High Peak Power Density Research Articles

Silver decorated cobalt carbonate to enable high bifunctional activity for oxygen electrocatalysis and rechargeable Zn-air batteries

Rechargeable zinc–air batteries (ZABs) is primarily driven by the couple of oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Currently,it is still challenging to develop cost-effective, highly efficient, and robust bifunctional catalysts for ZABs. Herein, a novel silver decorated cobalt carbonate (Ag@CoCO3) hybrid catalyst is proposed as the potential bifunctional catalyst to drive OER and ORR for ZABs. Engineering Ag nanoparticles onto the surface of CoCO3 microsphere not only facilitates the charge transfer, but also modulates the electronic structure, which are beneficial to intrinsic bifunctional activity. As a result, this Ag@CoCO3 catalyst yields a substantially enhanced bifunctionality compared to the pristine CoCO3 catalyst. Moreover, the homemade Ag@CoCO3 based ZABs provides a high peak power density of 146 mW cm−2, superior to 107 mW cm−2 for CoCO3 based ZABs and 111 mW cm−2 for commercial Pt/C-IrO2 based ZABs.

Iron polyphthalocyanine-derived ternary-balanced Fe3O4/Fe3N/Fe-N-C@PC as a high-performance electrocatalyst for the oxygen reduction reaction

The oxygen reduction reaction (ORR) is the cornerstone reaction of the cathode in metal-air batteries; however, slow kinetics requires high-performance catalysts to promote the reaction. Polyphthalocyanine (PPc) has a typical chemical cross-linking structure and uniformly dispersed metal active sites, but its poor activity and conductivity limit its applications as an ORR catalyst. Herein, a manageable and convenient strategy is proposed to synthesize ternary ORR catalysts through the low-temperature pyrolysis of FePPc. The optimal catalyst, Fe3O4/Fe3N/Fe-N-C@PC-2.5, exhibits excellent ORR activity in alkaline solution with a half-wave potential of 0.90 V, which is significantly higher than that of commercial 20% Pt/C (0.84 V). Electrochemical tests and extended X-ray absorption fine structure spectroscopy reveal that the superior ORR activity of Fe3O4/Fe3N/Fe-N-C@PC-2.5 could be ascribed to the balance of its ternary components (i.e., Fe3O4, Fe3N, and Fe-N4 species). A Zn-air battery incorporating Fe3O4/Fe3N/Fe-N-C@PC-2.5 as an air cathodic catalyst delivers a high open-circuit voltage and peak power density. During galvanostatic discharge, the battery demonstrates a specific capacity of 815.7 mA h g−1. The facile strategy of using PPc to develop high performance composite electrocatalysts may be expanded to develop new types of catalysts in the energy field.

Thermal Engineering of NiCo‐Codoped Carbon Nanofibers toward Enhanced Oxygen Electrocatalysis for Zn–Air Batteries

Electrospinning is an efficient and facile method to prepare carbon nanofibers (CFs) embedded with a NiCo alloy as efficient oxygen electrocatalysts for Zn–air batteries. The subsequent pyrolysis of electrospun‐woven is significant to the crystallization degree of CFs and NiCo alloy. Herein, the effect of the crystallization degree of the alloy and carbon on the oxygen electrocatalytic activity is explored through controlled thermal engineering (the annealing temperature). As the temperature increases, the degree of crystallization and agglomeration of nanoparticles increases simultaneously, accompanied by the increase of the graphitization degree of CFs. Among all the samples, NiCo/CF‐800 exhibits the best oxygen bifunctional catalytic activity (ΔE = 0.73 V). A Zn–air battery based on the NiCo/CF‐800 catalyst exhibits a high peak power density (168.6 mW cm−2), high specific capacity (802.6 mA h gZn−1), and excellent charge/discharge cycling stability. This work provides new insight into catalysts through thermal engineering, promoting the practical application of electrospinning as a large‐scale production method.

