Electrically Activated Ultrathin PVDF‐TrFE Air Filter for High‐Efficiency PM1.0 Filtration

Ultrafine particulate matter (PM) in indoor air has become a serious concern for public health. Therefore, there is a growing interest in filters that can be installed on the window frames of ordinary homes to improve the indoor air quality by natural passive ventilation without using expensive forced air circulation systems. Thus, these filters require a high filtering efficiency and high air permeability and visibility, which do not compromise the original functionality of the windows. The filters developed for this purpose to date have demonstrated a high filtering efficiency for PM_2.5 but a relatively low efficiency for PM_1.0. Here, the performance of the ultrathin poly[(vinylidenefluoride‐co‐trifluoroethylene) (PVDF‐TrFE) nanofiber air filter capable of high‐efficiency PM_1.0 filtration is reported. To enhance the PM_1.0 filtering efficiency, the filter is electrically activated by the polarization of dipoles and triboelectrification using the ferroelectric nature and triboelectrically negative property of the PVDF‐TrFE filter layer. The electrically activated PVDF‐TrFE filter demonstrates a PM_1.0 filtering efficiency of over ≈88% after polarization, which is further improved to ≈94% after triboelectrification. In addition, the filter is ultrathin and air‐permeable with 65% light transmittance. The methods introduced in this work can be adopted to develop high performance, highly visible, and air‐permeable filter media.     

A Fluffy Dual‐Network Structured Nanofiber/Net Filter Enables High‐Efficiency Air Filtration

Particulate matter (PM) pollution has posed a huge health and economic burden worldwide. Most existing air filters used to remove PMs are structurally monotonous, cumbersome, and inevitably suffer from the compromise between removal efficiency and air permeability; developing an advanced air filter that can overcome these limitations is of significance but highly challenging. Herein, a novel strategy to create ultrathin, high‐performance air filters based on fluffy dual‐network structured polyacrylonitrile nanofiber/nets, via a humidity‐induced electrospinning/netting technique, is reported. By tailoring the ejection and phase separation of the charged liquids, this approach causes 2D ultrafine (≈20 nm) nanonets tightly bonded with fluffy pseudo‐3D nanofiber scaffolds to form dual‐network structures, with controllable pore size and stacking density on a large scale. The resultant nanofiber/net filters possess the integrated features of small pore size (<300 nm), high porosity (93.9%), low packing density, combined with desirable surface chemistry (4.3‐D dipole moment), resulting in high‐efficiency PM_0.3 removal (>99.99%), low air resistance (only <0.11% of atmosphere pressure), and promising long‐term PM_2.5 purification. The synthesis of such materials may provide new insights into the design and development of high‐performance filtration and separation materials for various applications.     

High‐Performance PM0.3 Air Filters Using Self‐Polarized Electret Nanofiber/Nets

Particulate matter (PM) pollution in air is thought to be an important mortality risk factor globally. Most existing air filters face the extreme challenge of effectively removing PM_0.3, which has the most penetration particle size (MPPS) of ≈0.3 µm yet is particularly harmful. Here, an innovative in situ electret electrospinning/netting technique that can manipulate both solution phase separation and crystal phase transition is reported to develop self‐polarized polyvinylidene fluoride nanofiber/net membranes with 2D networks and superior surface adhesion. By combining the true nanoscale diameter (≈21 nm), small pore size (≈0.26 µm), and highly electret surface (6.8 kV potential) of the 2D nanonets, the synergistic effect of sieving and adhesion for MPPS PM_0.3 is achieved. Such double capture characteristic enables the high‐efficiency (≈99.998%) capture of PM_0.3 while maintaining low air resistance (≈0.1% atmosphere pressure). Moreover, the nanofiber/net filters show integrated properties of superhydrophobicity, desirable transparency (91%), and long‐term stability. The synthesis of such attractive nanomaterials presents a promising attempt toward the development of high‐performance filtration/separation materials for numerous applications.     

