High-efficiency Oxygen Reduction Reaction Research Articles

Interfacial Engineering of a Phase-Controlled Heterojunction for High-Efficiency HER, OER, and ORR Trifunctional Electrocatalysis.

The development of low-cost and high-performance electrocatalysts for simultaneously boosting the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) is highly crucial but still challenging. Herein, a facile one-step solid-phase polymerization and confined pyrolysis strategy is developed for scalable synthesis of a FexP/Fe3C-based (x = 1, 2) heterojunction with controllable iron phosphide crystal phases. By effective heterojunction interface regulation, the strong synergic effect between FeP/Fe3C and N- and P-codoped carbon (NPC) modified the electronic structure, resulting in an excellent electrocatalytic performance for the HER, OER, and ORR synchronously. Typically, the FeP/Fe3C@NPC catalyst exhibits efficient HER activity with a low overpotential of 10 mA cm–2 for the HER (97 mV) and OER (440 mV) and a high half-wave potential of 0.87 V for the ORR, as well as excellent stability in alkaline media. Theoretical calculations demonstrated that Fe3C can promote the activation of water molecules, while FeP is beneficial to the removal of H2 and the FeP/Fe3C heterojunction can facilitate both Volmer and Heyrovsky steps in the HER process simultaneously. Moreover, FeP has a stronger inhibitory effect on OH adsorption, revealing that the FeP/Fe3C heterojunction also shows a better promoting effect for both the OER and ORR, respectively.

Well entrapped platinum-iron nanoparticles on three-dimensional nitrogen-doped ordered mesoporous carbon as highly efficient and durable catalyst for oxygen reduction and zinc-air battery

The high-performance and durable oxygen reduction reaction (ORR) catalyst on air cathode is a key component in assembly of Zn-air batteries. Herein, three-dimensional N-doped ordered mesoporous carbon (3D N-OMC) was first prepared with silica as a template via pyrolysis with assistance of dicyandiamide as a N-doping agent, combined by full adsorption of platinum (II) acetylacetonate (Pt(acac)2) and iron (II) phthalocyanine (FePc) via π-π interactions. After further pyrolysis of the resulting mixture, many PtFe nanoparticles were efficiently incorporated in 3D N-OMC (termed as PtFe@3D N-OMC for simplicity). Control experiments were certificated the important role of the pyrolysis temperature played in this synthesis. The resultant composite synergistically combines advantages of hierarchically accessible surfaces, highly open structure, and well-dispersed PtFe particles, which endow the PtFe@3D N-OMC with onset and half-wave potentials of 0.98 and 0.86 V in alkaline media, respectively, showing appealing catalytic activity for the ORR. Most significantly, the PtFe@3D N-OMC based Zn-air battery has a high power density of 80.57 mW cm−2 and long-term durability (220 h, 660 cycles). This work opens a new avenue for design of high-efficiency and durable ORR electrocatalysts in energy conversion and storage systems.

Porphyrin polymer-derived single-atom Fe assisted by Fe2O3 with oxygen vacancy for efficient oxygen reduction reaction

Single-atom catalysts (SACs) have been deemed as one of the most prospective substitutes for high-efficiency oxygen reduction reaction (ORR) catalysts due to its theoretical maximum atomic utilization. However, the convenient preparation and the further improvement in activity of SACs are laborious. Herein, the N-doped porous carbon (NC) material with in site produced Fe-N4 single-atom catalytic sites (FeSA) accompanied by Fe2O3 species with abundant oxygen vacancies (Ov-Fe2O3) as co-catalytic sites (Ov-Fe2O3@FeSA@NC) is successfully obtained by using a well-designed porphyrin conjugated mesoporous polymer (CMP) consisting of iron porphyrin and metal free porphyrin units as a precursor, and followed by pyrolysis. A series of controllable experiments reveal that FeSA assisted by Ov-rich Fe2O3 render Ov-Fe2O3@FeSA@NC outstanding ORR activity in the alkaline medium with the onset and half-wave potentials (Eonset and E1/2) of 0.987 V and 0.901 V vs RHE, which significantly outperformed the electrochemical activity of FeSA@NC (Eonset = 0.962 V, E1/2 = 0.850 V) and Ov-Fe2O3@NC (Eonset = 0.913 V, E1/2 = 0.821 V) with individual FeSA and Ov-Fe2O3 active sites, respectively. This work innovatively demonstrates the importance of oxygen vacancy-assisted single-atom catalysts for oxygen reduction catalysis, and also provides guidance for the design of high-performance SACs.

