Although current high-energy-density lithium-ion batteries (LIBs) have taken over the commercial rechargeable battery market, increasing concerns about limited lithium resources, high cost, and insecurity of organic electrolyte scale-up limit their further development. Rechargeable aqueous zinc-ion batteries (ZIBs), an alternative battery chemistry, have paved the way not only for realizing environmentally benign and safe energy storage devices but also for reducing the manufacturing costs of next-generation batteries. This Review underscores recent advances in aqueous ZIBs; these include the design of a highly reversible Zn anode, optimization of the electrolyte, and a wide range of cathode materials and their energy storage mechanisms. We also present recent advanced techniques that aim at overcoming the current issues in aqueous ZIB systems. This Review on the future perspectives and research directions will provide a guide for future aqueous ZIB study.

Recent Advances in Aqueous Zinc-Ion Batteries

Zinc-ion batteries built on water-based electrolytes featuring compelling price-points, competitive performance, and enhanced safety represent advanced energy storage chemistry as a promising alternative to current lithium-ion battery systems. Attempts to develop rechargeable aqueous zinc-ion batteries (ZIBs) can be traced to as early as the 1980s; however, since 2015, the research activity in this field has surged throughout the world. Despite the achievements made in exploring electrode materials so far, significant challenges remain at the material level and even on the whole aqueous ZIBs system, leading to the failure of ZIBs to meet commercial requirements. This review aims to discuss how to pave the way for developing aqueous ZIBs. The current research efforts related to aqueous ZIBs electrode materials and electrolytes are summarized, including an analysis of the problems encountered in both cathode/anode materials and electrolyte optimization. Some concerns and feasible solutions for achieving practical aqueous ZIBs are discussed in detail. We would like to point out that merely improving the electrode materials is not enough; synergistic optimization strategies toward the whole battery system are also deeply needed. Finally, some perspectives are provided on the subsequent optimization design for further research efforts in the aqueous ZIB field.

Issues and opportunities facing aqueous zinc-ion batteries

Aqueous Zn anodes have been revisited for their intrinsic safety, low cost, and high volumetric capacity; however, deep-seated issues of dendrite growth and intricate side-reactions hindered their rejuvenation. Herein, a “brightener-inspired” polyamide coating layer which elevates the nucleation barrier and restricts Zn2+ 2D diffusion is constructed to effectively regulate the aqueous Zn deposition behavior. Importantly, serving as a buffer layer that isolates active Zn from bulk electrolytes, this interphase also suppresses free water/O2-induced corrosion and passivation. With this synergy effect, the polymer-modified Zn anode produces reversible, dendrite-free plating/stripping with a 60-fold enhancement in running lifetime (over 8000 hours) compared to the bare Zn, and even at an ultrahigh areal capacity of 10 mA h cm−2 (10 mA cm−2 for 1 h, 85% depth of discharge). This efficient rechargeability for Zn anodes enables a substantially stable full-cell paired with a MnO2 cathode. The strategy presented here is straightforward and scalable, representing a stark, but promising approach to solve the anode issues in advanced Zn batteries.

Long-life and deeply rechargeable aqueous Zn anodes enabled by a multifunctional brightener-inspired interphase

https://www.cell.com/joule/pdf/S2542-4351(20)30094-5.pdf

Scientific Challenges for the Implementation of Zn-Ion Batteries

Safety concerns about organic media-based batteries are the key public arguments against their widespread usage. Aqueous batteries (ABs), based on water which is environmentally benign, provide a promising alternative for safe, cost-effective, and scalable energy storage, with high power density and tolerance against mishandling. Research interests and achievements in ABs have surged globally in the past 5 years. However, their large-scale application is plagued by the limited output voltage and inadequate energy density. We present the challenges in AB fundamental research, focusing on the design of advanced materials and practical applications of whole devices. Potential interactions of the challenges in different AB systems are established. A critical appraisal of recent advances in ABs is presented for addressing the key issues, with special emphasis on the connection between advanced materials and emerging electrochemistry. Last, we provide a roadmap starting with material design and ending with the commercialization of next-generation reliable ABs.

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Roadmap for advanced aqueous batteries: From design of materials to applications.

/pdf/recent-advances-in-zn-ion-batteries-utvauxy3ub.pdf

Recent Advances in Zn-Ion Batteries

Polynary transition-metal atom catalysts are promising to supersede platinum (Pt)-based catalysts for oxygen reduction reaction (ORR). Regulating the local configuration of atomic catalysts is the key to catalyst performance enhancement. Different from the previously reported single-atom or dual-atom configurations, a new type of ternary-atom catalyst, which consists of atomically dispersed, nitrogen-coordinated Co-Co dimers, and Fe single sites (i.e., Co2 -N6 and Fe-N4 structures) that are coanchored on highly graphitized carbon supports is developed. This unique atomic ORR catalyst outperforms the catalysts with only Co2 -N6 or Fe-N4 sites in both alkaline and acid conditions. Density functional theory calculations clearly unravels the synergistic effect of the Co2 -N6 and Fe-N4 sites, which can induce higher filling degree of Fe-d orbitals and favors the binding capability to *OH intermediates (the rate determining step). This ternary-atom catalyst may be a promising alternative to Pt to drive the cathodic ORR in zinc-air batteries.

Atomically Dispersed Co2 -N6 and Fe-N4 Costructures Boost Oxygen Reduction Reaction in Both Alkaline and Acidic Media.

Understanding the Synergistic Effects of Cobalt Single Atoms and Small Nanoparticles: Enhancing Oxygen Reduction Reaction Catalytic Activity and Stability for Zinc-Air Batteries

Aqueous Zinc-ion batteries (ZIBs), using zinc negative electrode and aqueous electrolyte, have attracted great attention in energy storage field due to the reliable safety and low-cost. A composite material comprised of VO2·0.2H2O nanocuboids anchored on graphene sheets (VOG) is synthesized through a facile and efficient microwave-assisted solvothermal strategy and is used as aqueous ZIBs cathode material. Owing to the synergistic effects between the high conductivity of graphene sheets and the desirable structural features of VO2·0.2H2O nanocuboids, the VOG electrode has excellent electronic and ionic transport ability, resulting in superior Zn ions storage performance. The Zn/VOG system delivers ultrahigh specific capacity of 423 mAh·g−1 at 0.25 A·g−1 and exhibits good cycling stability of up to 1,000 cycles at 8 A·g−1 with 87% capacity retention. Systematical structural and elemental characterizations confirm that the interlayer space of VO2·0.2H2O nanocuboids can adapt to the reversible Zn ions insertion/extraction. The as-prepared VOG composite is a promising cathode material with remarkable electrochemical performance for low-cost and safe aqueous rechargeable ZIBs.

VO2·0.2H2O nanocuboids anchored onto graphene sheets as the cathode material for ultrahigh capacity aqueous zinc ion batteries

/pdf/partial-nitridation-induced-electrochemistry-enhancement-of-m98khkbbsh.pdf

Hua Tan

Papers

Recent Advances in Zn-Ion Batteries

Atomically Dispersed Co2 -N6 and Fe-N4 Costructures Boost Oxygen Reduction Reaction in Both Alkaline and Acidic Media.

Understanding the Synergistic Effects of Cobalt Single Atoms and Small Nanoparticles: Enhancing Oxygen Reduction Reaction Catalytic Activity and Stability for Zinc-Air Batteries

VO2·0.2H2O nanocuboids anchored onto graphene sheets as the cathode material for ultrahigh capacity aqueous zinc ion batteries

Partial Nitridation-Induced Electrochemistry Enhancement of Ternary Oxide Nanosheets for Fiber Energy Storage Device