too expensive to be viable for large-scale commercial applications. Therefore, designing robust and cost-effective bifunctional oxygen electrocatalysts is prime of importance for RZAB to be commercialized [2]. One of the most promising oxygen bifunctional catalyst are perovskite oxides due to their structural and compositional flexibility [3]. Moreover, the electronic structure of perovskite oxides can be tuned by varying the transition metals at the B site and thus their electrocatalytic performance [4-5].In this work, first we will demonstrate phase pure fabrication of double perovskite oxide series of NdBaCoXO5+δ (X= Fe, Ni, Mn). Second, OER and ORR performances of the series of NdBaCoXO5+δ (X= Fe, Ni, Mn) will be explained in relation with their electronic structure and work function. Here, we applied NdBaCoMnO6 on a home-made RZAB as air cathode, according to its bifunctional index. Therefore, we will finally present charge-discharge performance of RZAB with NdBaCoMnO6 as air cathode. J. Fu, Z. P. Cano, M.G. Park, A. Yu, M. Fowler, Z. Chen, Advanced Materials, 29, 1604685 (2016).Y. Tong, J. Wu, P. Chen, H. Liu, W. Chu, C. Wu, Y. Xie, Journal of the American Chemical Society, 140, 11165-11169 (2018).W. Yin, B. Weng, J. Ge, Q. Sun, Z. Li, Y. Yan, Energy & Environmental Science, 12, 442-462 (2019).J. Ahmed, N. Alhokbany, M. Ubaidullah, S. Mutehri, M. M. Khan, S. M. Alshehri, Ceramics International, 46, 20038-20044 (2020).A. Mulder, N. Benedek, J. Rondinelli and C. Fennie, Advanced Functional Materials, n/a-n/a (2013).

As one of the proposed post lithium-ion technologies, zinc-air batteries have received revived interest in the recent years, which is driven by the increased demand of high-performance, efficient, safe and environmentally friendly energy storage solutions. These energy storage systems need to address variable power, capacity and profitability requests. Zinc-air batteries with specific energy density higher than lithium-ion and low-cost, highly available, eco-friendly active materials are suitable to fulfill these requirements. The use of a flow battery type with zinc-particles suspended in alkaline solution (zinc-slurry) in addition with high performance oxygen-reduction electrodes enables the development of high-power zinc-air batteries. This setup also enables the independent scaling of capacity and power. The cooperative project, ZnMobil, founded by the Federal Ministry of Economic Affairs and Energy in Germany combines the experience of industrial and academic partners (Covestro Deutschland AG; Grillo-Werke AG; VARTA Microbattery GmbH; Accurec Recycling GmbH; Technical University Freiberg, Gottfried Wilhelm Leibniz University Hannover; University of Duisburg-Essen; the fuel cell research center ZBT GmbH) to develop a high-performance and low-cost zinc-air flow battery. Here we present strategies to improve the depth-of-discharge of zinc-air flow batteries. The battery system consists of a 100 cm² copper plate as current collector for the zinc-suspension electrode and an oxygen reduction electrode with gas-diffusion layer (supplied by Covestro). The zinc-slurry contains zinc particles (supplied by Grillo) suspended in alkaline solution (30 wt-% KOH) and stabilized with polyacrylic acid. The battery performance and depth-of-discharge were measured for several additives added to the zinc-slurry. Furthermore, the influence of the discharge current density on the depth-of-discharge was evaluated for these setups. Depending on the current density and additive selection, it is possible to achieve depth-of-discharge up to 90 %.

High-performance rechargeable zinc-air batteries enabled by cobalt iron anchored on nitrogen-doped carbon matrix as bifunctional electrocatalyst

The century-old zinc-air (Zn-air) battery concept has been revived in the last decade due to its high theoretical energy density, environmental-friendliness, affordability, and safety. Particularly, electrically rechargeable Zn-air battery technologies are of great importance for bulk applications like electric vehicles, grid management, and portable electronic devices. Nevertheless, Zn-air batteries are still not competitive enough to realize widespread practical adoption because of issues in efficiency, durability, and cycle life. Here, following an introduction to the fundamentals and performance testing techniques, the latest research progress related to electrically rechargeable Zn-air batteries is compiled, particularly new key findings in the last five years (2013-2018). The strategies concerning the development of Zn and air electrodes are in focus. The design of other battery components, namely electrolytes and separators are also discussed. Poor performance of O2 electrocatalysts and the lack of the long-term stability of Zn electrodes and electrolytes remain major challenges. Finally, recommendations regarding the testing routines and materials design are provided. It is hoped that this up-to-date account will help to shape the future research activities toward the development of practical electrically rechargeable Zn-air batteries with extended lifetime and superior performance.

