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Research Papers

# A Low-Cost Mechanically Rechargeable Aluminum–Air Cell for Energy Conversion Using Low-Grade Aluminum FoilOPEN ACCESS

[+] Author and Article Information
Binbin Chen

Department of Mechanical Engineering,
The University of Hong Kong,
Hong Kong
e-mail: cbbchris@connect.hku.hk

Dennis Y. C. Leung

Department of Mechanical Engineering,
The University of Hong Kong,
Hong Kong
e-mail: ycleung@hku.hk

Manuscript received November 16, 2015; final manuscript received January 21, 2016; published online March 2, 2016. Editor: San Ping Jiang.

J. Electrochem. En. Conv. Stor. 13(1), 011001 (Mar 02, 2016) (5 pages) Paper No: JEECS-15-1007; doi: 10.1115/1.4032669 History: Received November 16, 2015; Revised January 21, 2016

## Abstract

The performance of a mechanically rechargeable aluminum (Al)–air cell, fabricated with low-cost materials including low-grade aluminum foil and carbon paper electrodes, was evaluated. The design adopted a free gravity flow for the electrolyte to eliminate the use of an external pump. A tank for storing waste electrolyte was designed with a dedicated channel for the collection of hydrogen gas generated during the cell discharge. The cell achieved a high utilization efficiency of aluminum. Considering both the electricity and hydrogen generated, an overall utilization efficiency of around 90% or even higher could be achieved under different working voltages. Results of repeated recharging/discharging showed that the performances of the cell could be maintained for repeated refilling.

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## Introduction

Growing energy demands from daily lives and industrial manufacturing have been a driving motivation for progress in advanced energy research for decades. Great emphasis has been focused on developing energy sources and storages with high energy and capacity densities, low cost and environmental friendliness [1]. Metal–air cells, featuring high energy density, have received sustained interest from the research community and have been envisioned as promising energy sources for electric vehicles, energy storage, emergency power supply, and other applications [2,3].

Among the different kinds of metal–air cells, Al–air cells hold the highest volumetric capacity density at 8.05 A h cm−3, benefitting from the trivalence of Al ions [4]. Additional advantages of an Al–air cell include low cost and environmental friendliness. Furthermore, the Al energy conversion process is characterized by 100% recyclability in theory [5]. With a large base of raw material reserves, Al attracts considerable attention as a promising material to be integrated within the global energy system [6]. The Al–air cell is a promising alternative to conventional batteries and power sources and has been investigated since the 1960s [7]. In 2014, Phinergy Company first demonstrated an electric vehicle based on Al–air cells with a 1100-mile range [8].

However, successful early applications in the military services notwithstanding [9], several problems exist that prevent the wider civilian use of Al–air cells. The two most serious issues considered by researchers are: (a) the parasitic corrosion of Al when contacting with electrolyte [10,11] (Eq. (1)), due to its quite high chemical reactivity with water Display Formula

(1)$A1+3H2O=A1(OH)3+32H2$

and (b) the formation of a passive oxide or hydroxide layer on the Al surface, which inhibits the continuous reaction and increases the overpotential of the anode [12]. By employing a high-pH alkaline aqueous electrolyte, the passive layer could be destroyed by the hydroxide ions (Eqs. (2) and (3)) Display Formula

(2)$A12O3+2OH−=2 A1O2−+H2O$

(3)$A1(OH)3+OH−=A1(OH)4−$

Nevertheless, the high-pH electrolyte will also accelerate the corrosion reaction of Al with water, generating hydrogen that lowers its utilization efficiency. The rate of the corrosion reaction determines the loss in utilization efficiency of Al within the cell.

