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Benefiting from the advantageous features of high safety, abundant reserves, low cost, and high energy density, aqueous Zn‐based rechargeable batteries (AZBs) have received extensive attention as promising candidates for energy storage. To achieve high‐performance AZBs with high reversibility and energy density, great efforts have been devoted to overcoming their drawbacks by focusing on the modification of electrode materials and electrolytes. Based on different cathode materials and aqueous electrolytes, the development of aqueous AZBs with different redox mechanisms are discussed in this review, including insertion/extraction chemistries (e.g., Zn2+, alkali metal ion, H+, NH4+, and so forth) dissolution/deposition reactions (e.g., MnO2/Mn2+), redox couples in flow batteries (e.g., I3−/3I−, Br2/Br−, and so forth), oxygen electrochemistry (e.g., O2/OH−, O2/O22−), and carbon dioxide electrochemistry (e.g., CO2/CO, CO2/HCOOH). In particular, the basic reaction mechanisms, issues with the Zn electrode, aqueous electrolytes, and cathode materials as well as their design strategies are systematically reviewed. Finally, the remaining challenges faced by AZBs are summarized, and perspectives for further investigations are proposed. The main mechanisms, challenges, and most recent advances of various aqueous Zn‐based batteries (AZBs) are comprehensively reviewed. The development of the design of Zn anodes, electrolytes, cell configurations, and the modification of cathode materials are highlighted. Finally, future perspectives regarding different components are proposed. This review provides valuable instructions on the design of high‐performance AZBs.

The rapid expansion of renewable energies asks for great progress of energy-storage technologies for sustainable energy supplies, which raises the compelling demand of high-performance rechargeable batteries. To satisfy the huge demand from the coming energy-storage market, the resource and cost-effectiveness of rechargeable batteries become more and more important. Manganese (Mn) as a key transition element with advantages including high abundance, low cost, and low toxicity derives various kinds (spinels, layered oxides, polyanions, Prussian blue analogs, etc. ) of high-performance Mn-based electrode materials, especially cathodes, for rechargeable batteries ranging from Li-ion batteries, Na-ion batteries, aqueous batteries, to multivalent metal-ion batteries. It is anticipated that Mn-based materials with Mn as the major transition-metal element will constitute a flourishing family of Mn-based rechargeable batteries (MnRBs) for large-scale and differentiated energy-storage applications. On the other hand, several critical issues including Jahn-Teller effect, Mn dissolution, and O release greatly hinder the pace of MnRBs, which require extensive material optimizations and battery/system improvements. This review aims to provide an investigation about Mn-based materials and batteries for the coming energy-storage demands, with compelling issues and challenges that must be overcome.

Conducting polyaniline (PANI) with high conductivity, ease of synthesis, high flexibility, low cost, environmental friendliness and unique redox properties has been extensively applied in electrochemical energy storage and conversion technologies including supercapacitors, rechargeable batteries and fuel cells. Pure PANI exhibits inferior stability as supercapacitive electrode, and can not meet the ever-increasing demand for more stable molecular structure, higher power/energy density and more N-active sites. The combination of PANI and other active materials like carbon materials, metal compounds and other conducting polymers (CPs) can make up for these disadvantages as supercapacitive electrode. As for rechargeable batteries and fuel cells, recent research related to PANI mainly focus on PANI modified composite electrodes and supported composite electrocatalysts respectively. In various PANI based composite structures, PANI usually acts as a conductive layer and network, and the resultant PANI based composites with various unique structures have demonstrated superior electrochemical performance in supercapacitors, rechargeable batteries and fuel cells due to the synergistic effect. Additionally, PANI derived N-doped carbon materials also have been widely used as metal-free electrocatalysts for fuel cells, which is also involved in this review. In the end, we give a brief outline of future advances and research directions on PANI.

