Statistical approach to design Zn particle size, shape, and crystallinity for alkaline batteries
Brian Lenhart1, Devadharshini Kathan1, Valerie Hiemer1,2, Mike Zuraw3, Matt Hull3, William E. Mustain1()
1. Department of Chemical Engineering, University of South Carolina, Columbia, SC 29208, USA 2. Department of Chemical Engineering, Virginia Polytechnic Institute, Blacksburg, VA 24060, USA 3. Duracell, Bethel, CT 06801, USA
In modern alkaline batteries, the zinc anode is the performance-limiting and lifetime-limiting electrode, making the choice of zinc powder critical. Due to the various material fabrication processes that are used to manufacture industrial zinc powder, there exists a wide array of possible zinc particle shapes, sizes, and crystallinities. These industrial zinc powders are typically conceived, produced, and tested through trial-and-error processes using historical “rules of thumb.” However, a data-driven approach could more effectively elucidate the optimum combination of zinc particle properties. In this paper, the effect of Zn particle size, shape, and crystallinity on the achievable capacity and corrosion current is investigated. The Zn types are tested in both powder and slurry form. Following the data collection, a factorial-based statistical analysis is performed to determine the most statistically significant variables affecting capacity and corrosion. This information is then used to down-select to a subset of particles that are tested in cylindrical cells with an AA-equivalent geometry. The reported technique can be used to develop actionable principles for battery manufacturers to create cells that are more stable, longer lasting, and have higher energy densities.
. [J]. Frontiers in Energy, 2024, 18(5): 650-664.
Brian Lenhart, Devadharshini Kathan, Valerie Hiemer, Mike Zuraw, Matt Hull, William E. Mustain. Statistical approach to design Zn particle size, shape, and crystallinity for alkaline batteries. Front. Energy, 2024, 18(5): 650-664.
W Dong, J L Shi, T S Wang. et al.. 3D zinc on carbon fiber composite framework anode for aqueous Zn-MnO2 batteries. RSC Advances, 2018, 8(34): 19157–19163 https://doi.org/10.1039/C8RA03226B
2
X Chen, Z Zhou, H E Karahan. et al.. Recent advances in materials and design of electrochemically rechargeable zinc–air batteries. Small, 2018, 14(44): 1801929 https://doi.org/10.1002/smll.201801929
3
G Prentice, Y Chang, X Shan. A model for the passivation of the zinc electrode in alkaline electrolyte. Journal of the Electrochemical Society, 1991, 138(4): 890–894 https://doi.org/10.1149/1.2085742
4
J F Parker, J S Ko, D R Rolison. et al.. Translating materials-level performance into device-relevant metrics for zinc-based batteries. Joule, 2018, 2(12): 2519–2527 https://doi.org/10.1016/j.joule.2018.11.007
5
D Desai, X Wei, D A Steingart. et al.. Electrodeposition of preferentially oriented zinc for flow-assisted alkaline batteries. Journal of Power Sources, 2014, 256: 145–152 https://doi.org/10.1016/j.jpowsour.2014.01.026
6
D Chao, C R Zhu, M Song. et al.. A high-rate and stable quasi-solid-state zinc-ion battery with novel 2D layered zinc orthovanadate array. Advanced Materials, 2018, 30(32): 1803181 https://doi.org/10.1002/adma.201803181
7
Z Mao, R E White. Mathematical modeling of a primary zinc/air battery. Journal of the Electrochemical Society, 1992, 139(4): 1105–1113 https://doi.org/10.1149/1.2069348
8
C Cachet, B Saidani, R Wiart. The behavior of zinc electrode in alkaline electrolytes: II. A kinetic analysis of anodic dissolution. Journal of the Electrochemical Society, 1992, 139(3): 644–654 https://doi.org/10.1149/1.2069279