To overcome this problem, super-pure Al (≥99.99%), alloyed with various trace elements such as Pb, Hg, Mg, Sn, In, and Ga, can be used to increase the corrosion resistance [1315]. These elements are expected to increase the overpotential of hydrogen generation. Nevertheless, high-purity Al alloys are costly and require high energy consumption during production process [5]. This method could not really provide a widely practical way for Al electric energy conversion. An alternative approach is to add inhibitors or additives directly into the electrolyte, including using organic or alternative solvents to replace aqueous solvent [16,17]. However, such additives would increase the internal ohmic resistance of the cell by changing the electrolyte to gel during operation, and would hamper the cell performance due to the formation of an insoluble precipitate of Al(OH)3. Furthermore, it normally requires the use of anionic exchange membranes to provide an independent environment for the air cathode [18], in case of tampering the reduction of oxygen. Researchers have also investigated the grain size of Al as a factor on corrosion resistance, and found that the corrosion resistance can be improved by refining the grain size of Al [19]. However, these methods have so far not provided satisfactory solutions for the problems within Al–air cells. A novel idea to solve the low utilization efficiency problem proposed by recent research is to utilize the hydrogen generated from the corrosion as a clean fuel [20].

For the operation of aqueous Al–air cells, there are still other minor problems. One of them is the formation of aluminum hydroxide in the electrolyte, which is a reaction product of Al oxidation during discharging. This process increases the electrolyte density and decreases its ionic conductivity [21]. Another problem is the carbonation process within the gas diffusion layer of the cathode. The CO2 from the air would react with the alkaline electrolyte forming carbonates that would block the porosity of the gas diffusion electrode [4]. Both these problems degrade performance of the cells.

The present work aims to restructure an operation system for Al–air cells. This operation system provides a low-cost strategy for harvesting energy from secondary Al, which is abundant in our society. During experiment, pure hydrogen gas could be obtained and collected for various commercial uses such as for fuel cells and the internal combustion engine. As both the electricity and hydrogen generated from the parasitic corrosion could be utilized, this is considered an effective approach for utilization of Al, eliminating the necessity of using super-pure Al alloys or inhibitors in the cells. In the first part of this research work, to ensure the repeatability of the flows, we investigated the performance of the mechanically rechargeable Al–air cell with a constant electrolyte flow rate using a syringe pump. Then the whole system was assembled together without the syringe pump and the feasibility of operation was demonstrated.

## Methodology

###### Chemicals.

Electrolyte of 1 M of a potassium hydroxide (KOH) aqueous solution was prepared by dissolving KOH pellets (≥85%, Sigma Aldrich, Shanghai) in de-ionized water (Barnstead, NANOpure Dlamond). Kitchen Al foil, which contained low-grade Al, was used as anode. The compositions of this Al foil were analyzed by EDX (energy-dispersive X-ray; Leo 1530 FEG SEM) to be 99.0% purity of Al with trace amounts of Fe and Ag as impurities. The Al foil was folded in several layers to a thickness of about 0.5 mm and cut to fit the specially designed anode cartridge. Low-cost HCP 120 carbon paper (Hesen Company, Shanghai, China) was used as a gas diffusion cathode without any catalyst loading. All experiments were conducted under standard ambient temperature (25 °C/ ±1 °C) and pressure conditions.

###### System Fabrication.

The operation system was composed of four parts: a fresh electrolyte tank, a mechanically rechargeable Al–air cell, a waste electrolyte tank and a hydrogen collection device.

Figure 1(a) shows the schematic illustration of the mechanically rechargeable Al–air cell structure. The structure consisted of five polymethylmethacrylate (PMMA) plates with consecutive thicknesses of 1.0 mm, 0.5 mm, 2.0 mm, 2.0 mm, and 1.0 mm, cut by a carbon dioxide laser ablation system (VLS 2.30, Universal Laser System, Warminster, PA). Adjacent PMMA plates were adhered by double-sided adhesive tape. The carbon paper cathode, with an active area of 22 mm × 13 mm, was assembled within the cathode structure layers. The anode structure layers left a cuboid space for the Al anode cartridge. As shown in Fig. 1(b), the anode cartridge consisted of three PMMA plates with thicknesses of 1.0 mm, 0.5 mm, and 0.5 mm, respectively. Al foil was put within the middle layer. The block layer was utilized for pressing the Al foil, keeping it from contacting the cathode. Once the cell was assembled, AB glue was used to ensure good sealing of the cell. In the present design, the cathode was made of low-cost carbon paper, which could be replaced economically when the cell performance decreased due to carbonation or porosity structure damage. Fluidic electrolyte could remove aluminum hydroxide precipitate and solve the electrolyte deterioration problem.