Semi‐Interpenetrating Polymer Network Biomimetic Structure Enables Superelastic and Thermostable Nanofibrous Aerogels for Cascade Filtration of PM2.5

Particulate matter (PM) has taken heavy tolls on the global economy and public health, calling for air filters that can remove PM from high‐temperature emission sources. However, creating desirable filter media capable of capturing polydisperse fine particles (PFPs) effectively and enduringly, while also withstanding high speed airstream, is extremely challenging. Here, a biomimetic and bottom‐up strategy to prepare superelastic, strong, and thermostable nanofibrous aerogels (NFAs) as cascade filters by assembling semi‐interpenetrating polymer network (semi‐IPN)‐based nanofibers into a gradient architecture is reported. Inspired by the robust loofah sponges originating from stiff cellulose networks, the mechanical property of NFAs is enhanced via tailoring the chain flexibility of heat‐resistant semi‐IPNs. Further constructing a gradient cellular architecture endows NFAs with a versatile cascade filtration behavior for capturing polydisperse fine particles. The resultant semi‐IPN‐based gradient NFAs exhibit temperature‐invariant superelasticity, a high compressive stress (7.9 kPa) and modulus (12 kPa), high filtration efficiency (>99.97%, PM_0.3), low pressure drop (≈50% that of membranes), and ultrahigh dust‐holding capacity (114 g m^?2). The fabrication of this attractive material paves the way for designing next‐generation air filters for industrial dust removal.     

基于VOQ输入缓存交换系统调度算法研究

基于VOQ缓存策略的信元调度算法是提升交换系统性能的关键因素。介绍了3种富有代表性的调度算法iSLIP算法、iLQF算法和DPA算法。iSLIP算法易于硬件实现,不大于log2N次迭代即可实现收敛,但对于突发通信效率不高,适用于中小规模的高速交换结构;iLQF算法调度效率高,但硬件实现较为困难,且时延较大,目前应用较少;DPA算法可以用简单的组合逻辑实现,时延小,但效率不高,适用于重载大规模的高速交换结构。     

In Situ Self‐Assembled Polyoxotitanate Cages on Flexible Cellulosic Substrates: Multifunctional Coating for Hydrophobic,Antibacterial, and UV‐Blocking Applications

Surface coating is a powerful approach to fabricate multifunctional materials that are essential for numerous applications. However, to achieve such multifunctional coating with a facile single‐step procedure, especially on flexible substrates, is still a big challenge, as current fabrication protocols usually require sophisticated equipment and complicated procedures. Here, a novel coating technology involving in situ self‐assembly of the polyoxotitanate (POT) cage [Ti₁₈Mn₄O₃₀(OEt)₂₀Phen₃] is reported to fabricate multifunctional cotton fabrics in a single step. The in situ generated spherical microparticles of 0.8 µm average diameter are firmly mounted on the underlying cotton substrate, imparting the coated surface with robust hydrophobicity (water contact angle of 148.1 ± 5.4°), antibacterial activity (against Escherichia coli, Staphylococcus epidermidis, and Staphylococcus aureus), and excellent UV‐blocking performance (89% blocked at 350 nm). This coating technology is efficient, straightforward, requires no specialized equipment, and most importantly, is readily extendable to other flexible substrates. Combined with the rapidly developing area of POT cages and similar molecular materials, the reported technology based on in situ self‐assembly holds great promise for further advancing the fabrication of multifunctional flexible devices via a single‐step coating operation.     

Catalyst Droplet-Based Puncturable Nanostructures with Mechano-Bactericidal Properties Against Bioaerosols

Bioaerosol contamination problems have led to the need for new technologies that effectively collect and inactivate airborne microorganisms. Typical nanomaterial-based filter membranes are usually sterilized using photocatalysts, electrical stimulation, and thermal treatment, which are expensive and require additional devices and cumbersome manufacturing. In this study, a membrane with nanotopographical features is manufactured via a catalyst droplet-based procedure to mechanically damage airborne bacteria. The catalyst droplets are used as templates for in situ novel puncturable nanopillar growth on the membrane surface. Numerical simulations and microscopic observations show that puncturable nanopillars with a thin and rough nano-edge are advantageous for rupturing the bacterial cell compared to flat nanopillars without a thin edge. A puncturable nanostructured air filter (PNAF) is compared to a bare air filter and exhibits higher bioaerosol collection efficiencies (>98% and 89.3–95.7%, respectively). PNAF is tested under breathing conditions as part of a face mask, where it effectively captures and deactivates E. coli aerosols through a mechano-bactericidal effect, resulting in the inhibition of bacterial proliferation and finally death. Thus, PNAF can be applied as an air purifier or face mask filter for bioaerosol collection presenting antibacterial effects without external stimulation.     

