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(a) Schematic illustration of rechargeable aprotic Li-O2 battery system. (b) Proposed mechanisms for Li2O2 growth in Li-O2 batteries. (c) In situ SERS during O2 reduction and re-oxidation on Au positive electrode. (d) Proposed solvent-controlled Li2O2 decomposition mechanism. (b) Reproduced with permission from Ref. [25], copyright 2016, Nature Publishing Group. (c) Reproduced with permission from Ref. [26], copyright 2011, Wiley-VCH. (d) Reproduced with permission from Ref. [34], copyright 2018, Elsevier.

(a) Schematic illustration of rechargeable aprotic Li-O2 battery system. (b) Proposed mechanisms for Li2O2 growth in Li-O2 batteries. (c) In situ SERS during O2 reduction and re-oxidation on Au positive electrode. (d) Proposed solvent-controlled Li2O2 decomposition mechanism. (b) Reproduced with permission from Ref. [25], copyright 2016, Nature Publishing Group. (c) Reproduced with permission from Ref. [26], copyright 2011, Wiley-VCH. (d) Reproduced with permission from Ref. [34], copyright 2018, Elsevier.

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Rechargeable aprotic lithium-oxygen (Li-O2) batteries have attracted significant interest in recent years owing to their ultrahigh theoretical capacity, low cost, and environmental friendliness. However, the further development of Li-O2 batteries is hindered by some ineluctable issues, such as severe parasitic reactions, low energy efficiency, poor...

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Context 1
... illustrated in Figure 1a, a rechargeable aprotic Li-O2 battery usually consists of a lithium metal negative electrode, aprotic electrolyte, a separator and a porous catalyzed positive electrode, where the following reversible electrochemical reactions occur [10]: ...
Context 2
... are two different growth modes of the discharge product Li2O2 [21]. As schematically shown in Figure 1b, in the first step, the solvated O2 molecule is reduced by one electron, forming a solvated O2 − intermediate. While divergence occurs in the second step, if the adsorption toward the intermediate is strong enough, the solvated O2 − intermediate can be adsorbed on the electrode surface, attracting a Li + to neutralize the negative charge, and being further reduced or undergoing a disproportionation on the electrode surface to form Li2O2 in the surface pathway. ...
Context 3
... with the help of in-situ surface-enhanced Raman spectroscopy (SERS), Bruce's group [26] directly detected the existence of LiO2 during the discharging progress. As shown in Figure 1c, in the very beginning period of discharging, peak with short lifetime arose at 1137 cm −1 which was associated with the O-O bond vibration in LiO2. Such a result directly proved the formation of unstable LiO2 discharge intermediate which underwent a quick disproportionation to form the final discharge product Li2O2. ...
Context 4
... on, Lu et al. [34] proposed that the oxidation mechanism of Li2O2 is closely related to the DN of electrolyte solvent. Through rotating ring-disk electrode (RRDE) and X-ray absorption near-edge structure, they confirmed the different OER mechanisms of Li-O2 batteries using different solvent varied in DN as described in Figure 1d. In a high DN solvent, the oxidation of Li2O2 followed a solution way with the formation of soluble LiO2 intermediate (e.g., dimethyl sulfoxide, 1-methylimidazole), while for the low DN solvent (e.g., acetonitrile (ACN), tetraethylene glycol dimethyl ether (TEGDME)), the oxidation of Li2O2 proceeded by way of solid delithiation, pretty similar to the behavior of the positive electrode in LIBs under charging. ...

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