The fresh and the waste electrolyte tanks were cast with an alkaline-resistant polymer as shown in Fig. 2. The inset in Fig. 2 shows a sectional view of the inner channel of the waste electrolyte tank. The altitude difference between electrolyte and gas outlets ensures that liquid electrolyte and gas can flow out through their own outlets separately. The fresh electrolyte tank was located at a higher level, so that it could drive the electrolyte flow by gravity force. A gas sample bag, connected to the gas outlet, was used as a hydrogen collection device.

The inlets and outlets of different components were connected via 1.5 mm of tubing bonded to the ports with epoxy. The outlet of the fresh electrolyte tank was connected to the cell inlet. The cell outlet was connected to inlet of the waste electrolyte tank. On the tube connecting the outlet of the cell and the inlet of the waste electrolyte tank, a valve was mounted and used to control the flow rate of electrolyte.

###### Cell Performance Testing.

For the cell performance testing, the cell and the waste electrolyte tank were assembled together, while the fresh electrolyte tank was dismantled. For better control of the flow rate during the test, the electrolyte was driven into the cell by a syringe micropump (LSP02-1B, LongerPump, Hebei, China) at a constant flow rate of 500 μl/min. During operation, the gas generated was carried away by the continuous flow of electrolytes.

###### Composition of the Gas Collected.

The composition of the gas collected during cell operation was first analyzed. The Al–air cell was discharged at a constant voltage of 0.7 V. The gas was separated from the reacted electrolyte within the channel of the waste electrolyte tank and then was collected by a gas sample bag. After that, the composition of the gas in the sample bag was analyzed by an Agilent 7890B gas chromatography (GC) system equipped with a thermal conductivity detector.

###### Efficiency Testing.

Before assembling, the mass of the Al foil in the anode cartridge used was measured by a laboratory balance (Shimadzu Libror AEG-120). The volume of gas collected by the sample bag during the process was determined by the water displacement method.

In the gas composition testing, the gas was analyzed as consisting of pure hydrogen (as discussed in Sec. 3.1.1). Both the electricity and hydrogen generated were considered as useful energy and thus effective utilization of Al. The Faradaic efficiency of the system was calculated as Display Formula

(4)$E1=e3qmolmAlMAl$

The hydrogen energy efficiency was calculated as Display Formula

(5)$E2=2V3vmAlMAl$

The total efficiency of Al utilization was Display Formula

(6)$E=E1+E2=e3qmolmAlMAl+2V3vmAlMAl$

In an Al–air cell, the parasitic corrosion reaction rate of Al is related to the working voltage of the cell [20]. When the cell works at a lower voltage, the corrosion rate will be lower. More electrons are released from aluminum oxidation as electrical energy. In this work, Al utilization efficiency under three voltages (e.g., open circuit, 0.7 V and short circuit) was investigated.

###### Charging and Discharging Test.

For the mechanical recharge testing, an open-circuit voltage (OCV) test was first conducted for 200 s. Then the polarization curve was obtained by a potentiostatic current measurement at every 0.2 V for 50 s from 1.4 V to short-circuit (e.g., 0 V) by a CHI 666 E electrochemical workstation (Shanghai Chenhua Instruments Co., Ltd., Shanghai). The average current data in the last 25 s was used to represent the current at that specific voltage. After that, the cell was discharged at 0.7 V until all the Al was consumed. The empty cartridge was then taken out and replaced by a new one. The above testing procedures were repeated ten times during the test.

After ten recharging/discharging cycles, the carbon paper cathode was cut for analysis by scanning electron microscope (Leo 1530 FEG SEM).

###### System Operation Test.

All the four components were assembled together as a whole operation system for the system operation test. Fresh KOH electrolyte was stored at the fresh electrolyte tank and flowed through the cell by gravity. The electrolyte flow rate was affected by many factors such as the height of the fresh electrolyte tank and the position of the valve opening. The flow rate of electrolyte therefore slightly varied during the test. However, the influence of flow rate on performance was found insignificant. To prove the feasibility of this system operation, the polarization curve was measured and compared with the one driven by the micropump. Then a 1 hr discharge test was conducted at a voltage of 0.7 V.

