Abstract
Current lithium ion battery technology is tied in with conventional reaction mechanisms such as insertion, conversion, and alloying reactions even though most future applications like EVs demand much higher energy densities than current ones. Exploring the exceptional reaction mechanism and related electrode materials can be critical for pushing current battery technology to a next level. Here, we introduce an exceptional reaction with a Co(OH)2 material which exhibits an initial charge capacity of 1112 mAh g-1, about twice its theoretical value based on known conventional conversion reaction, and retains its first cycle capacity after 30 cycles. The combined results of synchrotron X-ray diffraction and X-ray absorption spectroscopy indicate that nanosized Co metal particles and LiOH are generated by conversion reaction at high voltages, and CoxHy, Li2O, and LiH are subsequently formed by hydride reaction between Co metal, LiOH, and other lithium species at low voltages, resulting in a anomalously high capacity beyond the theoretical capacity of Co(OH)2. This is further corroborated by AIMD simulations, localized STEM, and XPS. These findings will provide not only further understanding of exceptional lithium storage of recent nanostructured materials but also valuable guidance to develop advanced electrode materials with high energy density for next-generation batteries.
Original language | English |
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Pages (from-to) | 2909-2921 |
Number of pages | 13 |
Journal | ACS Nano |
Volume | 12 |
Issue number | 3 |
DOIs | |
State | Published - Mar 27 2018 |
Funding
This work was supported by Samsung Research Funding & Incubation Center of Samsung Electronics under Project Number MA1401-52. Preliminary XAS studies at sector-20 BM and sector-12 BM in Argonne’s Advanced Photon Source are gratefully acknowledged. We thank Dr. Sungsik Lee for support at 12 BM. M.B. is supported by the U.S. DOE, Office of Science (Contract No. DE-AC02-06CH11357). This work was supported by Samsung Research Funding & Incubation Center of Samsung Electronics under Project Number MA1401-52. Preliminary XAS studies at sector-20 BM and sector-12 BM in Argonne's Advanced Photon Source are gratefully acknowledged. We thank Dr. Sungsik Lee for support at 12 BM. M.B. is supported by the U.S. DOE, Office of Science (Contract No. DE-AC02-06CH11357).