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82 Page 2 of 13 1 Introduction While dominating the rechargeable (i.e., secondary) bat- tery market with outstanding energy-/power-density and long lifespan, lithium-ion batteries (LIBs) are still seriously suffering from cost and, especially safety issues [1], due to the use of scarce/high-price elements (e.g., Li, Co) [2] and flammable organic electrolytes [3]. Therefore, the traditional aqueous Pb-acid batteries, despite low energy–density, short-lived and polluting-potential, are still widely adopted in many application scenarios where operational safety and/ or cost are the top priorities [4]. With the rapid development of smart grid and large-scale electrochemical energy storage devices, it becomes urgent to develop aqueous batteries that are simultaneously safe, low-cost, green, long-lasting, and high-performance [5]. Significantly, Zn is not only the anode of the historic “vol- taic pile,” but also one of the rare metallic anodes success- fully commercialized in primary aqueous batteries (e.g., Zn alkaline, Ag-Zn, and Zn-air batteries) [6, 7], thanks to its multifaceted advantages including large theoretical capacity, abundant resource, low-cost, non-toxicity, and high electri- cal conductivity [8]. Encouraged by the success in primary batteries, numerous attempts have recently been devoted to the development of rechargeable zinc metal batteries (ZMBs) [9, 10]. Nevertheless, converting primary ZMBs into rechargeable is difficult [11], because the repeated Zn striping/plating processes on the anodes dramatically accel- erate detrimental parasitic reactions [12], including dendritic Zn deposition [13, 14], surface corrosion/passivation [15], and electrolyte decomposition/consumption [16]. Further- more, many intercalation-type ZMBs’ cathodes are unstable in the aqueous electrolytes [17], due to byproduct-derived surface passivation [18] and/or electrolyte etching [19–21]. Remarkably, iodine (I2) cathode stores electrons through the direct conversion reaction between solid I2 and solu- ble I− anions, providing a significant theoretical capacity of 211 mAh g−1 [22, 23]. This reaction does not generate irreversible byproduct, thus is highly reversible and virtually passivation-free [24]. Even when the I2 is etched or reduced by specific component in the electrolytes, the resulting I− species can still contribute capacity by oxidizing back to I2 in following charge process, thanks to its high solubility and proper redox potential [25, 26]. The major problems of this affordable cathode lie on the low electrical conductivity Nano-Micro Lett. (2022) 14:82 of I2, as well as the formation of soluble triiodide (i.e., I3−) intermediate species via I2/I− complexing (I2 + I− → I3−) [27, 28]. The I3− dissolving in electrolyte can easily penetrate through routine glass fibers (GFs) [29] or polypropylene [30] separators, and quickly react with the metallic Zn anode (by I3− + Zn → Zn2+ + I−), leading to fast I2 loss and self-dis- charge [23, 31]. − To restrain the free migration of I3 , the I2 active materials are usually confined into porous matrix with high adsorption capability (e.g., active carbon [28–30, 32] and MXene [33]) and even electrocatalytic ability (Co/Fe-hexacyanoferrate [27]). The nano-pore confining design restrains both I3− gen- eration and migration, leading to much-improved cycle and shelf life [27, 29]. At the same time, the AC (active carbon) and MXene matrix contribute not only additional capacity, but also prominent electrical conductivity, ensuring high I2-utilizing efficiencies even at high-rate charge/discharge [28]. Moreover, manipulating the electrolytes with novel zinc salts [29] or immobile anionic gelatinizing skeletons [34] prove also effective to suppress the I3−-shuttling from cathode to anode, by means of modulating either coordina- tion [29] or electrostatic repulsion between I3− and the elec- trolyte [34], respectively. In the well-established Zn||I2 flow batteries, the famous nafion cation-exchange membranes, as benchmark commercial separators, are usually employed to suppress the crossover migration of I3− anions [35]. Unfor- tunately, nafion membranes are, currently, too expensive to maintain the cost competitiveness of the Zn||I2 batteries, even being robust and durable. To circumvent this dilemma, Zhou’s group invented an artful ionic-sieve membrane sepa- rator based on Zn-BTC metal organic framework (MOF) [23]. This MOF separator can block not only I3− shuttling, but also parasitic reactions by regulating the electrolyte sol- vation structure. In Zn||I2 batteries, almost all the parasitic reactions termi- nate on the surfaces of Zn anodes [16, 17]. Therefore, modi- fying Zn anode’s surface with protecting coatings should be one of the most straightforward and thorough approaches to synchronously restrain these detrimental processes [13, 36, 37]. An adequate protecting coating can virtually isolate Zn anodes from the aqueous electrolytes [38], effectively sup- pressing Zn corrosion/passivation, H2 evolution and electro- lyte consumption that associate with the reaction between Zn and electrolyte [16, 39], as well as the quick self-discharge caused by reactions between I3− and Zn [40]. It means that © The authors https://doi.org/10.1007/s40820-022-00825-5PDF Image | Boosting Zn Battery by Coating a Zeolite‐Based Cation‐Exchange
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