Cathode Design Research Articles

Research Progress on Novel Electrochemical Descaling Technology for Enhanced Hardness Ion Removal

In recent years, electrochemical descaling technology has gained widespread attention due to its environmental friendliness and ease of operation. However, its single-pass removal efficiency could be higher, severely limiting its practical application. To overcome the limitations of traditional electrochemical descaling processes, this paper first focuses on the separation efficiency of H+ and OH− in the scale removal process based on numerous recent research papers. It mainly emphasizes how innovative cathode design can enhance the efficiency and stability of electrochemical descaling. Furthermore, this paper explores the coupling of electrochemical processes with different water treatment technologies, such as the combination of electrodeposition with electrocoagulation, filtration crystallization, microfiltration, and electrodialysis, and how these methods synergistically enhance descaling effects. Additionally, this paper discusses potential future directions for electrochemical descaling technology, including innovations in scale expansion, material updates, process optimization, system integration, and automation. Finally, this paper analyzes the practical challenges of electrochemical descaling technology, such as cost, energy consumption, equipment durability, and environmental impact, and proposes solutions. The implementation of these strategies is expected to promote the commercialization of electrochemical descaling technology, making it more aligned with the sustainability requirements of industry and the environment.

Highly active and robust A-site deficient La0.77Sr0.2Co0.2Fe0.8O3-δ fiber base electrode for intermediate temperature solid oxide cells

The combination of solid oxide electrolysis cells (SOECs) and solid oxide fuel cells (SOFCs) is expected to solve the problems of energy conversion and storage. However, the insufficient catalytic capacity and poor durability of the oxygen electrodes in solid oxide cells (SOCs) at intermediate temperatures pose a huge challenge for SOCs applications. In this work, A-site deficient La0.77Sr0.2Co0.2Fe0.8O3-δ nanorod materials coated with Ce0.8Gd0.2O1.9 (GDC) are prepared to suppress cation surface segregation and enhance charge transfer kinetics by reducing internal elastic force of perovskite and meanwhile applying external compressive stress with an oxygen-ion conductor. As a result, the composite cathode with a GDC to La0.77Sr0.2Co0.2Fe0.8O3-δ weight ratio of 0.59 (La0.77Sr0.2Co0.2Fe0.8O3-δ@GDC0.59) exhibits excellent electrochemical performance and long-term stability when operating in both SOFCs and SOECs modes. XPS results show that the La0.77Sr0.2Co0.2Fe0.8O3-δ@GDC0.59 oxygen electrode exhibits no significant Sr/Fe surface segregation after operating in SOFCs and SOECs modes for 200 h. Density functional theory calculation and physiochemical characterization confirm that Sr segregation phenomenon is well inhibited through the novel A-site deficient structural design of perovskite materials, which eliminates the major residual internal elastic force of La0.8Sr0.2Co0.2Fe0.8O3-δ crystal, and GDC coating further relieves the lattice transformation of La0.77Sr0.2Co0.2Fe0.8O3-δ upon the additional introduction of A-site deficiency and oxygen vacancy. This well-orchestrated composite cathode design provides a new perspective in stabilizing perovskite crystalline structure toward high-performance SOCs with extended operating life.

Construction of integrated oxygen-rich carbon-based metal-free cathode to simultaneous boost wastewater treatment performance and energy recovery in bio-electro-Fenton system

Fenton coupled microbial fuel cells (MFCs) used for antibiotic pollution purification are limited by energy recovery and metal leakage of electrode. Here, we constructed a two-compartment bio-electro-Fenton (MFC-Fenton) with biological anode and Fenton cathode, which using carbon nanotube based on carbon brushes (OCNT-80/CB) with active centers rich in oxygen-containing functional groups as metal-free cathode. The results show that C = O locked environmental oxygen in the cathode can in-situ use the electrons produced by the anode through two-electron oxygen reduction reaction (2e− ORR) synthesize H2O2. •OH is further generated under activation of H2O2, achieving effective degradation of tetracycline (TC) in the cathode chamber. This study breaks through the limitations of poor pH adaptability and environmental secondary pollution caused by metal dissolution. Moreover, with the advantageous features of oxygen-containing functional groups active centers, good conductivity, and cyclic stability, the OCNT-80/CB achieves a maximum power density increased by 79.4 % as compared to that of the CB control. More notably, Microbial analysis further indicated that OCNT-80/CB electrode could simultaneously enhance Proteobacteria and Firmicutes abundance in bioanode. Dominant bacteria can self-metabolize environmental wastewater generate and recycle green energy. This study proved that careful structural design of cathode could promote the electrode performance. MFC-Fenton can be a competitive technology to enhance wastewater treatment and energy recovery simultaneously.

