English

Cathode Materials for Rechargeable Magnesium-Ion Batteries: A Review

• Mochun Zhang ^{1, †,} ,
• Shuo Feng ^{1, †,} ,
• Yunling Wu ^{1, ,} ,
• Yanguang Li ^{1, 2, ,}

• 1.

  Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, Jiangsu Province, China

• 2.

  Macao Institute of Materials Science and Engineering, Macau University of Science and Technology, Taipa 999078, Macau SAR, China

Corresponding author: Email: ylwu@suda.edu.cn (Y.W.); Email: yanguang@suda.edu.cn (Y.L.)

• Received Date: 23 May 2022
  Accepted Date: 24 June 2022
  Revised Date: 22 June 2022
  Available Online: 15 February 2023
• Fund Project:

  the National Natural Science Foundation of China 

  the National Natural Science Foundation of China 

  the National Natural Science Foundation of China 

• ^†These authors contributed equally to this work.

Abstract: Using renewable energy sources such as wind, solar, and tidal power is one of the most effective ways to address the global energy crisis and the ensuing environmental issues. As essential complementary components to renewable energy, high-performance energy storage devices and systems are urgently required. Since the 1990s, the global battery market has been dominated by lithium-ion batteries (LIBs) owing to their high energy density and long cycle life. They have been widely used in portable electronics, and more recently, in electric vehicles. However, lithium resources are limited and unevenly distributed; therefore, the manufacturing costs of LIBs are still high. There is also increasing concern about their operational safety. Thus, it is crucial to develop next-generation battery technologies with lower costs and higher safety. In recent years, magnesium-ion batteries (MIBs) have attracted increasing attention as one of the most promising multivalent ion batteries. The use of magnesium is encouraged owing to its good air stability, lower reduction potential (−2.356 V vs. standard hydrogen electrode), higher volumetric specific capacity (3833 mAh∙cm⁻³), and dendrite-free deposition upon cycling. Moreover, magnesium reserves (2.3%) are 1045 times more than those of lithium (0.0022%), because of which, MIBs are considerably less expensive than LIBs. The development of MIBs has, however, encountered a few challenges arising from the comprising cathodes, electrolytes, and anodes. Mg²⁺ ions with smaller radii and higher charge densities have strong Coulomb interactions with electrode materials, which leads to sluggish kinetics and high diffusion barriers during de-/intercalation. Contemporary electrolytes generally have poor chemical compatibility with cathodes of MIBs, narrow electrochemical windows, and high deposition overpotential, which limits the development of high-voltage MIBs. Moreover, Mg tends to react with organic solvents (especially carbonates and nitriles), forming passivation layers on the surfaces, which increase the interfacial resistance and lead to battery irreversibility. Therefore, material design and technological innovation are crucial for developing commercially viable MIBs. This review focuses on recent advances on MIB cathode materials. First, we present a brief description of the characteristics of MIBs and discuss their strengths and drawbacks. Then, we overview three types of cathode materials, namely, intercalation-type cathodes, conversion-type cathodes, and organic cathodes, followed by a summary of their limitations and recent efforts for addressing the above-mentioned challenges. We conclude with perspectives for future research directions.

Key words:
• Magnesium-ion battery
•  /  Intercalation-type cathode
•  /  Conversion-type cathode
•  /  Organic cathode

• 1. [1]

     Dunn, B.; Kamath, H.; Tarascon, J. M. Science 2011, 334, 928. doi: 10.1126/science.1212741

  2. [2]

     Kittner, N.; Lill, F.; Kammen, D. M. Nat. Energy 2017, 2, 17125. doi: 10.1038/nenergy.2017.125

  3. [3]

     Andrews, J. L.; Mukherjee, A.; Yoo, H. D.; Parija, A.; Marley, P. M.; Fakra, S.; Prendergast, D.; Cabana, J.; Klie, R. F.; Banerjee, S. Chem 2018, 4, 564. doi: 10.1016/j.chempr.2017.12.018

  4. [4]

     Goodenough, J. B.; Park, K. S. J. Am. Chem. Soc. 2013, 135, 1167. doi: 10.1021/ja3091438

  5. [5]

     Canepa, P.; Sai Gautam, G.; Hannah, D. C.; Malik, R.; Liu, M.; Gallagher, K. G.; Persson, K. A.; Ceder, G. Chem. Rev. 2017, 117, 4287. doi: 10.1021/acs.chemrev.6b00614

