Developing Beyond Lithium Ion Batteries for Electrical Energy Storage



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To meet surging demands for sustainable energy and clean environment, one critical requirement is to develop safe and low-cost rechargeable batteries for electric transportation and grid energy storage. Lithium ion batteries (LIBs) are the dominant battery technology for portable electronics. However, the limited lithium resources on the Earth as well as safety issues of flammable electrolyte are causing serious concerns for large-scale energy storage. The objective of this dissertation is to develop beyond lithium ion batteries for building cheaper and safer next-generation energy storage technologies. At the foundation of these novel batteries are innovative strategies to control the movement of ions, electrons, and redox reactions. In this dissertation, I report four types of beyond lithium ion batteries, including sodium ion batteries (NIBs), magnesium rechargeable batteries (MRBs), hybrid ion batteries, and magnesium-air batteries. I first demonstrate an interlayer expansion approach to overcome the large Na+ ion size to significantly enhance the diffusivity of Na+. Theory, synthesis, electrochemical measurements, and kinetic analysis are combined to double the Na+ storage capacity in the expanded MoS2, which boost the Na+ conductivity by two orders of magnitude. My second strategy is to control the oxygen vacancy in the electrode host structure to optimize the electronic conductivity. When 3% oxygen vacancy is introduced to MoO3, the electrode exhibits a significant increase in capacity and enhanced cycling stability. The third strategy is to construct a hybrid-ion battery utilizing a mixed Li-Mg-ion or Na-Mg-ion electrolyte, which reveals excellent power performance. Finally, I show a stable mixed-phase mullite electrocatalyst as an efficient substitute for Pt/C in pH-neutral oxygen reduction reaction. Magnesium-air batteries are demonstrated to power a red light-emitting diode. The work described in this dissertation will provide exciting opportunities for future materials development of beyond lithium ion batteries for electrical energy storage.



Lithium-ion batteries (LIB), Batteries, Energy storage


Portions of this document appear in: Li, Yifei, Xiaoxue Zhang, Hao-Bo Li, Hyun Deog Yoo, Xiaowei Chi, Qinyou An, Jieyu Liu, Meng Yu, Weichao Wang, and Yan Yao. "Mixed-phase mullite electrocatalyst for pH-neutral oxygen reduction in magnesium-air batteries." Nano Energy 27 (2016): 8-16. And in: Li, Yifei, Dandan Wang, Qinyou An, Bush Ren, Yaoguang Rong, and Yan Yao. "Flexible electrode for long-life rechargeable sodium-ion batteries: effect of oxygen vacancy in MoO 3− x." Journal of Materials Chemistry A 4, no. 15 (2016): 5402-5405. And in: Li, Yifei, Yanliang Liang, Francisco C. Robles Hernandez, Hyun Deog Yoo, Qinyou An, and Yan Yao. "Enhancing sodium-ion battery performance with interlayer-expanded MoS2–PEO nanocomposites." Nano Energy 15 (2015): 453-461. And in: Dong, Hui, Yifei Li, Yanliang Liang, Guosheng Li, Cheng-Jun Sun, Yang Ren, Yuhao Lu, and Yan Yao. "A magnesium–sodium hybrid battery with high operating voltage." Chemical Communications 52, no. 53 (2016): 8263-8266. And in: Yoo, Hyun Deog, Yifei Li, Yanliang Liang, Yucheng Lan, Feng Wang, and Yan Yao. "Intercalation pseudocapacitance of exfoliated molybdenum disulfide for ultrafast energy storage." ChemNanoMat 2, no. 7 (2016): 688-691. And in: An, Qinyou, Yifei Li, Hyun Deog Yoo, Shuo Chen, Qiang Ru, Liqiang Mai, and Yan Yao. "Graphene decorated vanadium oxide nanowire aerogel for long-cycle-life magnesium battery cathodes." Nano Energy 18 (2015): 265-272. And in: Fan, Jingjing, Yifei Li, Hang N. Nguyen, Yan Yao, and Debora F. Rodrigues. "Toxicity of exfoliated-MoS 2 and annealed exfoliated-MoS 2 towards planktonic cells, biofilms, and mammalian cells in the presence of electron donor." Environmental Science: Nano 2, no. 4 (2015): 370-379. And in: Liang, Yanliang, Hyun Deog Yoo, Yifei Li, Jing Shuai, Hector A. Calderon, Francisco Carlos Robles Hernandez, Lars C. Grabow, and Yan Yao. "Interlayer-expanded molybdenum disulfide nanocomposites for electrochemical magnesium storage." Nano letters 15, no. 3 (2015): 2194-2202. And in: Yoo, Hyun Deog, Yanliang Liang, Yifei Li, and Yan Yao. "High areal capacity hybrid magnesium–lithium-ion battery with 99.9% coulombic efficiency for large-scale energy storage." ACS applied materials & interfaces 7, no. 12 (2015): 7001-7007. And in: Zeng, Jianbo, Fusheng Zhao, Ji Qi, Yifei Li, Chien-Hung Li, Yan Yao, T. Randall Lee, and Wei-Chuan Shih. "Internal and external morphology-dependent plasmonic resonance in monolithic nanoporous gold nanoparticles." Rsc Advances 4, no. 69 (2014): 36682-36688. And in: Shuai, Jing, Hyun Deog Yoo, Yanliang Liang, Yifei Li, Yan Yao, and Lars C. Grabow. "Density functional theory study of Li, Na, and Mg intercalation and diffusion in MoS2 with controlled interlayer spacing." Materials Research Express 3, no. 6 (2016): 064001.