## Results

###### Gas Composition.

To ensure the feasibility of using the gaseous by-product from the Al–air cell, the composition of the gas collected was analyzed by GC. Figure 3 shows the GC result of the gas collected by the collection device. The only peak in the chromatogram appears at 1.290 min, corresponding to hydrogen. During operation, air would be the most possible impurity within the gas collected. However, there is no signal at the referential peak positions for air (mainly O2 and N2). The result indicates that only hydrogen was produced and collected during the discharge of the Al–air cell. The pure hydrogen can be used for various applications such as the fuel cell and internal combustion engine.

###### Utilization Efficiency.

Figure 4 shows the utilization efficiencies of Al in the Al–air cell under three different voltages (i.e., open circuit, 0.7 V and short circuit). At open circuit, electrons from the Al oxidation could not move to the cathode side, which meant there was no electricity generated. The Al only reacted with water to generate hydrogen. When the Al was consumed, in about 2 hrs, the hydrogen collected corresponded to an Al utilization efficiency of 92.0%. When anode and cathode of the cell were connected, a portion of the electrons generated from the Al oxidation could be transferred to the cathode side for oxygen reduction. At a working voltage of 0.7 V, 7.7% of the electrons generated from Al were transferred to the cathode as electricity. On the other hand, the hydrogen collected consumed 86.6% of Al, leading to a total utilization efficiency of 94.3%. At short circuit, an overall efficiency of 89.6% was achieved, including 49.6% from hydrogen and 40.0% from electricity.

As shown in Fig. 4, the overall efficiencies of the Al utilization at different working voltages could always achieve around 90% or even higher. Efficiency loss was due to the small amount of unreacted aluminum in the cell and hydrogen dissolved in the electrolyte, which could be reduced by improved design of the aluminum cartridge. As compared to other Al–air cells, the high conversion efficiencies in the present system are very promising for energy applications.

###### Performance of Repeated Recharging/Discharging.

The polarization performances of the Al–air cell with multiple recharging/discharging cycles (i.e., ten times) are shown in Fig. 5. The OCV of the Al–air cells varied little (1.42 ± 0.02 V) in different cycles. As can be seen, the cell performances significantly increased in the first few rounds. The short circuit current densities increased from 37.0 mA cm −2 to 45.8 mA cm−2. This performance enhancement was probably due to the activation of the carbon paper cathode. After seven recharging/discharging cycles, performance of the cell started to decrease. The cell performance of the tenth round decreased to the level of the first round performance. The total discharge time was over 20 hrs for these ten rounds of recharging/discharging cycles.

###### Cathode Characteristics.

Figure 6 shows comparison of the carbon paper before and after the ten recharging/discharging cycles. After working in the Al–air cell for more than 20 hrs, the carbon paper cathode developed a structure degradation as observed by the SEM. This accounted for the water flooding observed on the back surface of the carbon paper after a long time of discharge and is the cause of the decreasing cell performance. Considering the low cost of carbon paper, it was economically acceptable to replace a new cathode after the carbon paper degradation.

###### System Operation Characteristics.

Figure 7(a) shows comparison of the polarization curves of the Al–air cell system with electrolyte driven by its gravity and the cell with electrolyte driven by a micropump at a constant flow rate of 500 μl/min. As can be seen, the cell performance driven by gravity was slightly lower than that driven by the micropump. Nevertheless, their magnitudes were comparable. During the 1-hr discharge of the cell system at a voltage of 0.7 V (Fig. 7(b)), the current decreased at the first 600 s and then increased thereafter. This was due to the evolution of a passive hydroxide layer at the beginning stage of the discharge. After the outermost Al was consumed, the multilayer structure of the Al foil anode exposed more reaction area, leading to an increase in current. At the end of the 1 hr discharge, a total volume of 147 ml hydrogen was collected from this system.