  6. [6]

     Guo, Z.; Zhao, S.; Li, T.; Su, D.; Guo, S.; Wang, G. Adv. Energy Mater. 2020, 10, 1903591. doi: 10.1002/aenm.201903591

  7. [7]

     Bonnick, P.; Muldoon, J. Adv. Funct. Mater. 2020, 30, 1910510. doi: 10.1002/adfm.201910510

  8. [8]

     Muldoon, J.; Bucur, C. B.; Oliver, A. G.; Sugimoto, T.; Matsui, M.; Kim, H. S.; Allred, G. D.; Zajicek, J.; Kotani, Y. Energy Environ. Sci. 2012, 5, 5941. doi: 10.1039/c2ee03029b

  9. [9]

     Attias, R.; Salama, M.; Hirsch, B.; Goffer, Y.; Aurbach, D. Joule 2019, 3, 27. doi: 10.1016/j.joule.2018.10.028

  10. [10]

      阳源源, 王进芝, 杜俊哲, 杜奥冰, 赵井文, 崔光磊. 化工学报, 2021, 72, 3116. doi: 10.11949/0438-1157.20210124Yang, Y. Y.; Wang, J. Z.; Du, J. Z.; Du, A. B.; Zhao, J. W.; Cui, G. L. CIESC J. 2021, 72, 3116. doi: 10.11949/0438-1157.20210124

  11. [11]

      Aurbach, D.; Lu, Z.; Schechter, A.; Gofer, Y.; Gizbar, H.; Turgeman, R.; Cohen, Y.; Moshkovich, M.; Levi, E. Nature 2000, 407, 724. doi: 10.1038/35037553

  12. [12]

      Zhang, R.; Yu, X.; Nam, K.-W.; Ling, C.; Arthur, T. S.; Song, W.; Knapp, A. M.; Ehrlich, S. N.; Yang, X.-Q.; Matsui, M. Electrochem. Commun. 2012, 23, 110. doi: 10.1016/j.elecom.2012.07.021

  13. [13]

      Pan, B.; Zhou, D.; Huang, J.; Zhang, L.; Burrell, A. K.; Vaughey, J. T.; Zhang, Z.; Liao, C. J. Electrochem. Soc. 2016, 163, A580. doi: 10.1149/2.0021605jes

  14. [14]

      Rong, Z.; Malik, R.; Canepa, P.; Sai Gautam, G.; Liu, M.; Jain, A.; Persson, K.; Ceder, G. Chem. Mater. 2015, 27, 6016. doi: 10.1021/acs.chemmater.5b02342

  15. [15]

      Yu, S. H.; Lee, S. H.; Lee, D. J.; Sung, Y. E.; Hyeon, T. Small 2016, 12, 2146. doi: 10.1002/smll.201502299

  16. [16]

      Wu, F.; Yushin, G. Energy Environ. Sci. 2017, 10, 435. doi: 10.1039/c6ee02326f

  17. [17]

      Arthur, T. S.; Zhang, R.; Ling, C.; Glans, P. A.; Fan, X.; Guo, J.; Mizuno, F. ACS Appl. Mater. Interfaces 2014, 6, 7004. doi: 10.1021/am5015327

  18. [18]

      Lu, D.; Liu, H.; Huang, T.; Xu, Z.; Ma, L.; Yang, P.; Qiang, P.; Zhang, F.; Wu, D. J. Mater. Chem. A 2018, 6, 17297. doi: 10.1039/c8ta05230a

  19. [19]

      Tran, N. A.; Do Van Thanh, N.; Le, M. L. P. Chem. -Eur. J. 2021, 27, 9198. doi: 10.1002/chem.202100223

  20. [20]

      Yoo, H. D.; Liang, Y.; Dong, H.; Lin, J.; Wang, H.; Liu, Y.; Ma, L.; Wu, T.; Li, Y.; Ru, Q.; et al. Nat. Commun. 2017, 8, 339. doi: 10.1038/s41467-017-00431-9

  21. [21]

      Kumar, G.; Sivashanmugam, A.; Muniyandi, N.; Dhawan, S. K.; Trivedi, D. C. Synth. Met. 1996, 80, 279. doi: 10.1016/0379-6779(96)80214-1