3D Wearable Fabric-Based Micro-Supercapacitors with Ultra-High Areal Capacitance

Miniaturized electronics require integrated unit configuration in very limited space, where energy storage per unit area is thus extremely critical. Micro-supercapacitors (MSCs), mainly established on planar substrates, are superior but still suffer from limited areal capacitance. Herein, a novel strategy is introduced to construct high cross-section MSCs using 3D fabrics as the porous skeleton. Interdigitated poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) is patterned on 3D fabrics to achieve continuous conductive networks, while MnO₂ microspheres epitaxially grown on PEDOT:PSS are fully exposed to electrolyte with the support of fabric fibers. The unique architecture can utilize more active sites of thick electrodes and the high conductivity of interpenetrating fiber networks. The resulting fabric-based MSCs demonstrate ultra-high areal capacitance of 135.4 mF cm⁻², which is 3.5 times that of devices on polyethylene terephthalate substrates and is among the highest values for planar-based MSCs using the same interdigital geometry. Moreover, the flexible fabrics endow MSCs with extremely high bending stability with 94% capacitance retention even after 3000 cycles. These figures-of-merit enable fabric-based MSCs promising to be used in the next-generation of wearable electronics.     

Continuously Producing Watersteam and Concentrated Brine from Seawater by Hanging Photothermal Fabrics under Sunlight

Solar‐enabled evaporation for seawater desalination is an attractive, renewable, and environment‐friendly technique, and tremendous progress has been achieved by developing various photothermal membranes. However, traditional photothermal membranes directly float on water, resulting in some limitations such as unavoidable heat‐loss to bulk water and severe salt accumulation. To solve these problems, a hydrophilic, polymer nanorod‐coated photothermal fabric is designed and fabricated, and then an indirect‐contact evaporation system by hanging the fabric is demonstrated. The two ends of the fabric are designed to be in contact with seawater to guide water flow through capillary suction. Both arc‐shaped top/bottom surfaces of the hanging fabrics are exposed to air, which can prevent heat dissipation to bulk seawater and facilitate the double‐surface evaporation upon sunlight irradiation. Our design leads to an efficient evaporation rate of 1.94 kg m^?2 h^?1 and high solar efficiency of 89.9% upon irradiation with sunlight (1.0 kW m^?2). Importantly, the highly concentrated brine can drip from the bottom of the arc‐shaped fabric, without the appearance of solid‐salt accumulation. This indirect‐contact evaporation system establishes a new path to continuously and economically produce watersteam from seawater for fresh‐water and concentrated brine for the chlor‐alkali industry.     

Composition Engineering of All‐Inorganic Perovskite Film for Efficient and Operationally Stable Solar Cells

Cesium‐based inorganic perovskites have recently attracted great research focus due to their excellent optoelectronic properties and thermal stability. However, the operational instability of all‐inorganic perovskites is still a main hindrance for the commercialization. Herein, a facile approach is reported to simultaneously enhance both the efficiency and long‐term stability for all‐inorganic CsPbI_2.5Br_0.5 perovskite solar cells via inducing excess lead iodide (PbI₂) into the precursors. Comprehensive film and device characterizations are conducted to study the influences of excess PbI₂ on the crystal quality, passivation effect, charge dynamics, and photovoltaic performance. It is found that excess PbI₂ improves the crystallization process, producing high‐quality CsPbI_2.5Br_0.5 films with enlarged grain sizes, enhanced crystal orientation, and unchanged phase composition. The residual PbI₂ at the grain boundaries also provides a passivation effect, which improves the optoelectronic properties and charge collection property in optimized devices, leading to a power conversion efficiency up to 17.1% with a high open‐circuit voltage of 1.25 V. More importantly, a remarkable long‐term operational stability is also achieved for the optimized CsPbI_2.5Br_0.5 solar cells, with less than 24% degradation drop at the maximum power point under continuous illumination for 420 h.     

Inherent Guanidine Nanogels with Durable Antibacterial and Bacterially Antiadhesive Properties

Since bacterial infections seriously threaten human's health, considerable attention is devoted to the design of nanoscale antibacterial materials. Among them, metal nanoparticles cannot meet the requirements of durable antibacterial effects and are harmful to biological environments. In this study, environmentally friendly nanogels with durable antibacterial and antiadhesion properties are prepared by copolymerization of styrene, polycaprolactone‐hydroxyethyl methacrylate, and polyhexamethylene guanidine hydrochloride methacrylate. The resultant nanogels possess regular spherical morphologies with the size of about 200 nm. The nanogels exhibit a strong ability to kill bacteria and the mechanism is different from that of conventional antibacterial agent loaded nanoparticles. In addition, anti‐infection experiments explored by a wound model confirm the nanogels have the capability to prevent infection. Furthermore, the nanogels grafted on the surface of cotton fibers display good thermal stability, which is essential for finishing of fabrics. The cotton fabrics finished with nanogels can prevent the adhesion of bacteria by enhancing the hydrophobicity and the bacteriostatic rate. The antibacterial fabrics against Staphylococcus aureus and Escherichia coli are still more than 86% active after 50 times of mechanical washing. The biocompatible nanogels are unleachable from the antibacterial fabrics which demonstrate that they are ideal candidates for durable and environmental‐friendly nanoscaled antimicrobial materials.     