A Freestanding, Dissolution- and Diffusion-Limiting, Flexible Sulfur Electrode Enables High Specific Capacity at High Mass Loading.

The acquisition of stable and high-areal-capacity S cathodes over 10mA h cm-2 is a critical and indispensable step to realize the high energy density configuration. However, increasing the areal capacity of S cathodes often deteriorates the specific capacity and stability due to the aggravated dissolution of S and diffusion of solvable polysulfides in the thick electrode. Herein, the design of a freestanding composite cathode that leverages 3D covalent binding sites and chemical adsorption environment to offer dissolution-limiting and diffusion-blocking functions of S species is reported. By employing this architecture, the coin cell exhibits excellent cycling stability and an exceptional specific capacity of 1444.3mA h g-1 (13mA h cm-2), and the pouch cell configuration manifests a noteworthy areal capacity exceeding 11mA h cm-2. This performance is coupled with excellent flexibility, demonstrated through consecutive bending cycle tests, even at a sulfur loading of 9.00mg cm-2. This study lays the foundation for the development of flexible Li-S batteries with increased loading capacities and exceptional performance.

Bifunctional Potential Structure Design Breaks Electrolyte Limitations of Zinc Ion Battery

AbstractAqueous zinc‐ion batteries (ZIBs) are safe and economical for grid applications. However, current ZIBs have limitations in terms of inferior capacity and low output voltage, which are hampered by the electrolyte applicability of the Zn2+ hosts. In this study, we propose a novel organic cathode design strategy with a bifunctional potential region. This polymeric Zn2+ host combines the conjugated polyaniline backbone to tune the molecular surface pH and [Fe(CN)6]3−/4− redox couple for high output voltage and capacity. The polyaniline doped with ferricyanide (PAF) electrode exhibits two forms of charge storage in ZIBs: proton‐assisted Zn2+ doping below 1.2 V (mechanism I), and [Fe(CN)6]3−/4− redox pair above 1.8 V (mechanism II). Density functional theory calculations and in situ pH experiments demonstrated that the H+ doping process of mechanism I forms a localized pH regulation on the molecular chain surface, providing a favorable reaction environment for mechanism II. The Zn‐polymer battery delivered an outstanding discharge capacity (405.2 mAh g−1) and high output voltage (1.8 V) in the Zn(CF3SO3)2 electrolyte. This study provides a new route for enhancing the structural stability of electrodes and overcoming the electrolyte limitations of ferricyanide in weakly acidic electrolytes.

Bifunctional Potential Structure Design Breaks Electrolyte Limitations of Zinc Ion Battery.

Aqueous zinc-ion batteries (ZIBs) are safe and economical for grid applications. However, current ZIBs have limitations in terms of inferior capacity and low output voltage, which are hampered by the electrolyte applicability of the Zn2+ hosts. In this study, we propose a novel organic cathode design strategy with a bifunctional potential region. This polymeric Zn2+ host combines the conjugated polyaniline backbone to tune the molecular surface pH and [Fe(CN)6]3-/4- redox couple for high output voltage and capacity. The polyaniline doped with ferricyanide (PAF) electrode exhibits two forms of charge storage in ZIBs: proton-assisted Zn2+ doping below 1.2 V (mechanism I), and [Fe(CN)6]3-/4- redox pair above 1.8 V (mechanism II). Density functional theory calculations and in situ pH experiments demonstrated that the H+ doping process of mechanism I forms a localized pH regulation on the molecular chain surface, providing a favorable reaction environment for mechanism II. The Zn-polymer battery delivered an outstanding discharge capacity (405.2 mAh g-1) and high output voltage (1.8 V) in the Zn(CF3SO3)2 electrolyte. This study provides a new route for enhancing the structural stability of electrodes and overcoming the electrolyte limitations of ferricyanide in weakly acidic electrolytes.

Spatial Structure Design of Thioether-Linked Naphthoquinone Cathodes for High-Performance Aqueous Zinc-Organic Batteries.