Water-regulated and bioinspired one-step pyrolysis of iron-cobalt nanoparticles-capped carbon nanotubes/porous honeycombed nitrogen-doped carbon composite for highly efficient oxygen reduction

To achieve commercial applications of green fuel cells and rechargeable metal-air batteries, rational design and synthesis of low-cost, high-efficiency and ultra-stable transition metal-based electrocatalysts are of significant importance for alkaline oxygen reduction reaction (ORR). In this work, iron-cobalt (FeCo) nanoparticles-capped carbon nano-tubes/-porous nitrogen-doped honeycombed carbon composite (FeCo-CNTs/NHC-800) is synthesized by a water-regulated and bioinspired one-step pyrolysis method at 800 °C, where l-histidine behaves as the C and N sources combined by working as a chelating agent of Fe/Co. The formation mechanism is discussed by adjusting the pyrolysis temperature and water amount. The resultant FeCo-CNTs/NHC-800 exhibits a positive onset potential (Eonset = 1.091 V) and half-wave potential (E1/2 = 0.88 V), showing promising ORR activity, outperforming home-made controls and many lately reported catalysts. The hierarchically porous honeycombed structures have fascinating open porous spaces for fast diffusion of active species, large specific surface area, high conductivity, and stable sites for anchoring FeCo nanoparticles (NPs). Moreover, the N-doped carbon nanotubes coupling with homogeneous FeCo NPs greatly improve the catalytic activity and stability of ORR. This work provides some valuable insights to prepare hierarchical, reliable, and high-efficiency carbon-based ORR catalysts for new energy-correlated devices.

In-situ coupling FeN nanocrystals with Fe/Fe3C nanoparticles to N-doped carbon nanosheets for efficient oxygen electrocatalysis

Hetero-nanoparticles encapsulated in nitrogen-doped carbon show promising potential application in oxygen reduction reaction (ORR). Herein, a covalent-organic frameworks (COFs) based composite with FeN species and Fe/Fe3C nanoparticles embedded in N-doped carbon nanosheets (Fe/Fe3C@FeN-Cs) has been successfully synthesized by an in-situreduction of pre-designed Fe-N2-O2 units. Benefit from the compositional and structural synergistic effect, the optimized Fe/Fe3C@FeN-C-900 displays excellent ORR activity in both acidic (E1/2 = 0.77 V) and alkaline (E1/2 = 0.88 V) electrolytes, which are comparable and even superior to the benchmark Pt/C. Impressively, the maximum power density of fuel cell using Fe/Fe3C@FeN-C-900 as cathode catalyst reaches 408 mW cm−2. Moreover, the Fe/Fe3C@FeN-C-900-drived rechargeable zinc-air batteries (ZABs) deliver a higher power density (156.8 mW cm−2), larger specific capacity (775 mA h g−1) and better cycling stability (270 cycles) as compared with the state-of-the-art Pt/C counterpart. Theinterfacial electron transfer between Fe/Fe3C nanoparticles and neighboring FeN species, as well as the porous carbon architecture contribute to the excellent ORR performance of Fe/Fe3C@FeN-C-900, resulting in the easily adsorption/activation of O2 and accelerated ORR kinetics because of the fast mass transfer. The COF-derived synthetic strategy inspires new perspectives to develop hetero-nanoparticle composites as high-efficiency ORR electrocatalysts for the economical-practical energy conversion devices.