Controlled n‐Doping in Air‐Stable CsPbI2Br Perovskite Solar Cells with a Record Efficiency of 16.79%

Cesium‐based inorganic perovskites, such as CsPbI₂Br, are promising candidates for photovoltaic applications owing to their exceptional optoelectronic properties and outstanding thermal stability. However, the power conversion efficiency of CsPbI₂Br perovskite solar cells (PSCs) is still lower than those of hybrid PSCs and inorganic CsPbI₃ PSCs. In this work, passivation and n‐type doping by adding CaCl₂ to CsPbI₂Br is demonstrated. The crystallinity of the CsPbI₂Br perovskite film is enhanced, and the trap density is suppressed after adding CaCl₂. In addition, the Fermi level of the CsPbI₂Br is changed by the added CaCl₂ to show heavy n‐type doping. As a result, the optimized CsPbI₂Br PSC shows a highest open circuit voltage of 1.32 V and a record efficiency of 16.79%. Meanwhile, high air stability is demonstrated for a CsPbI₂Br PSC with 90% of the initial efficiency remaining after more than 1000 h aging in air.     

MXene Functionalized,Highly Breathable and Sensitive Pressure Sensors with Multi-Layered Porous Structure

Breathable, flexible, and highly sensitive pressure sensors have drawn increasing attention due to their potential in wearable electronics for body-motion monitoring, human-machine interfaces, etc. However, current pressure sensors are usually assembled with polymer substrates or encapsulation layers, thus causing discomfort during wearing (i.e., low air/vapor permeability, mechanical mismatch) and restricting their applications. A breathable and flexible pressure sensor is reported with nonwoven fabrics as both the electrode (printed with MXene interdigitated electrode) and sensing (coated with MXene/silver nanowires) layers via a scalable screen-printing approach. Benefiting from the multi-layered porous structure, the sensor demonstrates good air permeability with high sensitivity (770.86–1434.89 kPa⁻¹), a wide sensing range (0–100 kPa), fast response/recovery time (70/81 ms), and low detection limit (≈1 Pa). Particularly, this sensor can detect full-scale human motion (i.e., small-scale pulse beating and large-scale walking/running) with high sensitivity, excellent cycling stability, and puncture resistance. Additionally, the sensing layer of the pressure sensor also displays superior sensitivity to humidity changes, which is verified by successfully monitoring human breathing and spoken words while wearing a sensor-embedded mask. Given the outstanding features, this breathable sensor shows promise in the wearable electronic field for body health monitoring, sports activity detection, and disease diagnosis.     

Autocatalytic Metallization of Fabrics Using Si Ink,for Biosensors,Batteries and Energy Harvesting

Commercially available metal inks are mainly designed for planar substrates (for example, polyethylene terephthalate foils or ceramics), and they contain hydrophobic polymer binders that fill the pores in fabrics when printed, thus resulting in hydrophobic electrodes. Here, a low‐cost binder‐free method for the metallization of woven and nonwoven fabrics is presented that preserves the 3D structure and hydrophilicity of the substrate. Metals such as Au, Ag, and Pt are grown autocatalytically, using metal salts, inside the fibrous network of fabrics at room temperature in a two‐step process, with a water‐based silicon particle ink acting as precursor. Using this method, (patterned) metallized fabrics are being enabled to be produced with low electrical resistance (less than 3.5 Ω sq^?1). In addition to fabrics, the method is also compatible with other 3D hydrophilic substrates such as nitrocellulose membranes. The versatility of this method is demonstrated by producing coil antennas for wireless energy harvesting, Ag–Zn batteries for energy storage, electrochemical biosensors for the detection of DNA/proteins, and as a substrate for optical sensing by surface enhanced Raman spectroscopy. In the future, this method of metallization may pave the way for new classes of high‐performance devices using low‐cost fabrics.     