Hollow carbon-based nanostructures (HCNs) have found broad applications in various fields, particularly rechargeable batteries. However, the syntheses of HCNs usually rely on template methods, which are time-consuming, low-yield, and environmentally detrimental. Metal-organic frameworks (MOFs), constructed by organic ligands and inorganic metal nodes, have been identified as effect platforms for preparing HCNs without adding extra templates. This review summarized the recent progress in template-free synthesis of HCNs enabled by MOFs and their applications in rechargeable batteries. Different template-free strategies were introduced first with mechanistic insights into the hollowing mechanism. Then the electrochemical performances of the HCNs were discussed with highlight on the structure-function correlation. It is found that the built-in cavities and nonporous for HCNs is of critical importance to increase the storage sites for high capacity, to enhance charge and mass transport kinetics for high-rate capability, and to ensure the resilient electrode structure for stable cycling. Finally, the challenges and opportunities regarding MOFs-derived HCNs and their applications in rechargeable batteries were discussed.

The increasingly serious environmental challenges have gradually aroused people’s interest in electric vehicles. Over the last decade, governments and automakers have collaborated on the manufacturing of electric vehicles with high performance. Cutting-edge battery technologies are pivotal for the performance of electric vehicles. Zn–air batteries are considered as potential power batteries for electric vehicles due to their high capacity. Zn–air battery researches can be classified into three categories: primary batteries, mechanically rechargeable batteries, and chemically rechargeable batteries. The majority of current studies aim at developing and improving chemically rechargeable and mechanically rechargeable Zn–air batteries. Researchers have tried to use catalytic materials design and device design for Zn–air batteries to make it possible for their applications in electric vehicles. This review will highlight the state-of-the-art in primary batteries, mechanically rechargeable batteries, and chemically rechargeable batteries, revealing the prospects of Zn–air batteries for electric vehicles.

HighlightsA comprehensive discussion of the recent advances in zinc–bromine rechargeable batteries with flow or non-flow electrolytes is presented.The fundamental electrochemical aspects including the key challenges and promising solutions in both zinc and bromine half-cells are reviewed.The key performance metrics of ZBRBs and assessment methods using various ex situ and in situ/operando techniques are also discussed.Zinc–bromine rechargeable batteries (ZBRBs) are one of the most powerful candidates for next-generation energy storage due to their potentially lower material cost, deep discharge capability, non-flammable electrolytes, relatively long lifetime and good reversibility. However, many opportunities remain to improve the efficiency and stability of these batteries for long-life operation. Here, we discuss the device configurations, working mechanisms and performance evaluation of ZBRBs. Both non-flow (static) and flow-type cells are highlighted in detail in this review. The fundamental electrochemical aspects, including the key challenges and promising solutions, are discussed, with particular attention paid to zinc and bromine half-cells, as their performance plays a critical role in determining the electrochemical performance of the battery system. The following sections examine the key performance metrics of ZBRBs and assessment methods using various ex situ and in situ/operando techniques. The review concludes with insights into future developments and prospects for high-performance ZBRBs.

Unregulated lithium (Li) growth is the major cause of low Coulombic efficiency, short cycle life and safety hazards for rechargeable Li metal batteries. Strategies that aim to achieve large granular Li deposits have been extensively explored, and yet it remains a challenge to achieve the ideal Li deposits, which consist of large Li particles that are seamlessly packed on the electrode and can be reversibly deposited and stripped. Here we report a dense Li deposition (99.49% electrode density) with an ideal columnar structure that is achieved by controlling the uniaxial stack pressure during battery operation. Using multiscale characterization and simulation, we elucidate the critical role of stack pressure on Li nucleation, growth and dissolution processes and propose a Li-reservoir-testing protocol to maintain the ideal Li morphology during extended cycling. The precise manipulation of Li deposition and dissolution is a critical step to enable fast charging and a low-temperature operation for Li metal batteries. Li electrodeposition is a fundamental process in Li metal batteries and its reversibility is crucial for battery operation. The authors investigate the effects of stack pressure on Li deposition and associated processes and discuss strategies for achieving dense Li deposits and practical Li metal batteries.