ZnS modified N, S dual-doped interconnected porous carbon derived from dye sludge waste as high-efficient ORR/OER catalyst for rechargeable zinc-air battery

Facile and rational design of high-efficient oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) bifunctional electrocatalysts is significant for rechargeable Zinc-air batteries. In this study, ZnS modified N, S dual-doped interconnected porous carbon (ZnS/NSC) derived from the dye sludge waste is successfully fabricated via a facile ZnCl2-assisted pyrolysis process. The effect of ZnCl2 and carbonization temperature on the microstructure and electrocatalytic performance is systematically investigated. By virtue of the synergistic effect between ZnS nanoparticles and N, S dual-doped porous carbon network, the obtained catalyst ZnS/NSC calcined at 1000 °C exhibits a decent bifunctional electrocatalytic performance with potential gap (ΔE=EOER,10-EORR,1/2) of 0.76 V comparable with commercial electrocatalysts (Pt/C and RuO2). In addition, a rechargeable zinc-air battery employed ZnS/NSC-1000 as the air cathode also displays the favorable electrochemical performance, in which the power density is 125 mW cm−2, the specific capacity is 763.27 mAh g−1 and the cycling stability at 10 mA cm−2 is more than 85 h, indicating a promising application prospect in rechargeable Zinc-air batteries.

Zr enhanced Fe, N, S co-doped carbon-based catalyst for high-efficiency oxygen reduction reaction

Fe-N x catalysts have received widespread attention in recent years due to their excellent catalytic performance, hoping to replace platinum for oxygen reduction reactions (ORR). In recent years, more studies have shown that when the catalyst contains two or more metals doped, its catalytic performance will be improved. Herein, using the high temperature pyrolysis method, through the incorporation of the second phase metal (Zr), melamine as the nitrogen source, and thiourea as the sulfur source, a high-activity carbon-based catalyst doped with Fe and Zr bimetals was synthesized. Originating from the strong interaction between Fe species and ZrO 2 clusters and the promotion of O 2 adsorption by ZrO 2 nanoparticles supported on nitrogen-doped carbon, this catalyst has a better ORR electrocatalytic performance than 46% TKK commercial platinum carbon in 0.1 M KOH, exhibiting an onset potential of 1.047 V vs RHE, a half-wave potential of 0.909 V vs RHE. It provides a new idea for the preparation of high-performance bimetallic-doped carbon-based electrocatalysts. • Zr, Fe, N, S co-doped carbon-based catalyst derived from Ionic Liquids a simple method. • The catalysts possesses high active sites and porous structure. • The interaction between Fe and Zr and the abundant active group substances could greatly improve the basic ORR activity.

Engineering heterostructured Co0.7Fe0.3@Co doped leaf-like carbon nanoplates from dual metal-organic frameworks for high-efficiency oxygen reduction reaction in microbial fuel cell

Microbial fuel cell (MFC) satisfies the needs of power generation and pollutants removal but still requires active electrocatalysts to accelerate cathodic oxygen reduction reaction (ORR). Metal-nitrogen-carbon materials (M − NCs) derived from Prussian blue analogues (PBAs), known for low cost and high yield, fail with satisfactory surface structure and their intrinsic activity requires to be further improved. Here, a MOF@MOF precursor (Co-ZIF-L@CoFe PBA-1, MOF: metal-Organic framework) is skillfully fabricated by utilizing two-dimensional (2D) leaf-like cobalt-based zeolitic-imidazolate framework (Co-ZIF-L) as the mother MOF to give birth to cobalt iron Prussian blue analogue (CoFe PBA) by adjusting reaction time and solvents with a ligand exchange method. After carbonization, Co-ZIF-L@CoFe PBA-1 transforms into a leaf-shaped carbon nanoplate with heterostructured CoFe alloy and Co (Co 0.7 Fe 0.3 @Co-NC-1), which exhibits outstanding ORR activity and high MFC performance (2486 ± 56 mW m -2 ) compared with Co-NC and Co 0.7 Fe 0.3 -NC derived from Co-ZIF-L and leaf-like CoFe PBA, respectively. The interfacial Co 0.7 Fe 0.3 @Co efficiently optimizes electronic structure for fast electrons transfer and the porous carbon matrix provides desirable surface structure for oxygen transfer, synergistically triggering a high ORR activity. Our work offers new insights for controllable preparation of PBAs-based dual-MOFs precursors and provides a feasible avenue for enhancing the activity of PBAs-based M − NCs catalysts. • Co-ZIF-L gives birth to Co-Fe PBA through a ligand exchange method. • The amount of Co-Fe PBA on Co-ZIF-L can be adjusted by reaction time and solvents. • The ORR activity is attributed to the integration of dual-MOF precursor. • The maximum power density of Co 0.7 Fe 0.3 @Co-NC-1 air cathode is 2486 ± 56 mW m 2 .