Superplastic Air‐Dryable Graphene Hydrogels for Wet‐Press Assembly of Ultrastrong Superelastic Aerogels with Infinite Macroscale

Highly compressible graphene‐based monoliths with excellent mechanical, electrical, and thermal properties hold great potential as multifunctional structural materials to realize the targets of energy‐efficiency, comfort, and safety for buildings, vehicles, aircrafts, etc. Unfortunately, the ultralow mechanical strength and limited macroscale have hampered their practical applications. Herein, ultrastrong superelastic graphene aerogel with infinite macroscale is obtained by a facile wet‐press assembly strategy based on the novel superplastic air‐dryable graphene hydrogel (SAGH). The SAGH with isotropic, open‐cell, and highly porous microstructure is carefully designed by a dual‐template sol–gel method. Countless SAGH “bricks” can be assembled together orderly by press to form the strongly combined wet‐press assembled graphene aerogel (WAGA) “wall” after air‐drying. The WAGA with highly oriented, dense, multiple‐arch microstructure possesses arbitrary macroscale, outstanding compressive strength (47 MPa, over 10 times higher than the best ever reported), super elasticity (>97% strain), and high conductivity (378 S m^?1). The strong adhesion is attributed to the tightly face‐to‐face contacted graphene interfaces caused by wet‐press and air‐drying. The WAGAs prove to be excellent multifunctional structural materials in the fields of high pressure/strain sensor, tunable mechanical energy absorber, high‐performance fire‐resistance, and thermal insulation. This facile strategy is easily extended to fabricate other similar metamaterials.     

Visualizing the Oxidation Mechanism and Morphological Evolution of the Cubic‐Shaped Superoxide Discharge Product in Na–Air Batteries

Sodium–air (Na–O₂) batteries have recently developed as a high theoretical energy density energy storage and conversion system. In particular, Na–O₂ batteries with superoxide as the discharge product have a very high round‐trip energy efficiency over lithium–air batteries due to their significantly reduced charging overpotential. However, Na–O₂ batteries yet suffer from limited cycling lives because of the formation and incomplete removal of side products during oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) processes, while the mechanism of these processes is still not fully understood. Herein, a detailed investigation on tracking the decomposition pathway of cubic‐shaped micrometer‐sized NaO₂ discharge products in Na–O₂ batteries with carbon‐based air electrodes is reported. A detailed electrochemical charging mechanism is revealed during the charging process. The evolution of the chemical compositions of the discharge/side products in air electrode during charging is also verified by synchrotron‐based X‐ray absorption spectroscopy experiments. The formation of these intermediate phases other than NaO₂ during the charging process results in high overpotentials. These new findings can contribute to a better understanding and the rational design of future Na–O₂ batteries.     

Highly Improved Sb2S3 Sensitized‐Inorganic–Organic Heterojunction Solar Cells and Quantification of Traps by Deep‐Level Transient Spectroscopy

The light‐harvesting Sb₂S₃ surface on mesoporous‐TiO₂ in inorganic–organic heterojunction solar cells is sulfurized with thioacetamide (TA). The photovoltaic performances are compared before and after TA treatment, and the state of the Sb₂S₃ is investigated by X‐ray diffraction, X‐ray photoelectron spectroscopy, and deep‐level transient spectroscopy (DLTS). Although there are no differences in crystallinity and composition, the TA‐treated solar cells exhibit significantly enhanced performance compared to pristine Sb₂S₃‐sensitized solar cells. From DLTS analysis, the performance enhancement is mainly attributed to the extinction of trap sites, which are present at a density of (2–5) × 10¹⁴ cm^?3 in Sb₂S₃, by TA treatment. Through such a simple treatment, the cell records an overall power conversion efficiency (PCE) of 7.5% through a metal mask under simulated illumination (AM 1.5G, 100 mW cm^–2) with a very high open circuit voltage of 711.0 mV. This PCE is, thus far, the highest reported for fully solid‐state chalcogenide‐sensitized solar cells.     

Effect of Temperature and Illumination on the Electrical Characteristics of Polymer–Fullerene Bulk‐Heterojunction Solar Cells

