Zn-metal batteries (ZnBs) are safe and sustainable because of their operability in aqueous electrolytes, abundance of Zn, and recyclability. However, the thermodynamic instability of Zn metal in aqueous electrolytes is a major bottleneck for its commercialization. As such, Zn deposition (Zn2+ & RARR; Zn(s)) is continuously accompanied by the hydrogen evolution reaction (HER) (2H(+) & RARR; H-2) and dendritic growth that further accentuate the HER. Consequently, the local pH around the Zn electrode increases and promotes the formation of inactive and/or poorly conductive Zn passivation species (Zn + 2H(2)O & RARR; Zn(OH)(2) + H-2) on the Zn. This aggravates the consumption of Zn and electrolyte and degrades the performance of ZnB. To propel HER beyond its thermodynamic potential (0 V vs standard hydrogen electrode (SHE) at pH 0), the concept of water-in-salt-electrolyte (WISE) has been employed in ZnBs. Since the publication of the first article on WISE for ZnB in 2016, this research area has progressed continuously. Here, an overview and discussion on this promising research direction for accelerating the maturity of ZnBs is provided. The review briefly describes the current issues with conventional aqueous electrolyte in ZnBs, including a historic overview and basic understanding of WISE. Furthermore, the application scenarios of WISE in ZnBs are detailed, with the description of various key mechanisms (e.g., side reactions, Zn electrodeposition, anions or cations intercalation in metal oxide or graphite, and ion transport at low temperature).

“Water-in-polymer salt” electrolytes (WiPSEs) based on potassium polyacrylate (PAAK) belong to a new family of “water-in-salt” electrolytes that is envisioned as a potential solution for large-scale supercapacitors to balance the electric grid at short time scales. The WiPSEs display a broad electrochemical stability window up to 3 V, yet they are nonflammable and provide high ionic conductivity (100 mS/cm) as required in high-power devices. However, the transport of matter in PAAK-based WiPSEs has not been studied. In this work, we have extensively characterized PAAK by spectroscopic methods such as Raman spectroscopy and NMR diffusometry to determine the state of water and elucidate the mechanism of ionic transport as well as its interplay with water and polymer chain dynamics, which reveals that a significant proportion of the transport in WiPSEs is attributed to hydrated cations. The results are further supported by molecular dynamics (MD) simulations. Finally, the potential of WiPSEs based on PAAK is demonstrated in an activated carbon-based supercapacitor operating up to 2 V with reasonable self-discharge. This proof of concept shows promise for low-cost and large-scale supercapacitors.

Zn-ion batteries are one of the hot candidates for low-cost and sustainable secondary batteries. The hydrogen evolution and dendritic growth upon zinc deposition are todays challenges for that technology. One of the new strategies to cope with these issues is to use "water-in-salt" electrolyte (WISE), that is, super concentrated aqueous electrolytes, to broaden its electrochemical stability window (ESW), suppressing hydrogen evolution reaction (HER), and perturbing the dendritic growth. Herein, this work proposes to use "water-in-polymer salt" electrolyte (WIPSE) concept to mitigate the challenges with Zn ion batteries and bring this technology toward one of the cheapest, greenest, and most sustainable electrodes: Lignin-carbon (L-C) electrode. Potassium polyacrylate (PAAK) as WISE bears out as better electrolyte for L-C electrodes in terms of self-discharge, cyclic stability, and specific capacity compared to conventional electrolyte based on chemically cousin molecule potassium acetate. Zinc bis(trifluoromethanesulfonyl) imide (Zn(TFSI)(2)) added into WIPSE shows deposition and dissolution of Zn in Zn//Zn symmetric cell suggesting that Zn2+ are moving into the polyanionic network. Furthermore, the added bis (trifluor omethanesul fonyl) imide (TFSI-) metal salts trigger a approximate to 40% enhancement of the capacity of L-C electrode. These results show a new promising direction toward the development of cost-effective and sustainable Zn-lignin batteries.

Lignin, the most abundant biopolymer on earth, has been explored as an electroactive material in battery applications. One essential feature for such lignin-based batteries to reach successful usage and implementation, e.g., large-scale stationary grid applications, is to have slow self-discharge characteristics on top of the essential safety and life-cycle properties. Water-in-polymer salt electrolytes (WIPSEs) have been demonstrated as an attractive route to solve this issue; however, little has been done to understand the fundamentals of actual self-discharge mechanisms. Herein, the impact of some critical chemical and physical parameters (pH, dissolved oxygen, viscosity, and cutoff potential) on self-discharge of batteries based on WIPSE and lignin has been investigated. The pH range is crucial as there is an interplay between long-term stability and high energy density. Indeed, lignin derivatives typically store relatively more charge in acidic media but later promote corrosion affecting device stability. A robust and high-performing organic battery, incorporating potassium polyacrylate as WIPSE, is demonstrated, which expresses good self-discharge behavior for a broad range of pH and with little impact on the atmosphere used for manufacturing. It is believed that the investigation will provide critical insights to the research community to promote the advancement of printed large-scale energy storage devices.

Internet-of-things which requires electronics, energy convertor and storage must be low-cost, recyclable and environmentally friendly. In the development of printed batteries, ideally all the components (electrode and electrolyte) must be printable to ensure low-cost manufacturing via printing technologies. Most of the printed batteries suffer with low power. One of the reasons is the poor ionic conductivity of the electrolyte due to the high viscosity needed for printing relatively thick layers. In the present work we have demonstrated a new class of electrolyte promising for printed organic batteries following the concept of water-in-polymer salt electrolytes (WIPSEs). These highly concentrated electrolytes of potassium polyacrylate are non-flammable, low cost and environmentally friendly. They possess high ionic conductivities (45-87 mS/cm) independent on the macroscopic viscosities varying from 7 to 33000 cP. The decoupling between ionic transport and macroscopic viscosity enables us to demonstrate organic batteries based on WIPSEs that can deliver a high and constant power (similar to 4.5 kW/kg; 7.1-11 mW/cm(2)) independent on the viscosity of the electrolytes. The tunability of the viscosity presents a prerequisite for printed technology manufacturing and compatibility with printed batteries.