9
E Faegh, B Ng, D Hayman. et al.. Design of highly reversible zinc anodes for aqueous batteries using preferentially oriented electrolytic zinc. Batteries & Supercaps, 2020, 3(11): 1220–1232 https://doi.org/10.1002/batt.202000112
10
S Huang, W Wu, Y Su. et al.. Insight into the corrosion behaviour and degradation mechanism of pure zinc in simulated body fluid. Corrosion Science, 2021, 178: 109071 https://doi.org/10.1016/j.corsci.2020.109071
K E K Sun, T K A Hoang, T N L Doan. et al.. Suppression of dendrite formation and corrosion on zinc anode of secondary aqueous batteries. ACS Applied Materials & Interfaces, 2017, 9(11): 9681–9687 https://doi.org/10.1021/acsami.6b16560
13
P He, J Huang. Detrimental effects of surface imperfections and unpolished edges on the cycling stability of a zinc foil anode. ACS Energy Letters, 2021, 6(5): 1990–1995 https://doi.org/10.1021/acsenergylett.1c00638
14
D Ariosa, F Elhordoy, E A Dalchiele. et al.. Texture vs morphology in ZnO nano-rods: On the X-ray diffraction characterization of electrochemically grown samples. Journal of Applied Physics, 2011, 110(12): 124901 https://doi.org/10.1063/1.3669026
15
T Michlik, A Rosin, T Gerdes. et al.. Improved discharge capacity of zinc particles by applying bismuth-doped silica coating for zinc-based batteries. Batteries, 2019, 5(1): 32 https://doi.org/10.3390/batteries5010032
E Faegh, T Omasta, M Hull. et al.. Understanding the synamics of primary Zn−MnO2 alkaline battery gassing with operando visualization and pressure cells. Journal of the Electrochemical Society, 2018, 165(11): A2528–A2535 https://doi.org/10.1149/2.0321811jes
18
E Faegh, S Shrestha, X Zhao. et al.. In-depth structural understanding of zinc oxide addition to alkaline electrolytes to protect aluminum against corrosion and gassing. Journal of Applied Electrochemistry, 2019, 49(9): 895–907 https://doi.org/10.1007/s10800-019-01330-1
19
E Faegh, B Ng, B Lenhart. et al.. Partial deployment of Al in Zn–MnO2 alkaline battery anodes to improve the capacity and reversibility. Journal of Power Sources, 2021, 506: 230167 https://doi.org/10.1016/j.jpowsour.2021.230167
W Glaeser, S Künzel-Keune, P Merkel. The influence of discharge time on post-partial discharge gassing of zinc powder. Journal of Power Sources, 1999, 80(1–2): 72–77 https://doi.org/10.1016/S0378-7753(98)00252-3
Q Zhang, J Luan, L Fu. et al.. The three-dimensional dendrite-free zinc anode on a copper mesh with a zinc-oriented polyacrylamide electrolyte additive. Angewandte Chemie, 2019, 131(44): 15988–15994 https://doi.org/10.1002/ange.201907830
24
H Li, W Zhang, A Y Elezzabi. Transparent zinc-mesh electrodes for solar-charging electrochromic windows. Advanced Materials, 2020, 32(43): 2003574 https://doi.org/10.1002/adma.202003574
25
M Chamoun, B J Hertzberg, T Gupta. et al.. Hyper-dendritic nanoporous zinc foam anodes. NPG Asia Materials, 2015, 7(4): e178 https://doi.org/10.1038/am.2015.32
26
J S Ko, A B Geltmacher, B J Hopkins. et al.. Robust 3D Zn sponges enable high-power, energy-dense alkaline batteries. ACS Applied Energy Materials, 2019, 2(1): 212–216 https://doi.org/10.1021/acsaem.8b01946
27
G R Dillip, P C Nagajyothi, R Ramaraghavulu. et al.. Synthesis of crystalline zinc hydroxystannate and its thermally driven amorphization and recrystallization into zinc orthostannate and their phase-dependent cytotoxicity evaluation. Materials Chemistry and Physics, 2020, 248: 122946 https://doi.org/10.1016/j.matchemphys.2020.122946
