期刊
NANO LETTERS
卷 15, 期 9, 页码 5755-5763出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.5b01709
关键词
Sodiation; kinetics; nickel oxides; reaction pathways; conversion electrodes; in situ TEM
类别
资金
- U.S. DOE Office of Science Facility, at Brookhaven National Laboratory [DE-SC0012704]
- Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. DOE under the Batteries for Advanced Transportation Technologies (BATT) Program [AC02-05CH11231]
- U.S. DOE [DE-AC02-76SF00515]
- U.S. DOE
- Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies [DE-SC00112704]
- Minta Martin award at the University of Maryland
- National Science Foundation [TG-DMR130142]
- University of Maryland
The development of sodium ion batteries (NIBs) can provide an alternative to lithium ion batteries (LIBs) for sustainable, low-cost energy storage. However, due to the larger size and higher m/e ratio of the sodium ion compared to lithium, sodiation reactions of candidate electrodes are expected to differ in significant ways from the corresponding lithium ones. In this work, we investigated the sodiation mechanism of a typical transition metal-oxide, NiO, through a set of correlated techniques, including electrochemical and synchrotron studies, real-time electron microscopy observation, and ab initio molecular dynamics (MD) simulations. We found that a crystalline Na2O reaction layer that was formed at the beginning of sodiation plays an important role in blocking the further transport of sodium ions. In addition, sodiation in NiO exhibits a shrinking-core mode that results from a layer-by-layer reaction, as identified by ab initio MD simulations. For lithiation, however, the formation of Li antisite defects significantly distorts the local NiO lattice that facilitates Li insertion, thus enhancing the overall reaction rate. These observations delineate the mechanistic difference between sodiation and lithiation in metal-oxide conversion materials. More importantly, our findings identify the importance of understanding the role of reaction layers on the functioning of electrodes and thus provide critical insights into further optimizing NIB materials through surface engineering.
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