Organic electrode materials (OEMs) have gathered extensive attention for aqueous zinc-ion batteries (AZIBs) due to their structural diversity and molecular designability. However, the reported research mainly focuses on the design of the planar configuration of OEMs and does not take into account the important influence of the spatial structure on the electrochemical properties, which seriously hamper the further performance liberation of OEMs. Herein, this work has designed a series of thioether-linked naphthoquinone-derived isomers with tunable spatial structures and applied them as the cathodes in AZIBs. The incomplete conjugated structure of the elaborately engineered isomers can guarantee the independence of the redox reaction of active groups, which contributes to the full utilization of active sites and high redox reversibility. In addition, the position isomerization of naphthoquinones on the benzene rings changes the zincophilic activity and redox kinetics of the isomers, signifying the importance of spatial structure on the electrochemical performance. As a result, the 2,2'-(1,4-phenylenedithio) bis(1,4-naphthoquinone) (p-PNQ) with the smallest steric hindrance and the most independent redox of active sites exhibits a high specific capacity (279 mAh g-1 ), an outstanding rate capability (167 mAh g-1 at 100 A g-1 ), and a long-term cycling lifetime (over 2800h at 0.05 A g-1 ).

Boosting the power density of Zr and Ni co-doped BaFeO3 cathode for proton-conducing solid oxide fuel cells

A novel cathode material, denoted as BaZr0.26Fe0.64Ni0.1O3-δ (BZFN010), has been suggested for application in proton-conducting solid oxide fuel cells (H-SOFCs), aiming to enhance electrochemical performance. The introduction of Zr into the original BaFeO3-δ (BFO) results in improved chemical stability against CO2. However, despite this enhancement, the electrochemical performance remains unsatisfactory. Hence, we leveraged the outstanding stability of BZF and incorporated Ni, a well-known element renowned for its remarkable catalytic qualities, into the cell to augment its properties. This enhancement is substantiated by a combination of experimental and theoretical calculations. When employed as a cathode, the BZFN010 material exhibited markedly superior performance compared to the BaZr0.36Fe0.54O3 (BZF36) cathode. It demonstrated a 57% increase in power density, rising from 998 mW cm-2 to 1570 mW cm-2 at 700 °C. This study employs a chained-style cathode exploration strategy, commencing with the conventional BFO cathode, progressing to the enhanced stability of BZF36, and culminating in the optimized catalytic activity of BZFN010. Our work represents an intriguing strategy for the design of H-SOFC cathodes.

Theoretical exploration of photoemission characteristics of GaAs nanowire array cathode based on photon-enhanced thermionic emission

The theoretical photoemission models of single GaAs nanowire and nanowire array cathode based on photon-enhanced thermionic emission (PETE) mechanism are respectively developed by utilizing two-dimensional continuity equations. Based on the built models in this work, the effect of several key factors on the quantum efficiency are also discussed. Results show that GaAs nanowire cathode exhibits the superiority of photoemission performance compared with GaAs film cathode at the spectral range of 300∼600 nm. Besides, the optimal wire diameter of GaAs nanowire cathode is in the range of 340∼360 nm. In addition, the nanowire cathode with low electron affinity of 0.3 eV achieves PETE effect under low temperature of 400 K, which is conducive to improve the stability of cathode. Moreover, increasing the incident light angle or decreasing the array spacing provides an effective method of obtaining high quantum efficiency of nanowire array cathode. Furthermore, the numerical difference between quantum efficiency and effective quantum efficiency implies that the low collection efficiency of emitted electrons is the main issue that hinders the application of PETE cathodes of GaAs nanowire array. The proposed GaAs nanowire array model would provide theoretical guidance for optimum design of PETE cathodes with nanoarray structure.

Customizing polymeric binders for advanced lithium batteries: Design principles and beyond

As society strides toward a sustainable future powered by lithium-ion batteries, the integral role of polymeric binders becomes increasingly evident. Historically serving as a film former and chemical adhesive that amalgamates the active host materials and conductive carbon in battery electrodes, their role has been redefined with the advent of innovative battery systems and host materials. These emerging technologies pose unique challenges, propelling the shift toward “customizable” binder designs. Polymeric binders should now ensure structural robustness, especially for high-capacity host materials, by leveraging varied intermolecular interactions to counteract internal stresses. Additionally, incorporating high-voltage electrode materials or electrolytes demands binders with an expansive electrochemical stability window. The interface energy control of binders is also critical, especially when incorporating dissolving cathodes or transitioning to solid-state electrolytes. This review provides a comprehensive understanding, breaking down the design principles of polymeric binders into three distinct paradigms: (1) structural design for high-capacity anodes, (2) electrochemical design for high-voltage cathodes or electrolytes, and (3) interfacial design for dissolving cathodes and solid-state batteries. Our discourse offers both a reflection on the evolving multifunctional nature of binders and a roadmap for future endeavors in the binder design for advanced lithium battery chemistries.