  22. [22]

      Kim, K. I.; Guo, Q.; Tang, L.; Zhu, L.; Pan, C.; Chang, C. H.; Razink, J.; Lerner, M. M.; Fang, C.; Ji, X. L. Angew. Chem. Int. Ed. Engl. 2020, 59, 19924. doi: 10.1002/anie.202009172

  23. [23]

      Levi, E.; Lancry, E.; Mitelman, A.; Aurbach, D.; Ceder, G.; Morgan, D.; Isnard, O. Chem. Mater. 2006, 18, 5492. doi: 10.1021/cm061656f

  24. [24]

      Yoo, H. D.; Shterenberg, I.; Gofer, Y.; Gershinsky, G.; Pour, N.; Aurbach, D. Energy Environ. Sci. 2013, 6, 2265. doi: 10.1039/c3ee40871j

  25. [25]

      Ryu, A.; Park, M.-S.; Cho, W.; Kim, J.-S.; Kim, Y.-J. Bull. Korean Chem. Soc. 2013, 34, 3033. doi: 10.5012/bkcs.2013.34.10.3033

  26. [26]

      Levi, E.; Gofer, Y.; Vestfreed, Y.; Lancry, E.; Aurbach, D. Chem. Mater. 2002, 14, 2767. doi: 10.1021/cm021122o

  27. [27]

      Choi, S. H.; Kim, J. S.; Woo, S. G.; Cho, W.; Choi, S. Y.; Choi, J.; Lee, K. T.; Park, M. S.; Kim, Y. J. ACS Appl. Mater. Interfaces 2015, 7, 7016. doi: 10.1021/am508702j

  28. [28]

      Tao, Z. L.; Xu, L. N.; Gou, X. L.; Chen, J.; Yuan, H. T. Chem. Commun. 2004, 2080. doi: 10.1039/b403855j

  29. [29]

      Liu, M.; Jain, A.; Rong, Z.; Qu, X.; Canepa, P.; Malik, R.; Ceder, G.; Persson, K. A. Energy Environ. Sci. 2016, 9, 3201. doi: 10.1039/c6ee01731b

  30. [30]

      Sun, X.; Bonnick, P.; Nazar, L. F. ACS Energy Lett. 2016, 1, 297. doi: 10.1021/acsenergylett.6b00145

  31. [31]

      Kolli, S. K.; Van der Ven, A. Chem. Mater. 2018, 30, 2436. doi: 10.1021/acs.chemmater.8b00552

  32. [32]

      Emly, A.; Van der Ven, A. Inorg. Chem. 2015, 54, 4394. doi: 10.1021/acs.inorgchem.5b00188

  33. [33]

      Sun, X.; Bonnick, P.; Duffort, V.; Liu, M.; Rong, Z.; Persson, K. A.; Ceder, G.; Nazar, L. F. Energy Environ. Sci. 2016, 9, 2273. doi: 10.1039/c6ee00724d

  34. [34]

      Ni, Q.; Bai, Y.; Wu, F.; Wu, C. Adv. Sci. 2017, 4, 1600275. doi: 10.1002/advs.201600275

  35. [35]

      Ling, C.; Banerjee, D.; Song, W.; Zhang, M.; Matsui, M. J. Mater. Chem. 2012, 22, 13517. doi: 10.1039/c2jm31122d

  36. [36]

      Li, Y.; Nuli, Y.; Yang, J.; Yilinuer, T.; Wang, J. Chin. Sci. Bull. 2011, 56, 386. doi: 10.1007/s11434-010-4247-4

  37. [37]

      Chen, X.; Bleken, F. L.; Løvvik, O. M.; Vullum-Bruer, F. J. Power Sources 2016, 321, 76. doi: 10.1016/j.jpowsour.2016.04.094

  38. [38]

      Orikasa, Y.; Masese, T.; Koyama, Y.; Mori, T.; Hattori, M.; Yamamoto, K.; Okado, T.; Huang, Z. D.; Minato, T.; Tassel, C.; et al. Sci. Rep. 2014, 4, 5622. doi: 10.1038/srep05622

  39. [39]

      NuLi, Y.; Yang, J.; Li, Y.; Wang, J. Chem. Commun. 2010, 46, 3794. doi: 10.1039/c002456b