The current–voltage characteristics of ITO/PEDOT:PSS/OC₁C₁₀‐PPV:PCBM/Al solar cells were measured in the temperature range 125–320 K under variable illumination, between 0.03 and 100 mW cm^–2 (white light), with the aim of determining the efficiency‐limiting mechanism(s) in these devices, and the temperature and/or illumination range(s) in which these devices demonstrate optimal performance. (ITO: indium tin oxide; PEDOT:PSS: poly(styrene sulfonate)‐doped poly(ethylene dioxythiophene); OC₁C₁₀‐PPV: poly[2‐methoxy‐5‐(3,7‐dimethyl octyloxy)‐1,4‐phenylene vinylene]; PCBM: phenyl‐C₆₁ butyric acid methyl ester.) The short‐circuit current density and the fill factor grow monotonically with temperature until 320 K. This is indicative of a thermally activated transport of photogenerated charge carriers, influenced by recombination with shallow traps. A gradual increase of the open‐circuit voltage to 0.91 V was observed upon cooling the devices down to 125 K. This fits the picture in which the open‐circuit voltage is not limited by the work‐function difference of electrode materials used. The overall effect of temperature on solar‐cell parameters results in a positive temperature coefficient of the power conversion efficiency, which is 1.9 % at T = 320 K and 100 mW cm^–2 (2.5 % at 0.7 mW cm^–2). The almost‐linear variation of the short‐circuit current density with light intensity confirms that the internal recombination losses are predominantly of monomolecular type under short‐circuit conditions. We present evidence that the efficiency of this type of solar cell is limited by a light‐dependent shunt resistance. Furthermore, the electronic transport properties of the absorber materials, e.g., low effective charge‐carrier mobility with a strong temperature dependence, limit the photogenerated current due to a high series resistance, therefore the active layer thickness must be kept low, which results in low absorption for this particular composite absorber.     

Highly Stretchable,High‐Mobility,Free‐Standing All‐Organic Transistors Modulated by Solid‐State Elastomer Electrolytes

Highly stretchable, high‐mobility, and free‐standing coplanar‐type all‐organic transistors based on deformable solid‐state elastomer electrolytes are demonstrated using ionic thermoplastic polyurethane (i‐TPU), thereby showing high reliability under mechanical stimuli as well as low‐voltage operation. Unlike conventional ionic dielectrics, the i‐TPU electrolyte prepared herein has remarkable characteristics, i.e., a large specific capacitance of 5.5 µF cm^?2, despite the low weight ratio (20 wt%) of the ionic liquid, high transparency, and even stretchability. These i‐TPU‐based organic transistors exhibit a mobility as high as 7.9 cm² V^?1 s^?1, high bendability (R_c, radius of curvature: 7.2 mm), and good stretchability (60% tensile strain). Moreover, they are suitable for low‐voltage operation (V_DS = ?1.0 V, V_GS = ?2.5 V). In addition, the electrical characteristics such as mobility, on‐current, and threshold voltage are maintained even in the concave and convex bending state (bending tensile strain of ≈3.4%), respectively. Finally, free‐standing, fully stretchable, and semi‐transparent coplanar‐type all‐organic transistors can be fabricated by introducing a poly(3,4‐ethylenedioxythiophene):polystyrene sulfonic acid layer as source/drain and gate electrodes, thus achieving low‐voltage operation (V_DS = ?1.5 V, V_GS = ?2.5 V) and an even higher mobility of up to 17.8 cm² V^?1 s^?1. Moreover, these devices withstand stretching up to 80% tensile strain.     

Single‐Atom Fe‐Nx‐C as an Efficient Electrocatalyst for Zinc–Air Batteries

Highly efficient non‐noble metal electrocatalysts are vital for metal–air batteries and fuel cells. Herein, a noble‐metal–free single‐atom Fe‐N _x‐C electrocatalyst is synthesized by incorporating Fe‐Phen complexes into the nanocages in situ during the growth of ZIF‐8, followed by pyrolysis at 900 °C under inert atmosphere. Fe‐Phen species provide both Fe²⁺ and the organic ligand (Phen) simultaneously, which play significant roles in preparing single‐atom catalysts. The obtained Fe‐N_x‐C exhibits a half‐wave potential of 0.91 V for the oxygen reduction reaction, higher than that of commercial Pt/C (0.82 V). As a cathode catalyst for primary zinc–air batteries (ZABs), the battery shows excellent electrochemical performances in terms of the high open‐circuit voltage (OCV) of 1.51 V and a high power density of 96.4 mW cm^?2. The rechargeable ZAB with Fe‐N_x‐C catalyst and the alkaline electrolyte shows a remarkable cycling performance for 300 h with an initial round‐trip efficiency of 59.6%. Furthermore, the rechargeable all‐solid‐state ZABs with the Fe‐N_x‐C catalyst show high OCV of 1.49 V, long cycle life for 120 h, and foldability. The single‐atom Fe‐N_x‐C electrocatalyst may function as a promising catalyst for various metal–air batteries and fuel cells.