Highly efficient nitrogen-doped three-dimensional interconnected porous carbon supported heterogeneous Co/MnO nanoparticles oxygen electrocatalysts for rechargeable zinc air batteries

We report a hybrid battery that integrates a Zn-Ag battery and a Zn-air battery to utilize the unique advantages of both battery systems. In the positive electrode, Ag nanoparticles couple the discharge behaviors through the two distinct electrochemical systems by working as the active reactant and the effective catalyst in the Zn-Ag and Zn-air reactions, respectively. In the negative electrode, in situ grown Zn particles provide large surface areas and suppress the dendrite, enabling the long-term operating safety. The battery first exhibits two-step voltage plateaus of 1.85 and 1.53 V in the Zn-Ag reaction, after which a voltage plateau of 1.25 V is delivered in the Zn-air reaction, and the specific capacity reaches 800 mAh gZn-1. In addition, excellent reversibility and stability with maintaining high energy efficiency of 68% and a capacity retention of nearly 100% at 10 mA cm-2 are demonstrated through 100 cycles, outperforming both conventional Zn-air and Zn-Ag batteries. This work brings forth a conceptually novel high-performance battery, and more generally opens up new vistas for developing hybrid electrochemical systems by integrating the advantages from two distinct ones.

An advanced zinc air battery with nanostructured superwetting electrodes

High performance batteries currently used in laptop computers, cell phones, and other portable electronic devices have been making small improvements for decades. Nevertheless, such power supplies have inherent limitations which restrict the advancement of the technical capability of these electronic devices. For instance, the designer must strike a balance between compactness and run time. As batteries age, run time typically drop significantly, so the designer must oversize the battery system initially, thus adding weight and increasing the cost. Overall efficiency is also an issue, as losses occur during generation of electricity at the power plant, in transmission, in charging, in slow discharge during storage, and finally in conversion of stored chemical energy into electrical energy at time of use. Direct methanol fuel cells (DMFCs) are an emerging technology which has the potential to improve on several of these limitations. In the DMFC, methanol/water mixtures react and produce hydrogen ions and electrons electrochemically. The electrons flow through the load circuit, while the ions diffuse through a membrane electrolyte, completing the reduction reaction at the cathode in the presence of oxygen from air. This paper aims to compare the DMFC systems against conventional batteries in respect of energy capacity degradation, gravimetric and volumetric energy densities. It is concluded that, although the initial mass and volume of a DMFC system dominate the gravimetric and volumetric energy densities profile respectively for a short operation time, the methanol conversion efficiency becomes the dominant factor as the operation time increases. Depending on the initial system mass and volume and conversion efficiency, commercially available DMFC systems can offer weight advantages over current battery technology for operation times longer than 10 hours and volume advantages for the operation time longer than 50 hours. Near-term advances in these break-even times are expected to be an order of magnitude, given the relatively rapid development rate of the DMFC. Additionally, although the energy capacity of both the DMFC system and the battery degrades with operation time, the degradation for the battery is typically higher, especially for long time of service. For these reasons, DMFC systems appear to be highly promising for portable electronic devices.

Recent advances of micro-nanofiber materials for rechargeable zinc-air batteries

Li-ion batteries are widely used in portable electronic devices because of their higher specific capacity, higher energy density and good cycle life compared to previous batteries. However, they are limited to use for HEV(Hybrid Electronic Vehicle), EV(Electronic Vehicle) and other big electronic devices because most commonly used battery cathode material like the LiCoO2 (LCO) has insufficient performance. Thus, need to research continue to be directed finding new cathode materials for use large-scale electronic devices. Until now, several different materials have been investigated for alternative cathode materials in order to improve the performance of Li-ion batteries. In various cathode materials, poly-oxyanion compounds with strong binding with oxygen have excellent thermal stability than other cathode materials. Among these, phosphate (LiTMPO4(TM=Fe, Mn, Co and so on)) is interested in many researchers because this material is show the higher capacity (~170mAh/g) than existing material like LCO (~120mAh/g), and has very safety. And this cathode material has stable structure and was show almost theoretical capacity because phosphate has octahedral structure that six oxygen atoms are formed octahedron with transition metal (TM). The octahedral structure is very stable, so cannot occur structural problems when Li ion is extracted. However, phosphate has poor ionic conductivity and only one dimensional Li diffusion path so if this path is blocked, diffusivity is many decreased. And iron phosphate LiFePO4 has lower voltage (~3.4V), hence has low energy density and power density. Recently, orthosilicates materials (Li2TMSiO4(TM=Fe, Mn, Co and so on)) receive huge interest because have higher capacity (~330mAh/g) than other cathode materials and safer than commercialized cathode material. However in previous studies, silicate cannot show theoretical capacity and has poor electrochemical properties. For example, Li2FeSiO4 (LFS) only show more than 160mAh/g with reversible capacities of 120-140mAh/g cannot show theoretical capacity 330mAh/g. Silicates are polymorphism through synthesis method, so have many space groups like Pmn21, P21n, Pmnb and so on. These structures are all tetrahedral structures that four oxygen atoms are formed tetrahedron with transition metal (TM). The tetrahedral structure has structural problems when Li ion is extracted because relatively few oxygen atoms are formed. Therefore, polyhedrons are changed when Li ion is extracted, so this change is occurred structural problems and cannot shows theoretical capacity. If transition metal of phosphate and silicate is Fe, the materials have strong point at price because Fe is cheaper than other transition metals and the Fe is very safer than other transition metals. In this research, we suggest new design polyoxy-anion cathode material structure for develop battery performance. This material is that substituted from phosphorus(P) to silicon(Si) step by step, next we show that substituted structures have developed properties and structural stability when occurred charge and discharge process at Li ion battery. We named that this new design cathode material is phospho-silicate LiFeP1-xSixO4(LFPS). However, phosphate has olivine structure and silicates have all tetrahedral structures, so we don’t know the structure when mixed P and Si. Therefore we calculated the most stable structure when mixed P and Si based on first principles calculation among possible structures, and found that most stable structure is olivine structure. So we calculated several properties the olivine structure LFPS. As a result, the LFPS is controlled voltage because voltage is increased linearly following Si ratio. And this result is very positive because increased voltage is meant that increase energy density and power density. This point was critical disadvantage of olivine iron phosphate. Next when mixed Si and P, Li-O bonding length is increased linearly, this result means that diffusivity is better than original material’s kinetically. And Fe-O bonding length is decreased, that is Fe-O bonding strength is increased, so anti-site defect that induced Li path blocked is prevented. Finally, we validated this research result through experiment. This research of the new polyoxy-anion compound cathode material that used ab-initio study and experiment show the new promising cathode material compared with existing cathode material like LCO. Furthermore, the research provides the different directions that can develop the Li ion battery, so advanced for using HEV(Hybrid Electronic Vehicle), EV(Electronic Vehicle) and other big electronic devices.