Self-Anchored Platinum-Decorated Antimony-Doped-Tin Oxide as a Durable Oxygen Reduction Electrocatalyst

The lifetime of commercial proton exchange membrane fuel cells (PEMFCs) is circumscribed by the insufficient durability of commercial catalysts. The use of metal oxide supports in place of carbon significantly increases electrocatalyst durability. Herein, following density functional theory predictions of improved platinum (Pt) stability on antimony-doped tin oxide (ATO) supports, we synthesized ATO whose morphology and crystal structure were engineered using a Pt-anchoring technique. X-ray photoelectron spectroscopy indicated that the Pt anchor sites aided in the reduction of Pt precursors to Pt on the ATO surface. X-ray absorption near-edge spectroscopy revealed the existence of strong metal–support interactions (SMSIs) between Pt and ATO. The combination of SMSIs and high control over Pt dispersion enabled the Pt/Pt-aerogel-ATO (Pt supported on aerogel ATO with Pt anchor sites) electrocatalyst to achieve 2 × the area-specific activity of Pt/C in ex situ testing. In a H2/air PEMFC, Pt/Pt-aerogel-ATO cathodes enabled 20% higher peak power density and <1/6 the loss of active surface area as compared to Pt/C. In a PEMFC under rigorous potential cycling, the Pt/Pt-aerogel-ATO retained its initial peak power density as opposed to a 58% loss for Pt/C. Furthermore, cost models indicate that Pt/Pt-aerogel-ATO is 26% less expensive than Pt/C over its useful lifetime.

Double boosting single atom Fe–N4 sites for high efficiency O2 and CO2 electroreduction

Metal-N4 single-atom catalysts have emerged as the frontier of catalysis. However, the low metal loading and abundance of single atoms embedded in carbon skeleton hinder their practical application. Herein, we report an effective “trapping and exposing” strategy for constructing single-atom Fe–N4 catalysts with high density of single-atom active sites. The strategy involves the strong binding of metal ions to sucrose (trapping) to prevent the migration and agglomeration of Fe3+, followed by the introduction of a mesoporous structure using an SBA-15 template to achieve sufficient exposure of the Fe–N4 sites (exposing). The as-prepared catalyst comprises Fe–N4 moieties (10.8 wt%) with a hierarchical structure. Density functional theory calculations reveal that the chelating reaction between sucrose and Fe3+ ions has a low free energy, resulting in the formation of highly dispersed Fe–N4 single atoms. The single-atom catalyst displays a high peak power density of 0.784 W cm−2 in a H2–O2 proton exchange membrane fuel cell and achieves an impressive CO current density of 109 A g−1 at negligible overpotentials in a flow cell. This work provides an efficient strategy for designing high-performance single-atom catalysts for practical electrocatalysis applications.

N-doped carbon nanosheets with ultra-high specific surface area for boosting oxygen reduction reaction in Zn-air batteries

When designing carbon-based electrocatalysts as Pt-free catalysts for the oxygen reduction reaction (ORR), pore structures is crucial, in addition to creating active sites. Here, N-doped carbon nanosheets were rationally designed by tactfully introducing nitrogen source into the carbonization process, which could increase the density of pore structures and effective active sites. Owing to the ultra-high specific surface area (2127 m2 g−1), large pore volume (5.77 cm3 g−1), and bimodal-pore structure (micropores and mesopores), the optimized catalyst exhibited an excellent ORR activity (a half-wave potential of 0.86 V), as well as outstanding durability and methanol tolerance in alkaline medium. Moreover, it provided excellent stability and high peak power density when used as ORR catalyst in Zn-air battery, exceeding that driven by Pt/C catalyst. This work brings a feasible and universal strategy for fabricating metal-free ORR catalysts.

ZIF-derived two-dimensional Co@Carbon hybrid: Toward highly efficient trifunctional electrocatalysts

Hybrid electrocatalysts with stable two-dimensional (2D) framework and fine sub-structures are of great interest for enhancing the mass/electron transport and accessibility of maximized active sites. Here, we report a facile 2D-ZIF transformation strategy for fabricating highly efficient hybrid catalysts composed of highly dispersed Co quantum dots (~4.57 nm in diameter) embedded in ultrathin N-doped carbon layers (~3 nm in thickness), denoted as Co@NCL. The as-fabricated hybrids have excellent overall trifunctional electrocatalytic activities toward oxygen reduction (half-wave potential (E1/2) = 0.84 V), oxygen evolution (potential at 10 mA cm−2 (Ej10) = 1.63 V), and hydrogen evolution (Ej10 = −0.22 V) reactions in alkaline media. Notably, its reversible oxygen electrode index (ΔE = Ej10 − E1/2 = 0.79 V) is comparable with that of benchmarked noble-metal catalysts (0.80 V for Pt/C-RuO2) and superior to ZIF polyhedrons-derived counterpart (0.90 V) as well as most Co-based bifunctional catalysts ever reported. The as-constructed Zn–air battery and overall water splitting electrolyzer based on Co@NCL delivered a high peak power density of 170 mW cm−2 and a small voltage of 1.70 V that affords a current density of 10 mA cm−2 along with robust long-term stability, respectively, which demonstrates its promising applications in rechargeable metal-air batteries and water splitting.