###### Economy of the Al–Air Cell.

Due to the low energy required by the pretreatment process (0.39 kW hr/kg Al) [22], a relatively high efficiency and low cost can be achieved by the Al–air cell operated in the system. During operation, the energy in the Al transforms into electricity and hydrogen. Considering only the electricity transformation, a maximal value of 4 kW hr/kg Al could be achieved (calculated by multiplying the OCV of 1.4 V with the capacity density of Al (2980 A h/kg-Al)). Based on the current international price of Al of US$1.45/kg [23], the cost of Al for electricity storage is US$0.36/kW hr. The cost for electrolyte, calculated based on Eq. (3) and an industrial KOH price of US$500/Ton, is US$0.25/kW hr. The carbon paper cathode (without other noble metal catalyst loading) could be obtained with a cost of US$10/m2 [24]. Considering the performance in the present operation system, the cost of carbon paper for electricity generation could be as low as US$3.40/kW hr. Another important fuel cell metrics is the cost for unit power output ($/kW). Based on a power density of 15 mW cm−2 in this work, the cost of carbon paper is estimated to be US$7/kW. The price for fabricating the system is estimated within a range of US$50–100, depends on the volume of manufacturing. This cost is more competitive than that of the polymer exchange membrane fuel cell with projected cost of US$53–280/kW by DOE [25].

Furthermore, secondary aluminum has been proved to be a promising source to generate hydrogen at a low cost [26]. For hydrogen generation from Al, 1 kg of hydrogen corresponds to a consumption of 9 kg of Al. The proposed production price for hydrogen is around US$13/kg-H2, which is comparable with different approaches (US$4–30/kg-H2) [27]. As these calculations are based on the present work with commercially available products, higher efficiency and lower cost would be achieved with special-purpose optimized materials. Furthermore, Al(OH)3 will be produced as a by-product of the Al energy conversion process, which can be recycled for the recovery of Al. The recycling process provides an environmentally friendly and sustainable path for Al energy conversion.

## Conclusion

Present work is directed to a cell operation system for metal–air electrochemical power sources, with particular focus on Al–air cells. The objective of this study is to develop a strategy for the utilization of low-cost materials (secondary Al and carbon paper) for energy production. By collecting the hydrogen from the parasitic corrosion of Al, this system eliminates the use of super pure Al alloys or corrosion inhibitors to overcome the low utilization efficiency problem. The fluidic electrolyte helps to refresh reaction materials, and flush away the produced aluminum hydroxide, avoiding precipitation or gelling of electrolyte. Driven by gravity force, the use of an external pump for liquid electrolyte can be avoided. The mechanically rechargeable cell structure allows replacement of new Al anode once consumed. The product in the waste electrolyte can be recycled to produce industrial grade Al.

In the present system, electricity transformation rate is low, compared with hydrogen generation. High overpotential loss on cathode (carbon paper) and impurities within the Al foil would accelerate the generation of hydrogen. In this study, the system and the microstructure of the carbon paper and Al foil used have not been optimized. Further works would be focused on the system and materials optimization, considering both cost and electrochemical properties, to improve the ratio of electricity to hydrogen generation. Solutions such as non-noble metal catalysts and corrosion-resistant Al alloys will help further improve the performance.

In the present system, a cartridge for the anode (Al) is designed as it is expected to be consumed much faster than the cathode (carbon paper). A similar cartridge system can be designed for the cathode if necessary so that all the consumable parts can be mechanically rechargeable. The system could also be applied in other metal–air cells and is suitable for emergency power supply, power plant, and other applications. The low-cost feature implies great potential for commercialization. Further optimization, such as scaling up and optimization of fabrication, will help to convert the technology into practical market offerings.

## Acknowledgements

The authors would like to acknowledge the support from the Hong Kong Research Grant Council GRF#714313 and SRT on Clean Energy of the University of Hong Kong.

