The use of energy storage devices (e.g., among the most typical, batteries and supercapacitors (SCs)) are increasing in nowadays’ industry society. While the development of electrodes can not satisfy the growing desire for high energy/power density devices, electrolytes design (especially aqueous electrolytes) is gaining significant attention due to its low cost and simplicity in assembling cells. Starting from 2015, water-in-salt (WIS) electrolytes first and solvent-in-salt (SIS) and bi-solvent-in-salt (BSiS), etc., afterwards have been offering wide electrochemical stability windows (ESWs) and thermal stability. Nonetheless, some obstacles caused by a high concentration of salts limit its practical service in devices. This Thesis is devoted to study various combinations of new aqueous electrolytes not only in terms of selection and synthesis of salts and solvents but also interaction mechanisms. The so-called aqueous eutectic-in-salt (AEIS), bi-solvent in zwitterionic-based protic ionic liquids (BSin-ZPIL) and tri-solvent-in-salt (TSIS) have been exhaustively introduced in Chapter 2, 3, and 4, respectively. With regarding the aim of developing low cost and excellently functional electrolytes, efforts have been taken to demonstrate the formation and evolution of the different concentrated solvation species and electrochemically active hydrogen bond (HB) complex structures following by techniques (such as Raman and NMR spectroscopies, and MD simulations). Ultimately, this essay is dedicated to present the high attractiveness of designing new and low-cost aqueous electrolytes that offered an improved performance.
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