Aluminum-air battery with cotton substrate: Controlling the discharge capacity by electrolyte pre-deposition

Conventional Al-air battery has many disadvantages for miniwatt applications, such as the complex water management, bulky electrolyte storage and potential leakage hazard. Moreover, the self-corrosion of Al anode continues even when the electrolyte flow is stopped, leading to great Al waste. To tackle these issues, an innovative cotton-based aluminum-air battery is developed in this study. Instead of flowing alkaline solution, cotton substrate pre-deposited with solid alkaline is used, together with a small water reservoir to continuously wet the cotton and dissolve the alkaline in-situ. In this manner, the battery can be mechanically recharged by replacing the cotton substrate and refilling the water reservoir, while the thick aluminum anode can be reused for tens of times until complete consumption. The cotton substrate shows excellent ability for the storage and transportation of alkaline electrolyte, leading to a high peak power density of 73 mW cm−2 and a high specific energy of 930 mW h g−1. Moreover, the battery discharge capacity is found to be linear to the loading of pre-deposited alkaline, so that it can be precisely controlled according to the mission profile to avoid Al waste. Finally, a two-cell battery pack with common water reservoir is developed, which can provide a voltage of 2.7 V and a power output of 223.8 mW. With further scaling-up and stacking, this cotton-based Al-air battery system with low cost and high energy density is very promising for recharging miniwatt electronics in the outdoor environment.

Porous N, B co-doped carbon nanotubes as efficient metal-free electrocatalysts for ORR and Zn-air batteries

The flexible design and construction of oxygen reduction reaction (ORR) catalysts with high activity, great stability, and superior cost efficiency are essential for metal-air batteries and fuel cells. Hollow carbon nanotubes (CNTs) are considered promising electrocatalysts owing to their outstanding thermal stability, robust chemical properties, and high specific surface area. Herein, a convenient and controllable solid-phase route is proposed for the preparation of porous nitrogen (N) and boron (B) co-doped carbon nanotubes (NBCNT) by using tubular polypyrrole (PPy) and sodium tetraphenylboron ((C6H5)4BNa), in which (C6H5)4BNa serves not only as a B source but also as a pore-forming agent that can help to regulate N configuration and expose more active sites. Due to the synergistic effects of porous one-dimensional hollow structure and the binary heteroatom doping, the optimized NBCNT catalyst demonstrates superior catalytic performance for ORR in both acidic and alkaline electrolytes. Moreover, Zn-air batteries are constructed based on the as-prepared catalysts, which reveal a high operating voltage (1.43 V) and peak power density (173.93 mW cm−2), further demonstrating a comparable electrocatalytic performance of the catalysts to commercial Pt/C catalyst. This work reveals a novel construction of high-efficiency and cost-effective metal-free catalysts for various energy conversion and storage technologies.

S, N co-doped carbon nanotube encased Co NPs as efficient bifunctional oxygen electrocatalysts for zinc-air batteries

For the practical application of metal-air batteries, developing high-active and low-cost bifunctional oxygen reduction reaction (ORR) and oxygen evolution reduction (OER) catalysts is crucial and challenging. This study designed a unique ordered three-dimensional (3D) core–shell nanostructure bifunctional ORR and OER electrocatalysts consisting of Co nanoparticles (NPs) embedded in S, N co-doped carbon nanotubes (S,N-Co@CNT). The prepared S,N-Co@CNT exhibited excellent bifunctional electrocatalytic performance, with a high half-wave potential of 0.874 V versus reversible hydrogen electrode (RHE) toward ORR, and a low overpotential of 276 mV at 10 mA·cm−2 for the OER. The unique core–shell nanostructure has delivered considerable durability and stability in the S,N-Co@CNT, demonstrating almost no change in the potential gap between the ORR and OER after more than 5000 cycles of the accelerated durability test. Moreover, the S,N-Co@CNT serves as a high-active and low-price air–cathode catalyst for a rechargeable zinc-air battery, with a high peak power density of 171 mW·cm−2, and a long continuous charging-discharging ability. Based on mechanistic studies, the high activity of the S,N-Co@CNT was derived from the suitable oxygen adsorption energy due to the effects from S, N co-doping. The outcomes from this study offer a novel strategy to prepare non-noble metal bifunctional oxygen catalysts for metal-air batteries.

