Aqueous Zn batteries that provide a synergistic integration of absolute safety and high energy density have been considered as highly promising energy-storage systems for powering electronics. Despite the rapid progress made in developing high-performance cathodes and electrolytes, the underestimated but non-negligible dendrites of Zn anode have been observed to shorten battery lifespan. Herein, this dendrite issue in Zn anodes, with regard to fundamentals, protection strategies, characterization techniques, and theoretical simulations, is systematically discussed. An overall comparison between the Zn dendrite and its Li and Al counterparts, to highlight their differences in both origin and topology, is given. Subsequently, in-depth clarifications of the specific influence factors of Zn dendrites, including the accumulation effect and the cathode loading mass (a distinct factor for laboratory studies and practical applications) are presented. Recent advances in Zn dendrite protection are then comprehensively summarized and categorized to generate an overview of respective superiorities and limitations of various strategies. Accordingly, theoretical computations and advanced characterization approaches are introduced as mechanism guidelines and measurement criteria for dendrite suppression, respectively. The concluding section emphasizes future challenges in addressing the Zn dendrite issue and potential approaches to further promoting the lifespan of Zn batteries.

Dendrites in Zn-Based Batteries.

Increased energy consumption stimulates the development of various energy types. As a result, the storage of these different types of energy becomes a key issue. Supercapacitors, as one important energy storage device, have gained much attention and owned a wide range of applications by taking advantages of micro-size, lightweight, high power density and long cycle life. From this perspective, numerous studies, especially on electrode materials, have been reported and great progress in the advancement in both the fundamental and applied fields of supercapacitor has been achieved. Herein, a review of recent progress in carbon materials for supercapacitor electrodes is presented. First, the two mechanisms of supercapacitors are briefly introduced. Then, research on carbon-based material electrodes for supercapacitor in recent years is summarized, including different dimensional carbon-based materials and biomass-derived carbon materials. The characteristics and fabrication methods of these materials and their performance as capacitor electrodes are discussed. On the basis of these materials, many supercapacitor devices have been developed. Therefore, in the third part, the supercapacitor devices based on these carbon materials are summarized. A brief overview of two types of conventional supercapacitor according to the charge storage mechanism is compiled, including their development process, the merits or withdraws, and the principle of expanding the potential range. Additionally, another fast-developed capacitor, hybrid ion capacitors as a good compromise between battery and supercapacitor are also discussed. Finally, the future aspects and challenges on the carbon-based materials as supercapacitor electrodes are proposed.

Recent progress in carbon-based materials for supercapacitor electrodes: a review

Strategies for the Stabilization of Zn Metal Anodes for Zn‐Ion Batteries

The construction of advanced Zn-ion hybrid supercapacitors (ZHSCs) with high energy density is promising but still challenging, especially at high current densities. In this work, a high-energy and ultrastable aqueous ZHSC is demonstrated by introducing N dopants into a hierarchically porous carbon cathode for the purpose of enhancing its chemical adsorption of Zn ions. Experimental results and theoretical simulations reveal that N doping not only significantly facilitates the chemical adsorption process of Zn ions, but also greatly increases its conductivity, surface wettability, and active sites. Consequently, the as-fabricated aqueous ZHSC based on this N-doped porous carbon cathode displays an exceptionally high energy density of 107.3 Wh kg-1 at a high current density of 4.2 A g-1 , a superb power density of 24.9 kW kg-1 , and an ultralong-term lifespan (99.7% retention after 20 000 cycles), substantially superior to state-of-the-art ZHSCs. Particularly, such a cathode also leads to a quasi-solid-state device with satisfactory energy storage performance, delivering a remarkable energy density of 91.8 Wh kg-1 . The boosted energy storage strategy by tuning the chemical adsorption capability is also applicable to other carbon materials.

Boosting Zn-Ion Energy Storage Capability of Hierarchically Porous Carbon by Promoting Chemical Adsorption.

