Extra storage capacity in transition metal oxide lithium-ion batteries revealed by in situ magnetometry

Li, Qiang; Li, Hongsen; Xia, Qingtao; Hu, Zhengqiang; Zhu, Yue; Shen, Yan; Chen, Ge; Zhang, Qinghua; Wang, Xiaoxiong; Shang, Xiantao; Fan, Shuting; Long, Yun-Ze; Gu, Lin; Miao, Guo‐Xing; Yu, Guihua; Moodera, Jagadeesh S.

doi:10.1038/s41563-020-0756-y

Cited by 454 publications

(309 citation statements)

References 35 publications

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“…[ 14–16 ] Just recently, we demonstrated that the surface capacitance on metal nanoparticles involving spin‐polarized electrons is the dominant source of the extra capacity in Fe 3 O 4 LIBs. [ 17–19 ] Therefore, the possible contribution of polymeric/gel films to the unusual capacity in CoO deserves to be revisited and clarified in more details, which can foster innovations in modern battery technologies based on this new storage mechanism.…”

Section: Figurementioning

confidence: 99%

Operando Magnetometry Probing the Charge Storage Mechanism of CoO Lithium‐Ion Batteries

Xia

et al. 2021

Advanced Materials

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reactions), indicating the existence of undiscovered extra charge reservoirs inside the system. [6-9] To shed light on this surprising behavior, Tarascon and co-workers proposed that it is the reversible formation/dissolution of polymeric films around the reduced Co nanoparticles that leads to the unusually large capacity, [10,11] which has been widely accepted. [6,7,12] However, using in situ X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses, Kim et al. demonstrated that the electrolyte decomposition cannot make major contributions to the extra capacity in RuO 2 LIBs. [13] In addition, Maier and co-workers presented an interfacial charge storage mechanism between Li salts and transition-metal nanocrystals. [14-16] Just recently, we demonstrated that the surface capacitance on metal nanoparticles involving spin-polarized electrons is the dominant source of the extra capacity in Fe 3 O 4 LIBs. [17-19] Therefore, the possible contribution of polymeric/gel films to the unusual capacity in CoO deserves to be revisited and clarified in more details, which can foster innovations in modern battery technologies based on this new storage mechanism.

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Section: Figurementioning

confidence: 99%

Operando Magnetometry Probing the Charge Storage Mechanism of CoO Lithium‐Ion Batteries

Xia

et al. 2021

Advanced Materials

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“…Table 3 lists a comparison of the details of capacities, Coulombic efficiencies and retention rates of all the investigated thin-film electrodes (pure references and composites). The charge capacity achieved in all the cases are higher than the theoretical capacity, which is due to the extremely thin films of active materials achieved by ALD (Mattelaer et al, 2015;Kint et al, 2019;Zhao et al, 2019;Li et al, 2020). The composite thin-films (SnO 2 -TiO 2 , SnO 2 -Fe 2 O 3 and SnO 2 -ZnO) show better electrochemical properties, either higher capacity or better retention rate than their individual counter parts (SnO 2 and TiO 2 , Fe 2 O 3 or ZnO).…”

Section: Synergistic Effect Between Sno 2 and Znomentioning

confidence: 83%

Atomic Layer Deposition of SnO2-Based Composite Anodes for Thin-Film Lithium-Ion Batteries

et al. 2020

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Transition metal oxides are promising anode materials for lithium-ion batteries thanks to their good electrochemical reversibility, high theoretical capacities, high abundance, and low cost. The mechanism of lithium insertion or deintercalation into or from these metal oxides can be different depending upon their lattice structure or chemical nature. Synergistic effects obtained from mixing different metal oxides with (dis)similar lithiation/delithiation mechanisms (intercalation, conversion and alloying) can significantly improve the device performances. In this research, we systematically investigate the impact on electrochemical properties of SnO2 thin-films upon mixing with TiO2, Fe2O3 and ZnO. In these pure thin-films, SnO2 displays conversion- as well as alloying-type lithiation and serves as the host material, whereas TiO2 represents an intercalation-type anode material, Fe2O3 exhibits conversion reactions and ZnO expresses alloying during lithiation-delithiation processes. Importantly, all the composite thin-films have an intermixed structure at the atomic scale, as they are precisely prepared by the atomic layer deposition method. The electrochemical properties demonstrate that the composite thin-films show better performance, either higher capacities or better cycling retentions, than the individual constituent material (SnO2, TiO2, Fe2O3 or ZnO). Overall cycling stability improves to a great extent along with a slight increase in capacity with the addition of TiO2. The supplement of Fe2O3 in the SnO2–Fe2O3 composite thin-films moderately improves both capacity and retention, while the SnO2–ZnO composite electrodes demonstrate a good cyclability and stabilize at a relatively high capacity. The systematic investigation of synergistic effects on the different types (intercalation, conversion and alloying) of metal oxide composites is expected to provide guidance towards the development of composite anode materials for lithium-ion batteries.

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“…The discharge capacities of the fourth and fifth cycles were about 610 mAh g −1 and 580 mAh g −1 , which are also higher than the theoretical capability 560 mAh g −1 of CuS. This extra capacity has been widely observed transition metal compounds [ 56 ], which can be attributed to the formation/decomposition of polymeric gel-like films around the transition metal particles [ 57 ], the interface lithium storage [ 58 , 59 ], and the surface conversion of LiOH to Li2O and LiH [ 60 ]. In the following cycles, the curves tended to overlap, which showed the outstanding cyclic stability of the CuS/Cu 1.8 S nanocomposites.…”

Section: Resultsmentioning

confidence: 99%

One-Pot Synthesis and High Electrochemical Performance of CuS/Cu1.8S Nanocomposites as Anodes for Lithium-Ion Batteries

et al. 2020

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CuS and Cu1.8S have been investigated respectively as anodes of lithium-ion batteries because of their abundant resources, no environment pollution, good electrical conductivity, and a stable discharge voltage plateau. In this work, CuS/Cu1.8S nanocomposites were firstly prepared simultaneously by the one-pot synthesis method at a relatively higher reaction temperature 200 °C. The CuS/Cu1.8S nanocomposites anodes exhibited a high initial discharge capacity, an excellent reversible rate capability, and remarkable cycle stability at a high current density, which could be due to the nano-size of the CuS/Cu1.8S nanocomposites and the assistance of Cu1.8S. The high electrochemical performance of the CuS/Cu1.8S nanocomposites indicated that the CuxS nanomaterials will be a potential lithium-ion battery anode.

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Extra storage capacity in transition metal oxide lithium-ion batteries revealed by in situ magnetometry

Cited by 454 publications

References 35 publications

Operando Magnetometry Probing the Charge Storage Mechanism of CoO Lithium‐Ion Batteries

Operando Magnetometry Probing the Charge Storage Mechanism of CoO Lithium‐Ion Batteries

Atomic Layer Deposition of SnO2-Based Composite Anodes for Thin-Film Lithium-Ion Batteries

One-Pot Synthesis and High Electrochemical Performance of CuS/Cu1.8S Nanocomposites as Anodes for Lithium-Ion Batteries

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