Waste Coffee Grounds-Derived Micropores Carbon Framework as an Efficient Iodine Host for Zinc Iodine Battery

Abstract

Aqueous zinc-iodine batteries (AZIBs) have attracted significant attention as the most promising next-generation energy storage technology due to their low cost, inherent safety, and high energy density. However, their practical application is hindered by the poor electronic conductivity of iodine cathodes and the severe shuttling effect of intermediate polyiodides. Here, we report a novel micropores carbon framework (MCF) synthesized from waste coffee grounds via a facile carbonization-activation process. The resultant MCF features an ultrahigh specific surface area and a high density of micropores, which not only physically confine iodine species to minimize iodine loss but also enhance the electronic conductivity of the composite cathode. Furthermore, biomass-derived heteroatom dopings (nitrogen functionalities) facilitate effective chemical anchoring of polyiodide intermediates, thereby mitigating the shuttle effect. UV–visible spectroscopy and electrochemical kinetic analyses further confirm the rapid transformation and inhibition mechanism of iodine species by MCF. Consequently, the MCF/I₂ cathode delivers superior specific capacities of 238.3 mA h g^–1 at 0.2 A g^–1 and maintains outstanding cycling performance with a capacity retention of 85.2% after 1200 cycles at 1.0 A g^–1. This work not only provides an important reference for the design of high-performance iodine-host porous carbon materials but also explores new paths for the sustainable, high-value utilization of waste biomass resources.

Keywords

iodine host / micropores carbon framework / polyiodide shuttle inhibition / waste coffee grounds / zinc iodine batteries

References

[1] L. Q. Zhang, H. L. Guo, W. Zong, Y. P. Huang, J. J. Huang, G. J. He, T. X. Liu, J. Hofkens, F. L. Lai, Energy Environ. Sci. 2023, 16, 4872.

[2] Y. Wang, L. F. Zhu, J. X. Wang, Z. Zhang, J. Yu, Z. Y. Yang, Chem. Eng. J. 2022, 433, 133792.

[3] J. Xu, Y. Qiu, J. Yang, H. Li, P. Han, Y. Jin, H. Liu, B. Sun, G. Wang, Adv. Funct. Mater. 2023, 34, 2306206.

[4] Z. Lv, H. Xu, W. Xu, B. Peng, C. Zhao, M. Xie, X. Lv, Y. Gao, K. Hu, Y. Fang, W. Dong, F. Huang, Adv. Energy Mater. 2023, 13, 2300790.

[5] H. Xu, Chem. Phys. Lett. 2024, 851, 141492.

[6] W. Xiao, K. Yoo, J. Kim, H. Xu, ACS Nano 2024, 18, 32732.

[7] L. Zhu, X. Guan, Z. Zhang, Z. Yuan, C. Zhang, Y. Wang, R. Xue, E. L. H. Mayes, Z. Yong, H. Xu, X. Li, H. Li, B. Jia, H. Yu, T. Ma, Y. Sun, Small 2025, 21, 2500223.

[8] W. Yan, Y. Liu, J. Qiu, F. Tan, J. Liang, X. Cai, C. Dai, J. Zhao, Z. Lin, Nat. Commun. 2024, 15, 9702.

[9] S.-J. Zhang, J. Hao, H. Wu, C.-C. Kao, Q. Chen, C. Ye, S.-Z. Qiao, ACS Nano 2024, 18, 28557.

[10] H. Xu, W. Yang, M. Li, H. Liu, S. Gong, F. Zhao, C. Li, J. Qi, H. Wang, W. Peng, J. Liu, Small 2024, 20, 2310972.

[11] Y. Su, X. Wang, M. Zhang, H. Guo, H. Sun, G. Huang, D. Liu, G. Zhu, Angew. Chem. Int. Ed. 2023, 62, e202308182.

[12] H. Ren, S. Li, B. Wang, Y. Zhang, T. Wang, Q. Lv, X. Zhang, L. Wang, X. Han, F. Jin, C. Bao, P. Yan, N. Zhang, D. Wang, T. Cheng, H. Liu, S. Dou, Adv. Mater. 2023, 35, e2208237.

[13] L. Zhu, Y. Qu, X. Huang, J. Luo, H. Zhang, Z. Zhang, Z. Yang, Chem. Commun. 2020, 56, 13201.

[14] L. Chai, X. Wang, Y. Hu, X. Li, S. Huang, J. Pan, J. Qian, X. Sun, Adv. Sci. 2022, 9, e2105063.