## Nomenclature

• e =

quantity of electricity transferred, C

• mAl =

mass of Al used, g

• MAl =

molar mass of Al, 26.98 g/mol

• qmol =

quantity of electricity of 1 mole of electrons, 9.65 × 104 C/mol

• v =

volume of 1 mole of gas at 25 °C, 25.4 l/mol

• V =

volume of hydrogen collected, l

## References

Wang, H. , Leung, D. , Leung, M. , and Ni, M. , 2009, “ A Review on Hydrogen Production Using Aluminum and Aluminum Alloys,” Renewable Sustainable Energy Rev., 13(4), pp. 845–853.
Armand, M. , and Tarascon, J.-M. , 2008, “ Building Better Batteries,” Nature, 451(7179), pp. 652–657. [PubMed]
Winter, M. , and Brodd, R. J. , 2004, “ What Are Batteries, Fuel Cells, and Supercapacitors?,” Chem. Rev., 105(10), pp. 4245–4270.
Li, Q. , and Bjerrum, N. J. , 2002, “ Aluminum as Anode for Energy Storage and Conversion: A Review,” J. Power Sources, 110(1), pp. 1–10.
Wang, H. , Leung, D. Y. , and Leung, M. K. , 2012, “ Energy Analysis of Hydrogen and Electricity Production From Aluminum-Based Processes,” Appl. Energy, 90(1), pp. 100–105.
Shkolnikov, E. , Zhuk, A. , and Vlaskin, M. , 2011, “ Aluminum as Energy Carrier: Feasibility Analysis and Current Technologies Overview,” Renewable Sustainable Energy Rev., 15(9), pp. 4611–4623.
Zaromb, S. , 1962, “ The Use and Behavior of Aluminum Anodes in Alkaline Primary Batteries,” J. Electrochem. Soc., 109(12), pp. 1125–1130.
Edelstein, S. , 2014, “ Aluminum–Air Battery Developer Phinergy Partners With Alcoa,” Green Car Reports, epub.
Tuck, C. D. , 1991, Modern Battery Technology, Ellis Horwood, New York.
Armstrong, R. , and Braham, V. , 1996, “ The Mechanism of Aluminium Corrosion in Alkaline Solutions,” Corros. Sci., 38(9), pp. 1463–1471.
Doche, M. , Novel-Cattin, F. , Durand, R. , and Rameau, J. , 1997, “ Characterization of Different Grades of Aluminum Anodes for Aluminum/Air Batteries,” J. Power Sources, 65(1), pp. 197–205.
Bernard, J. , Chatenet, M. , and Dalard, F. , 2006, “ Understanding Aluminum Behaviour in Aqueous Alkaline Solution Using Coupled Techniques: Part I. Rotating Ring-Disk Study,” Electrochim. Acta, 52(1), pp. 86–93.
Davis, J. R. , 1999, Corrosion of Aluminum and Aluminum Alloys, ASM International, Materials Park, OH.
Hunter, J. A. , ed., 1989, The Anodic Behavior of Aluminium Alloys in Alkaline Electrolytes, University of Oxford, Oxford, UK.
Macdonald, D. , Lee, K. , Moccari, A. , and Harrington, D. , 1988, “ Evaluation of Alloy Anodes for Aluminum–Air Batteries: Corrosion Studies,” Corrosion, 44(9), pp. 652–657.
Zhang, Z. , Zuo, C. , Liu, Z. , Yu, Y. , Zuo, Y. , and Song, Y. , 2014, “ All-Solid-State Al–Air Batteries With Polymer Alkaline Gel Electrolyte,” J. Power Sources, 251, pp. 470–475.
Abdel-Gaber, A. , Khamis, E. , Abo-ElDahab, H. , and Adeel, S. , 2008, “ Inhibition of Aluminium Corrosion in Alkaline Solutions Using Natural Compound,” Mater. Chem. Phys., 109(2), pp. 297–305.
Wang, L. , Liu, F. , Wang, W. , Yang, G. , Zheng, D. , Wu, Z. , and Leung, M. K. , 2014, “ A High-Capacity Dual-Electrolyte Aluminum/Air Electrochemical Cell,” RSC Adv., 4(58), pp. 30857–30863.
Fan, L. , and Lu, H. , 2015, “ The Effect of Grain Size on Aluminum Anodes for Al–Air Batteries in Alkaline Electrolytes,” J. Power Sources, 284, pp. 409–415.
Wang, L. , Wang, W. , Yang, G. , Liu, D. , Xuan, J. , Wang, H. , Leung, M. K. , and Liu, F. , 2013, “ A Hybrid Aluminum/Hydrogen/Air Cell System,” Int. J. Hydrogen Energy, 38(34), pp. 14801–14809.
Chu, D. , and Savinell, R. F. , 1991, “ Experimental Data on Aluminum Dissolution in KOH Electrolytes,” Electrochim. Acta, 36(10), pp. 1631–1638.
Choate, W. T. , and Green, J. A. S. , 2007, “ U.S. Energy Requirements for Aluminum Production: Historical Perspective, Theoretical Limits and Current Practices,” U.S. Department of Energy, Washington, DC.
LME, 2016, “ LME Aluminium,” London Metal Exchange Ltd., London,
Logan Lab, 2015, “ Frequently Asked Questions About MFCs and Our Replies,” Penn State University, University Park, PA,
Satyapal, S. , 2015, “ 2015 Annual Progress Report: No. I. Introduction,” U.S. Department of Energy Hydrogen and Fuel Cell Program, Washington, DC,
Riis, T. , Hagen, E. F. , Vie, P. , and Ulleberg, Ø. , 2006, “ Hydrogen Production and Storage—R&D Priorities and Gaps,” IEA Hydrogen Implementing Agreement (HIA), International Energy Agency (IEA), Paris.
Zhuk, A. Z. , Sheindlin, A. E. , Kleymenov, B. V. , Shkolnikov, E. I. , and Lopatin, M. Y. , 2006, “ Use of Low-Cost Aluminum in Electric Energy Production,” J. Power Sources, 157(2), pp. 921–926.
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## References