As one of the most promising power sources in converting and storing chemical energy, aqueous zinc-air batteries (ZABs) stand out because of their high theoretical energy density, low cost, high safety of aqueous electrolyte, and environmental friendliness. Three main types of ZABs including primary ZABs, mechanically rechargeable ZABs, and electrically rechargeable ZABs have been developed up to now.[1] Primary ZABs for single use are usually discarded after the Zn anode is consumed or passivated although other parts of battery remain intact, leading to enormous waste. To address it, the depleted anode and failure electrolyte can be physically replaced to recover the capacity in mechanically rechargeable ZABs. But the cumbersome disassembly/reassembly process and the performance deterioration after every recharge process limit its practical application. In addition, it is not feasible to replace zinc in some integrated systems, such as the large-scale ZAB stack. Electrically rechargeable ZABs with bifunctional oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) catalysts could be returned to the original state by electrochemical charging process, but also face some formidable challenges, such as dendritic zinc deposition, electrode deformation, and hydrogen evolution, limiting the long-term cycling performance. Besides, sluggish kinetics of ORR/OER and Zn passivation result in low energy efficiency, limited depth of discharge and power density. Especially in the resource-constrained and off-grid region, there isn’t external electricity source to charge the electrically rechargeable ZABs which limits their applications. Moreover, the reactions inherently take place on the surface of Zn anode and air cathode, in which the storage and conversion capability of the cell would be essentially constrained by the surface area of electrode and the volume of electrode compartment.The concept of redox targeting (RT) of battery materials offers a feasible solution to address these issues by employing redox mediators (RMs). To tackle the above challenges, here we demonstrate a redox-mediated Zn-air fuel cell (RM-ZAFC) based on the RT reactions of cobalt triisopropanolamine complex (CoTiPA) with O2 and 7,8-dihydroxy-2-phenazinesulfonic acid (DHPS) with Zn metal in the catholyte and anolyte, respectively. Both the 4-electron (4 e-) ORR and Zn oxidation reactions are liberated from the electrode surface and occur inside separate reactor tanks resorting to the RT processes. Upon operation, Co(III)TiPA in the catholyte is electrochemically reduced to Co(II)TiPA on the cathode and chemically oxidized back through ORR in the gas diffusion tank (GDT) into which O2 is fed. In conventional ZABs, ORR takes place on the triple-phase reaction interface of the heterogeneous electrocatalyst, and the catalytic performance is closely related to the density of exposed active site, electrical conductivity and reaction energy barrier. As compared, the redox-mediated ORR in GDT occurs homogeneously in the catholyte in which the dissolved RM could provide a large quantity of rection sites with tunable reaction energy barrier. For the negative side, DHPS-2H is firstly oxidized to DHPS on the anode and circulated into anodic tank, where it is regenerated by oxidizing Zn to ZnO. The discharge product ZnO is formed and deposited on the Zn granules loaded in the tank. After fully discharged, the cell can be feasibly refueled by replacing the Zn granules in the tank instead of disassembling and reassembling the whole cell. In this RM-ZAFC, the energy storage unit is decoupled from the power generation unit, thus offering greater operation flexibility and system scalability with modular design than the conventional ZABs. Compared with the commercial hydrogen tank used in hydrogen fuel cells, Zn granules loaded in the anodic tank present much higher volumetric capacity, greater safety and ease for storage and transportation. Therefore, as an energy conversion and storage device, RM-ZAFC would have great promise for automotive, backup, and stationary power applications.[2] In addition, we also propose an efficient and zinc regeneration method by RT reaction between RM and the product ZnO in RM-ZAFC to avoid the waste of ZnO and reduce the cost.