A global model for evaluating discharge characteristics and performance of hollow cathodes

Hollow cathode, with the highest plasma density, current density, and temperature, becomes one of the most important components in the electro-thruster system. As the electric-propulsion thruster performance is directly related to the ionization rate, reliability, and lifetime of the hollow cathode, this paper develops a global model to study the effects of discharge current, gas flow rate, and gas species on the discharge characteristics in the insert and orifice regions of the hollow cathode. The emitter wall temperatures of hollow cathodes predicted by the global model are compared with experimental results from NSTAR thruster neutralization cathodes, confirming the model's validity. The influence of hollow cathode emitter material and structure sizes on the plasma parameters in the internal regions was also evaluated. The simulation results show that there is an optimal matching relationship between the discharge current and gas flow rate to guarantee the maximum ionization rate. The optimal working region for the hollow cathode has been determined under different energetic, regime and structural parameters. The global model established in this paper can quickly determine the key structure and operating parameters of hollow cathode at the design stage, and provide the theoretical basis for hollow cathode design and development.

High performance all-solid-state Li–Se battery based on selenium loaded on Ti3C2 MXene cathode

Selenium has high theoretical volumetric capacity of 3253 mAh cm−3 and acceptable electronic conductivity of 1 × 10−5 S m−1, which is considered as a potential alternative to sulfur cathode for all-solid-state rechargeable batteries with high energy density. However, the development of all-solid-state Li–Se batteries (ASSLSBs) are hindered by sluggish kinetics and poor cycling life. In this work, trigonal Se nanocrystallines are homogenously distributed in the interspace and on the surface of MXene layers (denoted as Se@MXene composite) by a novel melt-diffusion method. ASSLSBs based on this Se@MXene composite cathode exhibit large specific capacity of 632 mAh g−1 at 0.05 A g−1, high-rate capability over 4 A g−1, and excellent cycling stability over 300 cycles at 1 A g−1. The ex-situ analytical techniques demonstrate that the excellent electrochemical performance of Se@MXene cathode largely arises from structural stability with the assistance of conductive MXene and reversible redox behavior between Li2Se and Se during the repeating charge/discharge process. Our study points out the potential of material design of Se cathode based on conducting 2D materials with good electrochemical behavior, which may accelerate the practicability of ASSLSBs.

Unique insights into the design of low-strain single-crystalline Ni-rich cathodes with superior cycling stability

Micro-sized single-crystalline Ni-rich cathodes are emerging as prominent candidates owing to their larger compact density and higher safety compared with poly-crystalline counterparts, yet the uneven stress distribution and lattice oxygen loss result in the intragranular crack generation and planar gliding. Herein, taking LiNi0.83Co0.12Mn0.05O2 as an example, an optimal particle size of 3.7 µm is predicted by simulating the stress distributions at various states of charge and their relationship with fracture free-energy, and then, the fitted curves of particle size with calcination temperature and time are further built, which guides the successful synthesis of target-sized particles (m-NCM83) with highly ordered layered structure by a unique high-temperature short-duration pulse lithiation strategy. The m-NCM83 significantly reduces strain energy, Li/O loss, and cationic mixing, thereby inhibiting crack formation, planar gliding, and surface degradation. Accordingly, the m-NCM83 exhibits superior cycling stability with highly structural integrity and dual-doped m-NCM83 further shows excellent 88.1% capacity retention.

Fabrication of cathode composite Co3O4/CC and study on electrochemical properties of zinc cobalt battery

Purpose Aqueous zinc-ion battery has broad application prospects in smart grid energy storage, power tools and other fields. Co3O4 is one of the ideal cathode materials for water zinc-ion batteries due to their high theoretical capacity, simple synthesis, low cost and environmental friendliness. Many studies were concentrated on the synthesis, design and doping of cathodes, but the effect of process parameters on morphology and performance was rarely reported. Design/methodology/approach Herein, Co3O4 cathode material based on carbon cloth (Co3O4/CC) was prepared by different temperatures hydrothermal synthesis method. The temperatures of hydrothermal reaction are 100°C, 120°C, 130°C and 140°C, respectively. The influence of temperatures on the microstructures of the cathodes and electrochemical performance of zinc ion batteries were investigated by X-ray diffraction analysis, scanning electron microscopy, cyclic voltammetry curve, electrochemical charging and discharging behavior and electrochemical impedance spectroscopy test. Findings The results show that the Co3O4/CC material synthesized at 120°C has good performance. Co3O4/CC nanowire has a uniform distribution, regular surface and small size on carbon cloth. The zinc-ion battery has excellent rate performance and low reaction resistance. In the voltage range of 0.01–2.2 V, when the current density is 1 A/g, the specific capacity of the battery is 108.2 mAh/g for the first discharge and the specific capacity of the battery is 142.6 mAh/g after 60 charge and discharge cycles. Originality/value The study aims to investigate the effect of process parameters on the performance of zinc-ion batteries systematically and optimized applicable reaction temperature.