Strategies for Dendrite-Free Anode in Aqueous Rechargeable Zinc Ion Batteries

Multivalent metal ion hybrid capacitors have been developed as novel electrochemical energy storage systems in recent years. They combine the advantages of multivalent metal ion batteries (e.g., zinc-ion batteries, magnesium-ion batteries, and aluminum-ion batteries) with those of supercapacitors, and are characterized by good rate capability, high energy density, high power output and ultralong cycle life. Herein, after a brief introduction to supercapacitors and multivalent metal ion batteries, we reviewed the recent progress in research on multivalent metal ion hybrid capacitors, with a focus on zinc-ion hybrid capacitors, from the perspectives of design concept, configuration, electrochemical behavior and energy storage mechanism. An outlook of the future research regarding multivalent metal ion hybrid capacitors was also presented. This review will be beneficial for researchers around the world to have a better understanding of multivalent metal ion hybrid capacitors and develop novel electrochemical energy storage systems to meet the demands of rapidly developing electric vehicles and wearable/portable electronic products.

Multivalent metal ion hybrid capacitors: a review with a focus on zinc-ion hybrid capacitors

Flexible and conductive scaffold-stabilized zinc metal anodes for ultralong-life zinc-ion batteries and zinc-ion hybrid capacitors

3D Oxygen-Defective Potassium Vanadate/Carbon Nanoribbon Networks as High-Performance Cathodes for Aqueous Zinc-Ion Batteries

Rechargeable aqueous zinc-ion hybrid capacitors and zinc-ion batteries are promising safe energy storage systems. In this study, amorphous RuO2·H2O for the first time was employed to achieve fast and ultralong-life Zn2+ storage based on a pseudocapacitive storage mechanism. In the RuO2·H2O||Zn zinc-ion hybrid capacitors with Zn(CF3SO3)2 aqueous electrolyte, the RuO2·H2O cathode can reversibly store Zn2+ in a voltage window of 0.4–1.6 V (vs. Zn/Zn2+), delivering a high discharge capacity of 122 mAh g−1. In particular, the zinc-ion hybrid capacitors can be rapidly charged/discharged within 36 s with a very high power density of 16.74 kW kg−1 and a high energy density of 82 Wh kg−1. Besides, the zinc-ion hybrid capacitors demonstrate an ultralong cycle life (over 10,000 charge/discharge cycles). The kinetic analysis elucidates that the ultrafast Zn2+ storage in the RuO2·H2O cathode originates from redox pseudocapacitive reactions. This work could greatly facilitate the development of high-power and safe electrochemical energy storage.

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High-Power and Ultralong-Life Aqueous Zinc-Ion Hybrid Capacitors Based on Pseudocapacitive Charge Storage.

Aqueous Zn-ion hybrid supercapacitors (ZHSs) are increasingly being studied as a novel electrochemical energy storage system with prominent electrochemical performance, high safety and low cost. Herein, high-energy and anti-self-discharge ZHSs are realized based on the fibrous carbon cathodes with hierarchically porous surface and O/N heteroatom functional groups. Hierarchically porous surface of the fabricated free-standing fibrous carbon cathodes not only provides abundant active sites for divalent ion storage, but also optimizes ion transport kinetics. Consequently, the cathodes show a high gravimetric capacity of 156 mAh g−1, superior rate capability (79 mAh g−1 with a very short charge/discharge time of 14 s) and exceptional cycling stability. Meanwhile, hierarchical pore structure and suitable surface functional groups of the cathodes endow ZHSs with a high energy density of 127 Wh kg−1, a high power density of 15.3 kW kg−1 and good anti-self-discharge performance. Mechanism investigation reveals that ZHS electrochemistry involves cation adsorption/desorption and Zn4SO4(OH)6·5H2O formation/dissolution at low voltage and anion adsorption/desorption at high voltage on carbon cathodes. The roles of these reactions in energy storage of ZHSs are elucidated. This work not only paves a way for high-performance cathode materials of ZHSs, but also provides a deeper understanding of ZHS electrochemistry.

/pdf/towards-high-energy-and-anti-self-discharge-zn-ion-hybrid-26oagk8kjt.pdf

Wang Yang

Papers

Multivalent metal ion hybrid capacitors: a review with a focus on zinc-ion hybrid capacitors

Flexible and conductive scaffold-stabilized zinc metal anodes for ultralong-life zinc-ion batteries and zinc-ion hybrid capacitors

3D Oxygen-Defective Potassium Vanadate/Carbon Nanoribbon Networks as High-Performance Cathodes for Aqueous Zinc-Ion Batteries

High-Power and Ultralong-Life Aqueous Zinc-Ion Hybrid Capacitors Based on Pseudocapacitive Charge Storage.

Towards High-Energy and Anti-Self-Discharge Zn-Ion Hybrid Supercapacitors with New Understanding of the Electrochemistry.