Aqueous rechargeable batteries are a possible strategy for large-scale energy storage systems. However, limited choices of anode materials restrict their further application. Here we report phenazine (PNZ) as stable anode materials in different alkali-ion (Li + , Na + , K + ) electrolyte. A novel full cell is assembled by phenazine anode, Na 0.44 MnO 2 cathode and 10 M NaOH electrolyte to further explore the electrochemical performance of phenazine anode. This battery is able to achieve high capacity (176.7 mAh·g −1 at 4 C (1.2·Ag −1 )), ultralong cycling life (capacity retention of 80% after 13,000 cycles at 4 C), and excellent rate capacity (92 mAh·g −1 at 100 C (30 A·g −1 )). The reaction mechanism of PNZ during charge—discharge process is demonstrated by in situ Raman spectroscopy, in situ Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations. Furthermore, the system is able to successfully operate at wide temperature range from −20 to 70 °C and achieves remarkable electrochemical performance.

With the excessive consumption of nonrenewable resources, the exploration of effective and durable materials is highly sought after in the field of sustainable energy conversion and storage system. In this aspect, metal‐organic frameworks (MOFs) are a new class of crystalline porous organic‐inorganic hybrid materials. MOFs have recently been gaining traction in energy‐related fields. Owing to the coordination flexibility and multiple accessible oxidation states of vanadium ions or clusters, vanadium‐MOFs (V‐MOFs) possess unique structural characteristics and satisfactory electrochemical properties. Furthermore, V‐MOFs‐derived materials also exhibit superior electrical conductivity and stability when used as electrocatalysts and electrode materials. This review summarizes the research progress of V‐MOFs (inclusive of pristine V‐MOFs, V/M‐MOFs, and POV‐based MOFs) and their derivatives (vanadium oxides, carbon‐coated vanadium oxide, vanadium phosphate, vanadate, and other vanadium doped nanomaterials) in electrochemical energy conversion (water splitting, oxygen reduction reaction) and energy storage (supercapacitor, rechargeable battery). Future possibilities and challenges for V‐MOFs and their derivatives in terms of design and synthesis are discussed. Lastly, their applications in energy‐related fields are also highlighted. Emerging metal‐organic framework‐based materials are widely used in energy‐related applications due to their structural and compositional advantages. This review discusses the research progress of V‐MOFs (the pristine V‐MOFs, V/M‐MOFs, and POV‐based MOFs) and their derivatives (vanadium oxides, carbon‐coated vanadium oxide, vanadium phosphate, vanadate) for electrochemical energy conversion and storage, focusing on electrolytic water, supercapacitors and metal‐ion batteries, and prospects for future research directions.

Reducing our carbon footprint is one of the most pressing issues facing humanity today. The technology of Li‐rechargeable batteries is permeating every corner of our lives as a result of our efforts to reduce the use of carbon energy. Batteries can be seen metaphorically as “living cells”, and approaching the future of that technology requires observing and understanding the real‐time phenomena that occur inside battery systems during (electro)chemical reactions. In this regard, in situ analysis techniques have made significant progress toward understanding the basic science of battery systems and finding better performance‐improving factors. There are various analysis methods utilizing electromagnetic waves, electrons, and neutrons to perform multifaceted analyses of battery systems from the atomic to the macroscopic scale. Now is the opportune moment to construct a comprehensive guide that facilitates the design of advanced Li‐rechargeable battery systems, adopting a highly discerning and all‐encompassing approach toward these cutting‐edge technologies. In this review article, we discuss and organize the key components such as capabilities, limitations, and practical tips with a comprehensive perspective on various in situ techniques. Moreover, this article covers a wide range of information from the nano to the micrometer scale, such as electronic, atomic, crystal, and morphological structures, from stereoscopic perspectives considering the probing depth. This review categorizes widely used in situ analytical techniques based on their sources, including electromagnetic waves, electrons, neutrons, and others. One or a combination of these techniques is effective in diagnosing complex dynamic phenomena from an electronic, atomic, molecular, crystal structure, and morphology perspective. These deeper insights are crucial for enhancing the performance of lithium rechargeable batteries.