Heteroatom sulfur-induced defect engineering in carbon nanotubes: Enhanced electrocatalytic activity of oxygen reduction reaction

Heteroatoms doped carbon nanotubes are prepared through a solid-state pyrolytic conversion strategy with low-cost and easy-to-get precursors. The use of inorganic sulfur source makes it possible for sulfur to be effectively introduced, which is found to increase the defective degree in the carbon plane. The defect augment is revealed by systematic physical characterizations to originate from the fact that S atoms get rid of the carbon crystal and diffuse to form bits of sulfides during the heat-treatment process, thus leaving abundant vacant spots and providing access to forming pyridine-N sites. Therefore, more catalytic active sites are exposed and the oxygen reduction reaction (ORR) activity can be improved. Benefiting from the advantages in structure and composition, the resultant catalyst shows a remarkable half-wave potential (0.86 V vs. RHE) and an outstanding durability, superior to that of Pt/C. The zinc-air battery with the resultant catalyst shows high peak power density and excellent rate capability. This work not only develops a facile method to prepare highly active and stable ORR catalyst but also makes deep researches on the activity-enhanced mechanism.

A wearable real-time power supply with a Mg3Bi2-based thermoelectric module

A wearable thermoelectric generator using human body temperature is a promising power supply for wearable electronics. Here we discuss the design and fabrication of one kind of wearable thermoelectric generator constructed by n-type Mg3.2Bi1.498Sb0.5Te0.002 legs, p-type Bi0.4Sb1.6Te3 legs, polyurethane matrices, and flexible Cu/polyimide electrodes. The proposed device has a low thermal bypass and an efficient thermal contact interface, resulting in a peak power density of ∼20.6 μW/cm2 when placed on a human arm at an ambient temperature of 289 K (air velocity, 1.1 m/s) and a high peak power density of 13.8 mW/cm2 at a temperature difference of 50 K. In addition, it can withstand 10,000 bending cycles at a bend radius of 13.4 mm, suggesting that the proposed wearable thermoelectric generator has the potential to be a real-time power supply for certain wearable electronics in daily life.

Achieving exceptional activity and durability toward oxygen reduction based on a cobalt-free perovskite for solid oxide fuel cells

In response to the shortcomings of cobalt-rich cathodes, iron-based perovskite oxides appear as promising alternatives for solid oxide fuel cells (SOFCs). However, their inferior electrochemical performance at reduced temperatures (<700 °C) becomes a major bottleneck for future progress. Here, a novel cobalt-free perovskite Ba0.75Sr0.25Fe0.875Ga0.125O3−δ (BSFG) is developed as an efficient oxygen reduction electrode for SOFCs, featuring cubic-symmetry structure, large oxygen vacancy concentration and fast oxygen transport. Benefiting from these merits, cells incorporated with BSFG achieve exceptionally high electrochemical performance, as evidenced by a low polarization area-specific resistance of 0.074 Ω cm2 and a high peak power density of 1145 mW cm−2 at 600 °C. Meanwhile, a robust short-term performance stability of BSFG cathode can be ascribed to the stable crystalline structure and favorable thermal expansion behavior. First-principles computations are also conducted to understanding the superior activity and durability toward oxygen reduction reaction. These pave the way for rationally developing highly active and robust cobalt-free perovskite-type cathode materials for reduced-temperature SOFCs.

Fluorination-assisted preparation of self-supporting single-atom Fe-N-doped single-wall carbon nanotube film as bifunctional oxygen electrode for rechargeable Zn-Air batteries

Freestanding membrane electrodes with a high electrocatalytic activity and stability are desirable for use in high-performance metal-air batteries. Here, we report a gas-phase fluorination-assisted method to anchor single atom Fe-Nx moieties on a freestanding single-wall carbon nanotube (SWCNT) film that involves fluorination and defluorination/ammoniation processes. It is shown that the fluorination followed by defluorination/ammoniation harvests Fe atoms from the residual Fe nanoparticles used for SWCNT growth to form high density of Fe-Nx active sites, while retaining the flexibility, integrity and high quality of the films so that they can be directly used as a bifunctional oxygen electrode for rechargeable Zn-Air batteries. The single-atom Fe-Nx loaded SWCNT film shows an even better catalytic activity than commercial Pt/C-Ir/C catalysts, and an assembled Zn-Air battery using it exhibits a low charge-discharge voltage gap of 0.84 V under 20 mA/cm2, a high peak power density of 210 mW/cm2, and excellent long-time cycling stability. In addition, a flexible all-solid-state Zn-Air battery was assembled which has a stable open circuit voltage when bent to different angles.

