A conventional two-electrode rechargeable zinc-air battery (RZAB) has two major problems. (1) Opposing requirements for the oxygen reduction (ORR) and oxygen evolution (OER) reactions from the catalyst at the air cathode. (2) Zinc dendrite formation, hydrogen generation and zinc corrosion at the zinc anode. To tackle these problems, we have developed a three-electrode RZAB (T-RZAB) including a hydrophobic discharge cathode, a hydrophilic charge cathode, and a zinc-free anode. The decoupled cathodes enable fast ORR and OER kinetics, and avoid oxidization of the ORR catalyst. The zinc-free anode using tin-coated copper foam that induces the growth of (002)Zn planes, suppresses hydrogen evolution and prevents Zn corrosion. As a result, the T-RZABs have a high discharge capacity per cycle of 800 mAh cm-2 , a low voltage gap between discharge/charge platforms of 0.66 V, and an ultra-long cycle life of 5220 hours at a current density of 10 mA cm-2 . We have developed a large T-RZAB which has a discharge capacity of 10 ampere-hours per cycle with no obvious degradation after cycling for 1000 hours. Finally, we assembled a T-RZAB pack that had an energy density of 151.8 watt-hours per kilogram and a low cost of 46.7 US dollars per kilowatt-hour. This article is protected by copyright. All rights reserved.

Rechargeable zinc-air batteries with an ultra-large discharge capacity per cycle and an ultra-long cycle life.

The practical application of infancy‐stage rocking‐chair Zn‐ion batteries is predominately retarded by the strong electrostatic interaction between traditional anode materials with bivalent Zn2+, resulting in irreversible serious structural damage, unsatisfactory cycling stabilities, and poor rate performances. Herein, an advanced dual electric field in situ induced intercalation/conversion dual‐mechanism Na1.6TiS2/CuSe2 heterointerface anode towards ultrastable aqueous rocking‐chair zinc‐ion batteries is successfully constructed. The rational constructions of huge heterointerfaces between different phases generate built‐in electric fields, reducing the energy barrier for ion migration, facilitating electron/ion diffusion, decreasing charge transfer resistances, and establishing an excellent conducting network. The enhanced interactions of different atoms at the phase interface alleviate the tensile strain and stabilize the lattice, achieving superior Zn2+ diffusion kinetics. The dual‐mechanism Na1.6TiS2/CuSe2 heterostructures can reach a discharge capacity of 142 mAh g−1 at 0.2 A g−1. It still reaches a discharge capacity of 133 mAh g−1 when the current density recovers to 0.2 A g−1 after a high current evaluation of 10 A g−1 with remarkable capacity retention (83.8% at 5A g−1 after 12 000 cycles). This breakthrough opens a new avenue for the targeted design of rocking‐chair zinc‐ion batteries and provides insights into the evolution of heterointerfaces.

Advanced In Situ Induced Dual‐Mechanism Heterointerface Towards Ultrastable Aqueous Rocking‐Chair Zinc‐Ion Batteries

Recently, aqueous zinc-ion batteries with conversion mechanisms have received wide attention in energy storage systems on account of excellent specific capacity, high power density, and energy density. Unfortunately, some characteristics of cathode material, zinc anode, and electrolyte still limit the development of aqueous zinc-ion batteries possessing conversion mechanism. Consequently, this paper provides a detailed summary of the development for numerous aqueous zinc-based batteries: zinc-sulfur (Zn-S) batteries, zinc-selenium (Zn-Se) batteries, zinc-tellurium (Zn-Te) batteries, zinc-iodine (Zn-I2 ) batteries, and zinc-bromine (Zn-Br2 ) batteries. Meanwhile, the reaction conversion mechanism of zinc-based batteries with conversion mechanism and the research progress in the investigation of composite cathode, zinc anode materials, and selection of electrolytes are systematically introduced. Finally, this review comprehensively describes the prospects and outlook of aqueous zinc-ion batteries with conversion mechanism, aiming to promote the rapid development of aqueous zinc-based batteries.

Advances in Aqueous Zinc Ion Batteries based on Conversion Mechanism: Challenges, Strategies, and Prospects.

Aqueous zinc‐ion micro‐batteries (ZIMBs) have attracted considerable attention owing to their reliable safety, low cost, and great potential for wearable devices. However, current ZIMBs still suffer from various critical issues, including short cycle life, poor mechanical stability, and inadequate energy density. Herein, the fabrication of flexible planar ZIMBs with ultrahigh energy density by interfacial engineering in the screen‐printing process based on high‐performance MnO2‐based cathode materials is reported. The Ce‐doped MnO2 (Ce‐MnO2) exhibits significantly enhanced capacity (389.3 mAh g−1), considerable rate capability and admirable cycling stability than that of the pure MnO2. Importantly, the fabrication of micro‐electrodes with ultrahigh mass loading of Ce‐MnO2 (24.12 mg cm−2) and good mechanical stability is achieved through optimizing the interfacial bonding between different printed layers. The fabricated planar ZIMBs achieve a record high capacity (7.21 mAh cm−2 or 497.31 mAh cm−3) and energy density (8.43 mWh cm−2 or 573.45 mWh cm−3), as well as excellent flexibility. Besides, a wearable self‐powered sensing system for environmental monitoring is further demonstrated by integrating the planar ZIMBs with flexible solar cells and a multifunctional sensor array. This work sheds light on the development of high‐performance planar ZIMBs for future self‐powered and eco‐friendly smart wearable electronics.