  40. [40]

      Zeng, J.; Yang, Y.; Lai, S.; Huang, J.; Zhang, Y.; Wang, J.; Zhao, J. Chem. - Eur. J. 2017, 23, 16898. doi: 10.1002/chem.201704303

  41. [41]

      Makino, K.; Katayama, Y.; Miura, T.; Kishi, T. J. Power Sources 2001, 99, 66. doi: 10.1016/s0378-7753(01)00480-3

  42. [42]

      Makino, K.; Katayama, Y.; Miura, T.; Kishi, T. J. Power Sources 2001, 97–98, 512. doi: 10.1016/s0378-7753(01)00694-2

  43. [43]

      Makino, K.; Katayama, Y.; Miura, T.; Kishi, T. J. Power Sources 2002, 112, 85. doi: 10.1016/s0378-7753(02)00345-2

  44. [44]

      Huang, Z.-D.; Masese, T.; Orikasa, Y.; Mori, T.; Yamamoto, K. RSC Adv. 2015, 5, 8598. doi: 10.1039/c4ra14416c

  45. [45]

      Kitchaev, D. A.; Dacek, S. T.; Sun, W.; Ceder, G. J. Am. Chem. Soc. 2017, 139, 2672. doi: 10.1021/jacs.6b11301

  46. [46]

      Ling, C.; Zhang, R.; Arthur, T. S.; Mizuno, F. Chem. Mater. 2015, 27, 5799. doi: 10.1021/acs.chemmater.5b02488

  47. [47]

      Rasul, S.; Suzuki, S.; Yamaguchi, S.; Miyayama, M. Solid State Ionics 2012, 225, 542. doi: 10.1016/j.ssi.2012.01.019

  48. [48]

      Rasul, S.; Suzuki, S.; Yamaguchi, S.; Miyayama, M. Electrochim. Acta 2012, 82, 243. doi: 10.1016/j.electacta.2012.03.095

  49. [49]

      Feng, Z.; Chen, X.; Qiao, L.; Lipson, A. L.; Fister, T. T.; Zeng, L.; Kim, C.; Yi, T.; Sa, N.; Proffit, D. L.; et al. ACS Appl. Mater. Interfaces 2015, 7, 28438. doi: 10.1021/acsami.5b09346

  50. [50]

      Zhao, X.; Yang, Y.; NuLi, Y.; Li, D.; Wang, Y.; Xiang, X. Chem. Commun. 2019, 55, 6086. doi: 10.1039/c9cc02556a

  51. [51]

      Yang, Y.; Wang, W.; Nuli, Y.; Yang, J.; Wang, J. ACS Appl. Mater. Interfaces 2019, 11, 9062. doi: 10.1021/acsami.8b20180

  52. [52]

      Yuan, H.; Yang, Y.; NuLi, Y.; Yang, J.; Wang, J. J. Mater. Chem. A 2018, 6, 17075. doi: 10.1039/c8ta04772c

  53. [53]

      Du, A.; Zhao, Y.; Zhang, Z.; Dong, S.; Cui, Z.; Tang, K.; Lu, C.; Han, P.; Zhou, X.; Cui, G. Energy Storage Mater. 2020, 26, 23. doi: 10.1016/j.ensm.2019.12.030

  54. [54]

      Duffort, V.; Sun, X.; Nazar, L. F. Chem. Commun. 2016, 52, 12458. doi: 10.1039/c6cc05363g

  55. [55]

      Tashiro, Y.; Taniguchi, K.; Miyasaka, H. Electrochim. Acta 2016, 210, 655. doi: 10.1016/j.electacta.2016.05.202

  56. [56]

      Zhang, Z.; Chen, B.; Xu, H.; Cui, Z.; Dong, S.; Du, A.; Ma, J.; Wang, Q.; Zhou, X.; Cui, G. Adv. Funct. Mater. 2018, 28, 1701718. doi: 10.1002/adfm.201701718

  57. [57]

      Cheng, X.; Zhang, Z.; Kong, Q.; Zhang, Q.; Wang, T.; Dong, S.; Gu, L.; Wang, X.; Ma, J.; Han, P.; et al. Angew. Chem. Int. Ed. Engl. 2020, 59, 11477. doi: 10.1002/anie.202002177

  58. [58]