P-Doped α-Ca2SiO4 and (Si, P)-Codoped CaO with Special Defect Microstructures and Luminescence due to an Enhanced Solid Solution by a Pulsed Laser Ablation Condensation Route

The α-Ca2SiO4 and rocksalt-type (R) CaO condensates/particulates with an enhanced solid solution of P and Si + P ions, respectively, were produced via pulsed laser ablation of a silicocarnotite (Ca5(PO4)2SiO4) target under a relatively high peak power density of 1.8 × 109 Watt/cm2 in high vacuum (8 × 10–5 torr). The condensates were dispersed in an amorphous phase of Ca–Si–P–O linkage as spheres up to submicrons in size or coalesced in particulates by the {100}R, {111}R, and {1̅21̅0}α facets to follow a preferred crystallographic relationship of (1̅1̅1)R//(1̅21̅0)α; [101]R//[101̅1]α, with a fair three-dimensional match of the lattice planes. The 1-D commensurate superstructures n × (200)R and n × (1̅21̅0)a, where n = 1.5 and 3, were commonly noted for the condensates in the particulates. The P-doped α-Ca2SiO4 and (Si, P)-codoped CaO showed characteristic luminescence at 407 and 537 nm, respectively, under the combined influences of internal compressive stress as well as substitutional and/or interstitial defects with charge/volume-compensating cation vacancies for potential optoelectronic and photocatalytic applications.

Solid-State Synthesis of Highly Dispersed Nitrogen-Coordinated Single Iron Atom Electrocatalysts for Proton Exchange Membrane Fuel Cells.

Fe-N-C with atomically dispersed Fe single atoms is the most promising candidate to replace platinum for the oxygen reduction reaction (ORR) in fuel cells. However, the conventional synthesis procedures require quantities solvents and metal precursors, sluggish adsorption process, and tedious washing, resulting in limited metal doping and uneconomical for large-scale production. For the first time, Fe2O3 is adopted as the Fe precursor to derive abundant single Fe atoms dispersed on carbon surfaces. The Fe-N-C catalyst synthesized by this simple method shows an excellent ORR activity with half-wave potentials of 0.82 and 0.90 V in acidic and alkaline solutions, respectively. A single fuel cell with an optimized Fe-N-C cathode shows a high peak power density of 0.84 W cm-2. The solid-state transformation synthesis method developed in this study may shed light on mass production of single-atom-based catalysts.

A hierarchical architecture of Fe/Co/Ni-doped carbon nanotubes/nanospheres grafted on graphene as advanced bifunctional electrocatalyst for Zn-Air batteries

Rational design and synthesis of non-precious-metal bifunctional catalysts for oxygen reduction and evolution reactions (ORR and OER) is highly pursued to improve reaction efficiency of Zn-air batteries. Herein, an innovative 0D-1D-2D hierarchical structure material (denoted as FeCoNi-N-rGO) is developed by a facile two-step synthesis strategy to construct N-doped carbon nanotubes (CNTs) and carbon nanospheres (CNSs) for encapsulating ternary Fe/Co/Ni alloy nanoparticles on the surface of reduced graphene oxide (rGO). Specifically, abundant Fe/Co/Ni alloy nanoparticles and M-N-C active sites generated by transition metals (Co, Ni, Fe) coupling with N-doped carbon (CNTs, CNSs, and rGO) can provide the FeCoNi-N-rGO with superior OER and ORR properties; meanwhile, the hierarchical structure endows large specific surface area to expose more active sites and to facilitate mass transfer. Typically, the FeCoNi-N-rGO exhibits a high ORR half-wave potential of 0.836 V and a low OER overpotential of 440 mV at 10 mA cm−2 in 0.1 M KOH. Moreover, the FeCoNi-N-rGO-based rechargeable Zn-air battery can deliver a high peak power density (152.5 mW cm−2), specific capacity (766 mAh g−1) and excellent stability (more than 200 h), surpassing commercial Pt/C-RuO2 catalysts. Therefore, this work will offer an easy fabrication strategy to design bifunctional catalysts with desirable performances for Zn-air batteries.