[15] J. Xu, J. Wang, L. Ge, J. Sun, W. Ma, M. Ren, X. Cai, W. Liu, J. Yao, J. Colloid Interface Sci. 2022, 610, 98.

[16] T. T. Liu, H. J. Wang, C. J. Lei, Y. Mao, H. Q. Wang, X. He, X. Liang, Energy Stor. Mater. 2022, 53, 544.

[17] S. Niu, B. Zhao, D. Liu, ACS Appl. Mater. Interfaces 2023, 15, 25558.

[18] P. F. Zhang, J. H. Li, S. J. Zhang, D. C. Li, S. Y. Zeng, S. L. Xu, Q. X. Yao, L. Y. Liu, L. Ding, H. X. Li, Y. Y. Hu, J. T. Li, Y. Zhou, Adv. Funct. Mater. 2024, 34, 2306359.

[19] W. Feng, Y. Wang, F. Tian, Z. Liu, X. Wei, C. Ma, G. Ma, Z. Li, D. Kong, L. Zhi, Energy Storage Mater. 2024, 73, 103812.

[20] L. F. Zhu, Y. Wang, M. J. Wang, Y. P. Xiong, Z. Zhang, J. Yu, Y. H. Qu, J. X. Cai, Z. Y. Yang, Carbon 2021, 184, 706.

[21] Y. Sun, X. L. Shi, Y. L. Yang, G. Q. Suo, L. Zhang, S. Y. Lu, Z. G. Chen, Adv. Funct. Mater. 2022, 32, 2201584.

[22] J. Kim, J. Park, J. Lee, W. G. Lim, C. Jo, J. Lee, Adv. Funct. Mater. 2021, 31, 2010882.

[23] N. Pianta, D. A. Florenzano, R. Lorenzi, L. Navarini, C. Santoro, R. Ruffo, Adv. Sustain. Syst. 2025,

[24] A. Forcina, A. Petrillo, M. Travaglioni, S. di Chiara, F. De Felice, J. Clean. Prod. 2023, 385, 135727.

[25] K. T. Lee, Y. T. Shih, S. Rajendran, Y. K. Park, W. H. Chen, Environ. Pollut. 2023, 324, 121330.

[26] P. H. Chiang, S. F. Liu, Y. H. Hung, H. Tseng, C. H. Guo, H. Y. Chen, Energy Fuel 2020, 34, 7666.

[27] L. F. Zhu, Z. Zhang, H. Zhang, Y. Wang, J. D. Luo, J. Yu, Y. H. Qu, Z. Y. Yang, Sci. China Technol. Sci. 2021, 64, 2047.

[28] H. Liu, X. X. Liu, W. Li, X. Guo, Y. Wang, G. X. Wang, D. Y. Zhao, Adv. Energy Mater. 2017, 7, 1700283.

[29] H. Wang, X. Li, Z. Cui, Z. Fu, L. Yang, G. Liu, M. Li, J. Colloid Interface Sci. 2020, 578, 491.

[30] T. Qi, S. Liu, L. Sun, X. Feng, B. Zhao, S. An, L. Xing, Q. Jing, H. Jiang, Q. Li, L. Wang, Sep. Purif. Technol. 2025, 364, 132585.

[31] M. Yu, M. Sun, L. Zhu, Z. Luo, G. Deng, C. Zou, F. Zeng, Y. Qu, M. Guo, K. Xu, C. Yuan, Z.-H. Lu, J. Energy Storage 2024, 86, 111211.

[32] L. Zhu, X. Guan, Z. Zhang, Y. Fu, Z. Yuan, C. Zhang, Y. Wang, H. Fan, H. Xu, X. Li, H. Li, B. Jia, H. Yu, Y. Sun, T. Ma, Chem. Commun. 2025, 61, 961.

[33] G. R. Li, W. Lei, D. Luo, Y. P. Deng, D. L. Wang, Z. W. Chen, Adv. Energy Mater. 2018, 8, 1702381.

[34] M. E. Lee, H. W. Kwak, H. J. Jin, Y. S. Yun, ACS Sustain. Chem. Eng. 2019, 7, 12734.

[35] L. S. Wei, X. Zhang, X. Li, C. X. Chen, D. F. Yu, G. Y. Zhao, J. Electroanal. Chem. 2024, 967, 118452.