Synergistic Fe and Co binary single atoms based air cathodes for high performance and ultra-stable Zn-air batteries

Cost-effective highly efficient and stable air cathodes are critical for practical applications of rechargeable Zn-air batteries (ZABs). In this work, air cathodes constructed by loading carbon nanotube supported N-doped carbon anchored Fe and Co binary single atoms, f-Fe1Co1/CNT, in carbon paper composited nickel foams, NF/CP, were developed for ZABs, exhibiting outstanding bifunctional oxygen electrocatalytic activities (ΔE = 0.671 V) with a half-wave potential (E1/2) of 0.880 V (vs. RHE) for oxygen reduction reaction (ORR) and an overpotential of 321 mV at 10 mA cm−2 (η10) for oxygen evolution reaction (OER) in 0.1 M KOH, which outperformed the benchmark (Pt/C+IrO2)-based air cathode (ΔE = 0.773 V, E1/2 = 0.850 V, η10 = 393 mV). With the unique air cathode design of compositing catalyst-loading layer (nickel foam) with gas diffusion layer (carbon paper), the f-Fe1Co1/CNT@NF/CP//Zn ZAB delivered a remarkable discharge peak power density of 282.1 mW cm−2 at an ultra-high current density of 427.7 mA cm−2 and maintained an ultra-small potential gap of 0.75 V after operations at 10 mA cm−2 for 3300 cycles (1100 h), largely outperforming the (Pt/C+IrO2)@NF/CP//Zn ZAB (162.4 mW cm−2 at 247.3 mA cm−2, 0.86 V, 590 cycles). Density functional theory calculations revealed the positive long-range synergy between Fe-N4 and Co-N4 single atoms, significantly reducing the free energies of the rate-determining steps, oxygen protonation for ORR and formation of oxyhydroxides for OER at the main active site Fe-N4, to realize the much enhanced oxygen electrocatalytic activities.

New Scalable Sulfur Cathode Containing Specifically Designed Polysulfide Adsorbing Materials.

Because of its considerable theoretical specific capacity and energy density, lithium-sulfur battery technology holds great potential to replace lithium-ion battery technology. However, a versatile, low-cost, and easily scalable bulk synthesis method is essential for translating bench-level development to large-scale production. This paper reports the design and synthesis of a new scalable sulfur cathode, S@CNT/PANI/PPyNT/TiO2 (BTX). The rationally chosen cathode components suppress the migration of polysulfide intermediates via chemical interactions, enhance redox kinetics, and provide electrical conductivity to sulfur, rendering outstanding long-term cycling performance and strong initial specific capacity in terms of electrochemical performance. This cathode's cell demonstrated an initial specific capacity of 740 mA h g-1 at 0.2 C (with a capacity decay rate of 0.08% per cycle after 450 cycles).

Unravelling the peculiar role of Co and Al in highly Ni-rich layered oxide cathode materials

Currently, the limited availability of cobalt resources has had a negative impact on the progress of commercial batteries, prompting the development of cobalt-free Ni-rich cathodes. However, the complete replacement of cobalt has faced challenges due to the lack of understanding the influence of dopants on cathode material performance. In this study, we aimed to address this knowledge gap by designing and preparing LiNi0.95Co0.05-xAlxO2 (x = 0.00, 0.01, 0.02, 0.03, 0.04, and 0.05) cathode materials. The impact of cobalt and aluminum doping on the morphology, crystallographic structure and electrothermal performance of Ni-rich cathode materials has been systematically investigated. Our findings confirmed the significant role of cobalt in increasing energy density and mitigating cationic disordering. However, it is found that cobalt doping contributes to the release of lattice oxygen during cycling, leading to rapid capacity fading. Conversely, aluminum doping could stabilize the crystal structure of the cathode material, resulting in slower capacity degradation. Furthermore, the substitution of aluminum effectively mitigates the crystal growth during the synthesis of highly Ni-rich cathode materials, leading to a reduced Li+ diffusion length and thereby excellent rate performance. Specifically, LiNi0.95Al0.05O2 could deliver a high discharge capacity of around 163 mAh g−1 at 10C. This study provides valuable insights for the design of cobalt-free Ni-rich cathodes and sheds light on the possibility of cobalt elimination.