Wang, H. , Leung, D. , Leung, M. , and Ni, M. , 2009, “ A Review on Hydrogen Production Using Aluminum and Aluminum Alloys,” Renewable Sustainable Energy Rev., 13(4), pp. 845–853.
Armand, M. , and Tarascon, J.-M. , 2008, “ Building Better Batteries,” Nature, 451(7179), pp. 652–657. [PubMed]
Winter, M. , and Brodd, R. J. , 2004, “ What Are Batteries, Fuel Cells, and Supercapacitors?,” Chem. Rev., 105(10), pp. 4245–4270.
Li, Q. , and Bjerrum, N. J. , 2002, “ Aluminum as Anode for Energy Storage and Conversion: A Review,” J. Power Sources, 110(1), pp. 1–10.
Wang, H. , Leung, D. Y. , and Leung, M. K. , 2012, “ Energy Analysis of Hydrogen and Electricity Production From Aluminum-Based Processes,” Appl. Energy, 90(1), pp. 100–105.
Shkolnikov, E. , Zhuk, A. , and Vlaskin, M. , 2011, “ Aluminum as Energy Carrier: Feasibility Analysis and Current Technologies Overview,” Renewable Sustainable Energy Rev., 15(9), pp. 4611–4623.
Zaromb, S. , 1962, “ The Use and Behavior of Aluminum Anodes in Alkaline Primary Batteries,” J. Electrochem. Soc., 109(12), pp. 1125–1130.
Edelstein, S. , 2014, “ Aluminum–Air Battery Developer Phinergy Partners With Alcoa,” Green Car Reports, epub.
Tuck, C. D. , 1991, Modern Battery Technology, Ellis Horwood, New York.
Armstrong, R. , and Braham, V. , 1996, “ The Mechanism of Aluminium Corrosion in Alkaline Solutions,” Corros. Sci., 38(9), pp. 1463–1471.
Doche, M. , Novel-Cattin, F. , Durand, R. , and Rameau, J. , 1997, “ Characterization of Different Grades of Aluminum Anodes for Aluminum/Air Batteries,” J. Power Sources, 65(1), pp. 197–205.
Bernard, J. , Chatenet, M. , and Dalard, F. , 2006, “ Understanding Aluminum Behaviour in Aqueous Alkaline Solution Using Coupled Techniques: Part I. Rotating Ring-Disk Study,” Electrochim. Acta, 52(1), pp. 86–93.
Davis, J. R. , 1999, Corrosion of Aluminum and Aluminum Alloys, ASM International, Materials Park, OH.
Hunter, J. A. , ed., 1989, The Anodic Behavior of Aluminium Alloys in Alkaline Electrolytes, University of Oxford, Oxford, UK.
Macdonald, D. , Lee, K. , Moccari, A. , and Harrington, D. , 1988, “ Evaluation of Alloy Anodes for Aluminum–Air Batteries: Corrosion Studies,” Corrosion, 44(9), pp. 652–657.
Zhang, Z. , Zuo, C. , Liu, Z. , Yu, Y. , Zuo, Y. , and Song, Y. , 2014, “ All-Solid-State Al–Air Batteries With Polymer Alkaline Gel Electrolyte,” J. Power Sources, 251, pp. 470–475.
Abdel-Gaber, A. , Khamis, E. , Abo-ElDahab, H. , and Adeel, S. , 2008, “ Inhibition of Aluminium Corrosion in Alkaline Solutions Using Natural Compound,” Mater. Chem. Phys., 109(2), pp. 297–305.