28
J Zhou, M Xie, F Wu. et al.. Encapsulation of metallic Zn in a hybrid MXene/graphene aerogel as a stable Zn anode for foldable Zn-ion batteries. Advanced Materials, 2022, 34(1): 2106897 https://doi.org/10.1002/adma.202106897
29
H Yang, Z Yang, X Wen. et al.. The in-situ growth of zinc-aluminum layered double hydroxides on graphene and its application as anode active materials for Zn–Ni secondary battery. Electrochimica Acta, 2017, 252: 507–515 https://doi.org/10.1016/j.electacta.2017.09.014
30
P Ruan. et al.. Achieving highly proton-resistant Zn–Pb anode through low hydrogen affinity and strong bonding for long-life electrolytic Zn//MnO2 battery. Advanced Materials, 2023, 35(31): e2300577
31
R Yi, X Shi, Y Tang. et al.. Carboxymethyl chitosan-modified zinc anode for high-performance zinc–iodine battery with narrow operating voltage. Small Structures, 2023, 4: 2300020 https://doi.org/10.1002/sstr.202300020
32
X Chen, X Shi, P Ruan. et al.. Construction of an artificial interfacial layer with porous structure toward stable zinc-metal anodes. Small Science, 2023, 3(6): 2300007 https://doi.org/10.1002/smsc.202300007
Z V Marinković, L Mančić, R Marić. et al.. Preparation of nanostructured Zn–Cr–O spinel powders by ultrasonic spray pyrolysis. Journal of the European Ceramic Society, 2001, 21(10–11): 2051–2055 https://doi.org/10.1016/S0955-2219(01)00170-4
36
S Lesz, T Tański, B Hrapkowicz. et al.. Characterisation of Mg–Zn–Ca–Y powders manufactured by mechanical milling. Journal of Achievements in Materials and Manufacturing Engineering, 2020, 103(2): 49–59 https://doi.org/10.5604/01.3001.0014.7194
37
M Inoguchi, K Suzuki, K Kageyama. et al.. Monodispersed and well-crystallized zinc oxide nanoparticles fabricated by microemulsion method. Journal of the American Ceramic Society, 2008, 91(12): 3850–3855 https://doi.org/10.1111/j.1551-2916.2008.02745.x
38
M Rusu, N Sofian, D Rusu. Mechanical and thermal properties of zinc powder filled high density polyethylene composites. Polymer Testing, 2001, 20(4): 409–417 https://doi.org/10.1016/S0142-9418(00)00051-9
39
Z Beji, M Sun, L S Smiri. et al.. Polyol synthesis of non-stoichiometric Mn–Zn ferrite nanocrystals: Structural/microstructural characterization and catalytic application. RSC Advances, 2015, 5(80): 65010–65022 https://doi.org/10.1039/C5RA07562A
40
C C Wang. Method for making irregular shaped single crystal particles and the use thereof in anodes for electrochemical cells. US patent 4487651, 1984
41
B Lenhart, M Zuraw, W Mustain. A scaleable method for enhancing the crystallinity of Zn powder to reduce corrosion and boost achievable capacity. Journal of the Electrochemical Society, 2023, 170(7): 070501 https://doi.org/10.1149/1945-7111/ace082
42
M Bockelmann, M Becker, L Reining. et al.. Passivation of zinc anodes in alkaline electrolyte: Part I. Determination of the starting point of passive film formation. Journal of the Electrochemical Society, 2018, 165(13): A3048–A3055 https://doi.org/10.1149/2.0331813jes
43
L Ye, Z Lai, J Liu. et al.. Effect of Ag particle size on electrical conductivity of isotropically conductive adhesives. IEEE Transactions on Electronics Packaging Manufacturing, 1999, 22(4): 299–302 https://doi.org/10.1109/6104.816098
44
M Bockelmann, L Reining, U Kunz. et al.. Electrochemical characterization and mathematical modeling of zinc passivation in alkaline solutions: A review. Electrochimica Acta, 2017, 237: 276–298 https://doi.org/10.1016/j.electacta.2017.03.143