Tailoring Cu-rich surface spinel phase for high-performance O3-type layered cathode materials for sodium-ion batteries

O3-type layered oxide cathodes are primarily limited by complex phase transitions and sluggish kinetics resulting in rapid capacity drop and poor rate capability. Even worse, its inherent air sensitivity leads to spontaneous extraction of lattice Na-ions and the deactivation of the cathode. Simultaneous modification of both the bulk phase and the surface structure is promising to offset the above deficiencies. A spinel@O3 type layered composite structure Na0.9Mn0.5Ni0.5Cu0.1O2+x (NMNCO-SL) was constructed for the design of cathodes with higher cycling, rate and air stability. The atomic-level Cu-rich spinel structure on the surface was identified by scanning transmission electron microscopy, elemental linear scanning analysis and Raman spectra. In situ charge-discharge X-ray diffraction results show that the phase transition of NMNCO-SL is significantly suppressed. Finally, the material maintains good electrochemical properties after exposure to stringent humidity environments. The results indicate that the spinel structure at the surface plays a significant role in improving ion-diffusion dynamics, enhancing structural integrity, and increasing air stability. 1 Ah pouch cell based on NMNCO-SL showed 92% capacity retention after 500 cycles of charge/discharge cycling at 1 C, demonstrating the potential prospects of customizing the surface phase structure for materials engineering applications.

Bipolar Current Collectors of Cu/polymer/Al Composite for Anode‐Free Batteries

AbstractThe all‐in‐one design of cathode and anode is a promising strategy to improve energy density and assembly efficiency for lithium batteries. However, it is an important prerequisite to combine negative and positive current collectors in a single sheet. Here, an asymmetric structure of bipolar composite current collector (BCCC), thin copper (Cu) and aluminum (Al) metal layers respectively deposited on each side of a thin polyethylene terephthalate (PET) polymer substrate is developed. Unlike conventional metal foils, the electronically insulative polymer blocks electron transfer between the cathode and anode coated on each side of BCCC. Buckling‐based mechanics measurement and molecular simulation are conducted to quantitatively evaluate the interfacial strength of metal/polymer, which is enhanced by introducing an intermediate chromium (Cr) layer. For applications in anode‐free wound batteries, the integrated sheet of separator/cathode/BCCC can simplify the alignment of the electrodes during the winding process. Without special surface and electrolyte optimizations, a higher Coulombic efficiency (99.1%) and larger capacity retention (50.0%) are achieved after 100 cycles in the LiNi0.8Co0.1Mn0.1O2 anode‐free battery than the battery using Cu foils.

Aerobically Autoxidized Self-Charge Concept Derived from Synergistic Pyrrolic Nitrogen and Catechol Configurations in N, O Co-Doped Carbon Cathode Material.

Aerobically autoxidized self-charging concept has drawn significant attraction due to its promising chemical charge features without external power supply. Particularly, heteroatom-doped carbon materials with abundant oxidizable sites and good conductivity are expected to be ideal cathode materials. However, there is no well-defined aerobically autoxidized self-charging concept based on heteroatom-doped carbon materials, significantly hindering the design of related carbon cathodes. An aerobically autoxidized self-chargeable concept derived from synergistic effect of pyrrolic nitrogen and catechol configuration in carbon cathode using model single pyrrolic nitrogen and oxygen (N-5, O) co-doped carbon and O-enriched carbon is proposed. First, self-charging of N-5, O co-doped carbon cathode can be achieved by aerobic oxidation of pyrrolic nitrogen and catechol to oxidized pyrrolic nitrogen and ortho-quinone configurations, respectively. Second, introducing a single pyrrolic nitrogen configuration enhanced acidic wettability of N-5, O co-doped carbon facilitating air self-charge/galvanic discharge involving proton removal/introduction. Third, synergistic effect of pyrrolic nitrogen and hydroxyl species with the strong electron-donating ability to conjugated carbon-based backbone endows N-5, O co-doped carbon with a higher highest occupied molecular orbital (HOMO) energy level more susceptible to oxidation charging. The assembled Cu/Carbon batteries can drive a timer after every air-charging run. This promising aerobically autoxidized self-charging concept can inspire exploring high-efficiency self-charging devices.