Electrochemical stability and interfacial reactions are crucial for rechargeable aqueous zinc batteries. Electrolyte engineering with low-cost aqueous electrolytes is highly required to stabilize their interfacial reactions. Herein, we propose a design strategy using glutamic additive and its derivatives with modification of hydrogen-bonding network to enable Zn aqueous battery at a low concentration (2 m ZnSO 4 + 1 m Li 2 SO 4 ). Computational, in situ/ex situ spectroscopic, and electrochemical studies suggest that additives with moderate interactions, such as 0.1 mol % glutamic additive (G1), preferentially absorb on the Zn surface to homogenize Zn 2+ plating and favorably interact with Zn 2+ in bulk to weaken the interaction between H 2 O and Zn 2+ . As a result, uniform deposition and stable electrochemical performance are realized. The Zn||Cu half-cell lasts for more than 200 cycles with an average Coulombic efficiency (CE) of >99.32% and the Zn||Zn symmetrical cells for 1400 h with a low and stable overpotential under a current density of 0.5 mA cm −2 , which is better than the reported results. Moreover, adding 0.1 mol % G1 to the Zn||LFP full cell improves its electrochemical performance with stable cycling and achieves a remarkable capacity of 147.25 mAh g −1 with a CE of 99.79% after 200 cycles.
Anode-free lithium–sulfur batteries (AFLSBs) show a surprisingly prolonged cycle life 2-fold higher than anode-free lithium metal batteries. The principal difference is the presence of an intrinsic polysulfide (PS) shuttle between electrodes in AFLSBs. However, the underlying mechanism for the impact of PS redox species on the electrochemical performance of AFLSBs is not clearly understood. Herein, we investigate the role of PS redox species in retrieving inactive lithium for compensating lithium inventory loss using titration gas chromatography, thereby quantifying inactive lithium accumulated after several cycles. Moreover, XPS analysis reveals reduced lithium sulfide (Li2S/Li2S2) species formed through PS redox shuttle refresh inactive solid electrolyte interface (SEI) composition and stabilize the consecutive cycle lithium deposition. Interestingly, synchrotron-based operando transmission X-ray microscopy (TXM) reveals dense and granular electrodeposited lithium morphologies in AFLSBs. Therefore, the interplay between reviving inactive lithium for compensating lithium inventory loss and stabilizing lithium electrodeposition endows high electrochemical performance in AFLSBs.
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