[36] L. F. Zhu, Z. Zhang, J. D. Luo, H. Zhang, Y. H. Qu, Z. Y. Yang, Carbon 2021, 174, 317.

[37] L. Zhu, X. Guan, Y. Fu, Z. Zhang, Y. Li, Q. Mai, C. Zhang, Z. Yuan, Y. Wang, P. Li, H. Li, D. Su, B. Jia, H. Yu, Y. Sun, T. Ma, Adv. Funct. Mater. 2024, 34, 2409099.

[38] Z. Quan, F. Wang, Y. Wang, Z. Liu, C. Zhang, F. Qi, M. Zhang, C. Ye, J. Tan, J. Liu, Small 2024, 20, e2305841.

[39] Y. Wang, Y. W. Liu, Z. Xuan, L. F. Zhu, Z. L. Yuan, J. Y. Xu, C. T. Li, Y. F. Sun, Int. J. Hydrog. Energy 2024, 58, 678.

[40] L. Zhu, Y. Wang, M. Wang, M. Huang, Y. Huang, Z. Zhang, J. Yu, Y. Qu, C. Li, Z. Yang, Carbon 2022, 187, 302.

[41] G. X. Lin, R. G. Ma, Y. Zhou, Q. Liu, X. P. Dong, J. C. Wang, Electrochim. Acta 2018, 261, 49.

[42] Y. Zhang, X. Zhang, X. Li, C. Chen, D. Yu, G. Zhao, J. Alloys Compd. 2024, 976, 173041.

[43] Y. D. Wang, X. Zhang, X. Li, Y. R. Jiang, T. X. Shen, J. S. Peng, C. X. Chen, D. F. Yu, G. Y. Zhao, Diam. Relat. Mater. 2024, 150, 111685.

[44] Y. Zhu, A. Wei, H. Shi, H. Hu, K. Tang, N. Li, J. Zou, J. Environ. Chem. Eng. 2024, 12, 113132.

[45] Y. Wen, X. Wang, J. Huang, Y. Li, T. Li, B. Ren, Carbon Lett. 2023, 33, 1265.

[46] L. Yan, S. Zhang, Q. Kang, X. Meng, Z. Li, T. Liu, T. Ma, Z. Lin, Energy Storage Mater. 2023, 54, 339.

[47] L. Zhou, N. Wang, Y. Chang, S. Zhu, Y. Zhang, W. Hou, Y. Zhao, G. Han, J. Energy Storage 2024, 88, 111538.

[48] Y. Hou, F. Kong, Z. Wang, M. Ren, C. Qiao, W. Liu, J. Yao, C. Zhang, H. Zhao, J. Colloid Interface Sci. 2023, 629, 279.

[49] B. Tang, Y. Wei, R. Jia, F. Zhang, Y. Tang, Small 2024, 20, 2308126.

[50] Y. Feng, G. Wang, J. Ju, Y. Zhao, W. Kang, N. Deng, B. Cheng, Energy Storage Mater. 2020, 32, 320.

[51] L. Ma, G. Zhu, Z. Wang, A. Zhu, K. Wu, B. Peng, J. Xu, D. Wang, Z. Jin, Nano Lett. 2023, 23, 5272.

[52] X. Yang, H. Fan, F. Hu, S. Chen, K. Yan, L. Ma, Nano-Micro Lett. 2023, 15, 126.

[53] Z. Gong, C. Song, C. Bai, X. Zhao, Z. Luo, G. Qi, X. Liu, C. Wang, Y. Duan, Z. Yuan, Sci. China Mater. 2023, 66, 556.

[54] M. Li, Y. Ding, S. Zhang, M. Liu, J. Li, Y. Sun, L. Zhu, H. Li, Z. G. Yu, Y.-W. Zhang, H. Pan, B. Yin, T. Ma, Angew. Chem. Int. Ed. 2024, 63, e202412735.

[55] S. Hong, Q. Li, J. Li, L. Jin, L. Zhu, X. Meng, Y. Che, Z. Yang, Z. Zhang, J. Yu, J. Cai, ACS Appl. Mater. Interfaces 2024, 16, 35063.

[56] Y. P. Xiong, K. Wu, S. Y. Hong, L. Q. Jin, Z. Zhang, L. F. Zhu, M. Z. Huang, Z. Y. Yang, J. X. Cai, J. Mater. Sci. Mater. Electron. 2022, 33, 14121.

RIGHTS & PERMISSIONS

2025 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.