A Flexible and Safe Planar Zinc‐Ion Micro‐Battery with Ultrahigh Energy Density Enabled by Interfacial Engineering for Wearable Sensing Systems

Abstract Covalent organic frameworks (COFs) are crystalline organic porous polymers that can be precisely integrated by building blocks to achieve pre‐designed composition, components, and functions, making them a powerful platform for the development of molecular devices in the field of electrocatalysis. The precise control of channel/dopant positions and highly ordered network structures of COFs provide an ideal material system for the applications of advanced electrocatalysis. In this paper, the topological structure design and synthesis methods of COFs are reviewed in detail, and their design principles are deeply analyzed. In addition, the applications of COFs and their derivatives in the field of electrocatalysis are systematically summarized and the optimization strategies are proposed. Finally, the application prospects of COFs and their derivatives in electrocatalysis and the challenges that may be encountered in the future are prospected, providing helpful guidance for future research. 

Optimization Strategies of Covalent Organic Frameworks and Their Derivatives for Electrocatalytic Applications

Selenium (Se) is an appealing alternative cathode material for secondary battery systems that recently attracted research interests in the electrochemical energy storage field due to its high theoretical specific capacity and good electronic conductivity. However, despite the relevant capacity contents reported in the literature, Se-based cathodes generally show poor rate capability behavior. To circumvent this issue, we propose a series of selenium@carbon (Se@C) composite positive electrode active materials capable of delivering a four-electron redox reaction when placed in contact with an aqueous copper-ion electrolyte solution (i.e., 0.5 M CuSO4) and copper or zinc foils as negative electrodes. The lab-scale Zn | |Se@C cell delivers a discharge voltage of about 1.2 V at 0.5 A g-1 and an initial discharge capacity of 1263 mAh gSe-1. Interestingly, when a specific charging current of 6 A g-1 is applied, the Zn | |Se@C cell delivers a stable discharge capacity of around 900 mAh gSe-1 independently from the discharge rate. Via physicochemical characterizations and first-principle calculations, we demonstrate that battery performance is strongly associated with the reversible structural changes occurring at the Se-based cathode. 

/pdf/enabling-fast-charging-selenium-based-aqueous-batteries-via-3jpiyyxr.pdf

Enabling fast-charging selenium-based aqueous batteries via conversion reaction with copper ions

Microbatteries (MBs) are promising candidates to provide power for various miniaturized electronic devices, yet they generally suffer from complicated fabrication procedures and low areal energy density. Besides, all cathodes of current MBs are solid state, and the trade-off between areal capacity and reaction kinetics restricts their wide applications. Here, we propose a dual-plating strategy to facilely prepare zinc-bromine MBs (Zn-Br2 MBs) with a liquid cathode to achieve both high areal energy density and fast kinetics simultaneously. The Zn-Br2 MBs deliver a record high areal energy density of 3.6 mWh cm−2, almost an order of magnitude higher than available planar MBs. Meanwhile, they show a polarity-switchable feature to tolerate confusion of cathode and anode. This strategy could also be extended to other battery systems, such as Zn-I2 and Zn-MnO2 MBs. This work not only proposes an effective construction method for MBs but also enriches categories of microscale energy storage devices.

Fast constructing polarity-switchable zinc-bromine microbatteries with high areal energy density

Mesoporous structure of carbon materials plays an important role in electrocatalyst design. Constructing carbon supports with tunable mesopores has long been a challenge. Herein, the elaborate regulation of mesopores in N-doped carbon materials is reported by pyrolyzing energetic metal-triazolate (MET) frameworks with different particle sizes and at different ramp rates. Higher thermal transfer rates brought about by smaller particle size and higher ramp rate lead to more violent decomposition with a large number of gases producing, which in turn result in larger mesopores in the derivatives. Consequently, a series of N-doped carbon materials with controllable mesopores are obtained. As a proof-of-concept, ultrafine Pt nanoparticles are enveloped inside these mesopores to acquire high-performance electrocatalysts for oxygen reduction reaction. The optimized catalyst achieves high mass activity of 1.52 A mgPt−1 at 0.9 ViR-free and peak power density of 0.8 W cm−2 (H2-Air) with an ultralow Pt loading of 0.05 mgPt cm−2 at cathode in fuel cells, highlighting the great advantages of MET-derived carbon materials with controllable mesopores in the preparation of advanced electrocatalysts. 

Metal–Organic Framework‐Derived N‐Doped Carbon with Controllable Mesopore Sizes for Low‐Pt Fuel Cells

To eliminate the concerns about fuel cell aroused by the scarcity of Pt and the sluggish kinetics of oxygen reduction reaction (ORR), shortening the pathway of mass transfer and optimizing the utilization of Pt are two effective ways. Herein, we report a facile strategy to efficiently anchor ultrafine Pt nanoparticles on ultrathin nanobowl-shaped N-doped carbon (Pt NP@BNC). Ultrathin layers of a two-dimensional covalent organic framework (COF) were synthesized as the support via a hard-template strategy and Pt precursors were homogeneously dispersed in the COF via a gas-phase diffusion method. Then the composite was pyrolyzed and converted into ultrathin nanobowl-shaped N-doped carbon (ca. 6 nm) embedded with ultrafine Pt NPs (ca. 3.28±0.7 nm). Compared with the catalyst obtained from the bulk COF, Pt NP@BNC achieved significantly elevated activity towards ORR. This work may pave a new way for the design and synthesis of novel ORR catalysts with high efficiency. 

Ultrafine Pt Nanoparticles Supported on Ultrathin Nanobowl‐shaped N‐doped Carbon for Remarkable Oxygen Reduction Reaction

Multi-twinned gold nanoparticles with tensile surface steps for efficient electrocatalytic CO2 reduction

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