      Qu, X.; Du, A.; Wang, T.; Kong, Q.; Chen, G.; Zhang, Z.; Zhao, J.; Liu, X.; Zhou, X.; Dong, S.; et al. Angew. Chem. Int. Ed. Engl. 2022. doi: 10.1002/anie.202204423

  59. [59]

      Sano, H.; Senoh, H.; Yao, M.; Sakaebe, H.; Kiyobayashi, T. Chem. Lett. 2012, 41, 1594. doi: 10.1246/cl.2012.1594

  60. [60]

      Senoh, H.; Sakaebe, H.; Tokiwa, H.; Uchida, M.; Sano, H.; Yao, M.; Kiyobayashi, T. ECS Trans. 2015, 69, 33. doi: 10.1149/06919.0033ecst

  61. [61]

      Dong, H.; Tutusaus, O.; Liang, Y.; Zhang, Y.; Lebens-Higgins, Z.; Yang, W.; Mohtadi, R.; Yao, Y. Nat. Energy 2020, 5, 1043. doi: 10.1038/s41560-020-00734-0

  62. [62]

      Pan, B.; Huang, J.; Feng, Z.; Zeng, L.; He, M.; Zhang, L.; Vaughey, J. T.; Bedzyk, M. J.; Fenter, P.; Zhang, Z.; et al. Adv. Energy Mater. 2016, 6, 1600140. doi: 10.1002/aenm.201600140

  63. [63]

      Dong, H.; Liang, Y.; Tutusaus, O.; Mohtadi, R.; Zhang, Y.; Hao, F.; Yao, Y. Joule 2019, 3, 782. doi: 10.1016/j.joule.2018.11.022

  64. [64]

      Nakahara, K.; Iwasa, S.; Satoh, M.; Morioka, Y.; Iriyama, J.; Suguro, M.; Hasegawa, E. Chem. Phys. Lett. 2002, 359, 351. doi: 10.1016/s0009-2614(02)00705-4

  65. [65]

      陈强, 努丽燕娜, 郭维, 杨军, 王久林, 郭玉国. 物理化学学报, 2013, 29, 2295. doi: 10.3866/PKU.WHXB201309241Chen, Q.; Nuli, Y. N.; Guo, W.; Yang, J.; Wang, J. L.; Guo, Y. G. Acta Phys. -Chim. Sin. 2013, 29, 2295. doi: 10.3866/PKU.WHXB201309241

  66. [66]

      Gu, S.; Wu, S.; Cao, L.; Li, M.; Qin, N.; Zhu, J.; Wang, Z.; Li, Y.; Li, Z.; Chen, J.; et al. J. Am. Chem. Soc. 2019, 141, 9623. doi: 10.1021/jacs.9b03467

  67. [67]

      Ha, S. Y.; Lee, Y. W.; Woo, S. W.; Koo, B.; Kim, J. S.; Cho, J.; Lee, K. T.; Choi, N. S. ACS Appl. Mater. Interfaces 2014, 6, 4063. doi: 10.1021/am405619v

  68. [68]

      Wu, M.; Cui, Y.; Bhargav, A.; Losovyj, Y.; Siegel, A.; Agarwal, M.; Ma, Y.; Fu, Y. Angew. Chem. Int. Ed. Engl. 2016, 55, 10027. doi: 10.1002/anie.201603897

  69. [69]

      NuLi, Y.; Guo, Z.; Liu, H.; Yang, J. Electrochem. Commun. 2007, 9, 1913. doi: 10.1016/j.elecom.2007.05.009

  70. [70]

      NuLi, Y.; Chen, Q.; Wang, W.; Wang, Y.; Yang, J.; Wang, J. Sci. World J. 2014, 2014, 107918. doi: 10.1155/2014/107918

  71. [71]

      Bitenc, J.; Pirnat, K.; Mali, G.; Novosel, B.; Randon Vitanova, A.; Dominko, R. Electrochem. Commun. 2016, 69, 1. doi: 10.1016/j.elecom.2016.05.009

  72. [72]

      Kaland, H.; Hadler-Jacobsen, J.; Fagerli, F. H.; Wagner, N. P.; Schnell, S. K.; Wiik, K. ACS Appl. Energy Mater. 2020, 3, 10600. doi: 10.1021/acsaem.0c01655

•