Wang, L. , Liu, F. , Wang, W. , Yang, G. , Zheng, D. , Wu, Z. , and Leung, M. K. , 2014, “ A High-Capacity Dual-Electrolyte Aluminum/Air Electrochemical Cell,” RSC Adv., 4(58), pp. 30857–30863.
Fan, L. , and Lu, H. , 2015, “ The Effect of Grain Size on Aluminum Anodes for Al–Air Batteries in Alkaline Electrolytes,” J. Power Sources, 284, pp. 409–415.
Wang, L. , Wang, W. , Yang, G. , Liu, D. , Xuan, J. , Wang, H. , Leung, M. K. , and Liu, F. , 2013, “ A Hybrid Aluminum/Hydrogen/Air Cell System,” Int. J. Hydrogen Energy, 38(34), pp. 14801–14809.
Chu, D. , and Savinell, R. F. , 1991, “ Experimental Data on Aluminum Dissolution in KOH Electrolytes,” Electrochim. Acta, 36(10), pp. 1631–1638.
Choate, W. T. , and Green, J. A. S. , 2007, “ U.S. Energy Requirements for Aluminum Production: Historical Perspective, Theoretical Limits and Current Practices,” U.S. Department of Energy, Washington, DC.
LME, 2016, “ LME Aluminium,” London Metal Exchange Ltd., London,
Logan Lab, 2015, “ Frequently Asked Questions About MFCs and Our Replies,” Penn State University, University Park, PA,
Satyapal, S. , 2015, “ 2015 Annual Progress Report: No. I. Introduction,” U.S. Department of Energy Hydrogen and Fuel Cell Program, Washington, DC,
Riis, T. , Hagen, E. F. , Vie, P. , and Ulleberg, Ø. , 2006, “ Hydrogen Production and Storage—R&D Priorities and Gaps,” IEA Hydrogen Implementing Agreement (HIA), International Energy Agency (IEA), Paris.
Zhuk, A. Z. , Sheindlin, A. E. , Kleymenov, B. V. , Shkolnikov, E. I. , and Lopatin, M. Y. , 2006, “ Use of Low-Cost Aluminum in Electric Energy Production,” J. Power Sources, 157(2), pp. 921–926.

## Figures

Fig. 1

Schematic illustration of the mechanically rechargeable Al–air cell (a) cell structure and (b) Al anode cartridge

Fig. 2

Exploded view of the operation system, including fresh electrolyte tank, mechanically rechargeable Al–air cell and waste electrolyte tank. The inset is the sectional view of the inner channel of the waste electrolyte tank.

Fig. 3

Chromatogram of the gas sample collected from the Al–air cell operation

Fig. 4

The utilization efficiencies of Al in Al–air cell considering both hydrogen and electricity under three working voltages

Fig. 5

Polarization curves of the Al–air cell with ten times the mechanical recharge

Fig. 6

SEM pictures of the carbon paper before (a) and after (b) discharging over 20 hrs

Fig. 7

(a) Comparison of polarization curves of Al–air cell system driven by gravity and by a micropump and (b) 1-hr discharge performance of the cell system at 0.7 V driven by gravity

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