Herein, a novel dual single-atom catalyst comprising adjacent Fe-N4 and Mn-N4 sites on 2D ultrathin N-doped carbon nanosheets with porous structure (FeMn-DSAC) was constructed as the cathode for a flexible low-temperature Zn-air battery (ZAB). FeMn-DSAC exhibits remarkable bifunctional activities for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Control experiments and density functional theory calculations reveal that the catalytic activity arises from the cooperative effect of the Fe/Mn dual-sites aiding *OOH dissociation as well as the porous 2D nanosheet structure promoting active sits exposure and mass transfer during the reaction process. The excellent bifunctional activity of FeMn-DSAC enables the ZAB to operate efficiently at ultra-low temperature of -40 °C, delivering 30 mW cm-2 peak power density and retaining up to 86 % specific capacity from the room temperature counterpart. 

Engineering Dual Single‐Atom Sites on 2D Ultrathin N‐doped Carbon Nanosheets Attaining Ultra‐Low Temperature Zn‐Air Battery

Quasi-solid-state Zn-air batteries are usually limited to relatively low-rate ability (<10 mA cm-2), which is caused in part by sluggish oxygen electrocatalysis and unstable electrochemical interfaces. Here we present a high-rate and robust quasi-solid-state Zn-air battery enabled by atomically dispersed cobalt sites anchored on wrinkled nitrogen doped graphene as the air cathode and a polyacrylamide organohydrogel electrolyte with its hydrogen-bond network modified by the addition of dimethyl sulfoxide. This design enables a cycling current density of 100 mA cm-2 over 50 h at 25 °C. A low-temperature cycling stability of over 300 h (at 0.5 mA cm-2) with over 90% capacity retention at -60 °C and a broad temperature adaptability (-60 to 60 °C) are also demonstrated. 

https://www.nature.com/articles/s41467-022-31383-4.pdf

Quasi-solid-state Zn-air batteries with an atomically dispersed cobalt electrocatalyst and organohydrogel electrolyte

Zinc‐based batteries are potential candidates for flexible energy storage due to their high capacity, low cost, and intrinsic safety. Hydrogel electrolytes with saturated aqueous solvents can provide remarkable electrochemical performance while retaining satisfactory flexibility for zinc‐based batteries. The past decades have witnessed their fast growth. However, the study of zinc‐based batteries with hydrogel electrolytes under extreme conditions is still in the early stages and many technical issues remain to be addressed. In this review, the physical and chemical properties of hydrogel electrolytes are discussed for application in zinc‐based batteries. Strategies towards hydrogel electrolytes and flexible zinc‐based batteries under extremely high/low temperatures or under deformation conditions and their behaviors are reviewed and analyzed. Moreover, design strategies for all‐around hydrogel electrolyte that are appropriate for use in all these extreme conditions are proposed. A perspective discussing the challenges and future directions of hydrogel electrolyte for zinc‐based batteries is also provided.

Multi-Functional Hydrogels for Flexible Zinc-Based Batteries Working under Extreme Conditions

The ever-increasing demand for flexible and portable electronics has stimulated research and development in building advanced electrochemical energy devices which are lightweight, ultrathin, small in size, bendable, foldable, knittable, wearable, and/or stretchable. In such flexible and portable devices, semi-solid/solid electrolytes besides anodes and cathodes are the necessary components determining the energy/power performances. By serving as the ion transport channels, such semi-solid/solid electrolytes may be beneficial to resolving the issues of leakage, electrode corrosion, and metal electrode dendrite growth. In this paper, the fundamentals of semi-solid/solid electrolytes (e.g., chemical composition, ionic conductivity, electrochemical window, mechanical strength, thermal stability, and other attractive features), the electrode-electrolyte interfacial properties, and their relationships with the performance of various energy devices (e.g., supercapacitors, secondary ion batteries, metal-sulfur batteries, and metal-air batteries) are comprehensively reviewed in terms of materials synthesis and/or characterization, functional mechanisms, and device assembling for performance validation. The most recent advancements in improving the performance of electrochemical energy devices are summarized with focuses on analyzing the existing technical challenges (e.g., solid electrolyte interphase formation, metal electrode dendrite growth, polysulfide shuttle issue, electrolyte instability in half-open battery structure) and the strategies for overcoming these challenges through modification of semi-solid/solid electrolyte materials. Several possible directions for future research and development are proposed for going beyond existing technological bottlenecks and achieving desirable flexible and portable electrochemical energy devices to fulfill their practical applications. It is expected that this review may provide the readers with a comprehensive cross-technology understanding of the semi-solid/solid electrolytes for facilitating their current and future researches on the flexible and portable electrochemical energy devices.

Opportunities of Flexible and Portable Electrochemical Devices for Energy Storage: Expanding the Spotlight onto Semi-solid/Solid Electrolytes.

Recent progress on advanced polymer-based electrolytes in zinc–air batteries

Flexible solid-state rechargeable batteries have attracted extensive attention for their potential to accommodate the deep integration between humans and flexible electronics. To achieve a wide ope...

A flexible and safe aqueous Zinc-Air battery with a wide operating temperature range from -20 to 70 °C

The development of transparent and flexible sensors suitable for the full-range monitoring of human activities is highly desirable, yet presents a daunting challenge due to the need for a combination of properties such as high stretchability, high sensitivity, and good linearity. Gradient structures are commonly found in many biological systems and exhibit excellent mechanical properties. Here, we report a novel surface-confined gradient conductive network (SGN) strategy to construct conductive polymer hydrogel-based stain sensors (CHSS). This CHSS showed an ultrahigh stretchability of 4000% strain, transparency above 90% at a wavelength of 600 nm, as well as skin-like Young's modulus of 40 kPa. Impressively, the sensitivity was improved to 3.0 and outstanding linear sensing performance was achieved simultaneously in the ultrawide range of 0% to 4000% strain with a high R-square value of 0.994. With the help of SGN strategy, this CHSS was able to monitor both large-scale and small-scale human motions and activities. This SGN strategy can open a new avenue for the development of novel flexible strain sensors with excellent mechanical, transparent, and sensing performance for full-range monitoring of human activities.

A Surface-Confined Gradient Conductive Network Strategy for Transparent Strain Sensors toward Full-Range Monitoring.

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A flexible and safe aqueous Zinc-Air battery with a wide operating temperature range from -20 to 70 °C

A Surface-Confined Gradient Conductive Network Strategy for Transparent Strain Sensors toward Full-Range Monitoring.