Rechargeable Zn-Air Batteries with Outstanding Cycling Stability Enabled by Ultrafine FeNi Nanoparticles-Encapsulated N-Doped Carbon Nanosheets as a Bifunctional Electrocatalyst.

Despite grand advances in Zn-air batteries in recently years, their commercialization remains challenging due largely to the lack of efficient bifunctional oxygen catalysts. Herein, we report the crafting of a bifunctional electrocatalyst comprising ultrafine alloyed FeNi nanoparticles encapsulated within N-doped layered carbon nanosheets (denoted FeNi/N-LCN) for high-efficiency Zn-air batteries. The FeNi/N-LCN electrocatalyst is yielded via the coordination of triphenylimidazole-containing polyaniline (TPANI) oligomer with Fe- and Ni-containing precursors, followed by hydrogen binding with melamine and subsequent pyrolysis. The as-constructed FeNi/N-LCN manifests outstanding activity and stability toward both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The primary Zn-air battery assembled with FeNi/N-LCN delivers both high specific capacity and peak power density. Remarkably, the rechargeable Zn-air battery can be repeatedly charged and discharged for 1100 h at 5 mA cm-2 and for 600 h at 10 mA cm-2, representing the highest cycling stability among various reported Zn-air batteries.

One-step integration of Co[sbnd]Ni phosphides in N, P co-doped carbons towards highly efficient oxygen electrocatalysis for rechargeable Zn-air battery

The development of highly efficient and robust bifunctional oxygen electrocatalysts is of great importance for optimizing the performance of rechargeable Zn-air batteries. In this study, CoNi phosphides encapsulated in N, P co-doped carbon (CoNiP/PNC) were prepared by a simple one-step pyrolysis method. The obtained catalyst exhibited outstanding oxygen reduction and oxygen evolution reaction (ORR and OER) activities in alkaline media. It exhibited a positive half-wave potential of 0.84 V versus the reversible hydrogen electrode for ORR, as well as a low overpotential of 470 mV to achieve 10 mA cm−2 for OER, comparable with the benchmark Pt/C and IrO2 catalysts. Furthermore, the rechargeable Zn-air battery was fabricated, which showed a high specific capacity of 729.3 mAh gZn-1, a high peak power density of 171.0 mW cm−2, and good stability. It reveals that the interplay between heteroatom-doped carbon layers and CoNi phase leads to the high ORR activity, and the in-situ formed bimetallic hydroxides/oxides contribute to the great OER performance. This work would inspire the future development of bifunctional electrocatalysts towards electrocatalysis in energy conversion and storage fields.

Octahedral distortion enhances exceptional oxygen catalytic activity of calcium manganite for advanced Zn-Air batteries

Calcium manganite (CMO) holds great potential for OER/ORR catalysis. But, the weak interaction between the oxygen intermediates and reaction sites leads to sluggish catalytic kinetics. Herein, to trigger the exceptional catalytic activity of CMO, we propose a thermal-induced MnO 6 octahedral distortion strategy to advance the absorption capability of intermediate reactants. Refined structural analysis and theoretical calculation reveal that the strong Jahn-Teller distortion of MnO 6 is capable of optimizing the surface electron redistribution and accelerating the electron transfer between the oxygen and Mn sites, which significantly boosts the intrinsic oxygen catalytic activities of the distorted CMO (D-CMO). Notably, the D-CMO functions as excellent bifunctional oxygen electrocatalysts and enables a high-performance solid-state Zn-air battery with satisfactory mechanical strength. Specifically, the as-assembled battery displays a remarkable open circuit voltage of 1.46 V and high peak power density of 149 mW cm −2 , even outstripping noble-metal-based counterparts. Modulating the octahedral units to ignite the intrinsic oxygen catalytic activity provides enlightening clues to design perovskite-type air cathodes. • A thermal-induced MnO 6 octahedral distortion strategy is proposed. • The octahedral distortion can optimize electron density and e g electron-filling states. • The octahedron-distortion CaMnO 3 (D-CMO) owns excellent oxygen catalytic activity. • The solid-state ZAB exhibits a high peak power density of 149 mW cm −2 .