Three-dimensional self-supporting superstructured double-sided nanoneedles arrays of iron carbide nanoclusters embedded in manganese, nitrogen co-doped carbon for highly efficient oxygen reduction reaction

Nitrogen- and transition metal-dual doped carbon materials with low cost and high catalytic performances are considered as one of promising alternatives for noble metal catalysts in acceleration of oxygen reduction reaction (ORR). In this work, three-dimensional (3D) self-supporting superstructures of iron carbide (Fe3C) nanoclusters entrapped in manganese (Mn)- and nitrogen (N)-dual doped carbon nanosheets covered with double-sided nanoneedles carbon arrays (Fe3C/Mn,N-NCAs) are simply synthesized by a coordination pyrolysis method, in which dicyandiamide mainly behaves as nitrogen source and 1-(2-pyridylazo)-2-naphthol (PAN) as carbon source. Integration of the unique 3D self-supporting superstructures and synergistic effects of the multi-compositions, the as-obtained catalyst displays appealing ORR performance such as the much positive onset potential (Eonset = 0.98 V vs. RHE) and half-wave potential (E1/2 = 0.88 V vs. RHE), as well as a just 10 mV negative shift in E1/2 after 2000 cycles, surpassing commercial Pt/C. This work provides some valuable perspectives for preparation of high-efficiency and low-cost non-noble metal ORR electrocatalysts in energy transformation and storage correlated systems.

Single-atom alloy with Pt-Co dual sites as an efficient electrocatalyst for oxygen reduction reaction

Reducing the usage of noble metals, such as platinum-based catalysts for oxygen reduction reaction (ORR) is pressingly demanded towards the practical applications of proton-exchange membrane fuel cells. One promising way is to develop Pt single atom catalysts (SACs), which, however, are plagued by their preference toward two-electron ORR pathway as well as stability issue. Herein, a single-atom alloy (SAA) catalyst with platinum-cobalt (Pt-Co) dual sites encapsulated in nitrogen-doped graphitized carbon nanotubes (Pt1Co100/N-GCNT) consisting of isolated Pt atoms decorated on the surface of Co nanoparticles was reported. Based on complementary spectroscopic characterizations and first-principle calculations, we propose that the unique Pt-Co dual sites in SAA facilitates the adsorption and dissociation of oxygen, particularly for the immobilization of OOH* intermediate and the dissociation of OH* intermediate, and thus result in high-efficiency four-electron ORR pathway. Consequently, the Pt1Co100/N-GCNT SAA catalyst achieves a mass activity of 0.81 A mg–1Pt at 0.90 V (versus the reversible hydrogen electrode) in 0.1 M HClO4 electrolyte, outperform commercial Pt/C catalyst for 5.4 times. The superior stability of the SAA catalyst was reflected by the results from the 30,000 potential-scanning cycles combined with the post characterization of the catalyst.

Nano3 Assisted Gelatin-Derived Multi-Level Porous Carbon Aerogel Loaded Fe Single-Atom for High Efficient Oxygen Reduction Reaction

Nano3 Assisted Gelatin-Derived Multi-Level Porous Carbon Aerogel Loaded Fe Single-Atom for High Efficient Oxygen Reduction Reaction

Heteroatom doped M–N–C single-atom catalysts for high-efficiency oxygen reduction reaction: regulation of coordination configurations

Recent advances of heteroatom-doped M–N–C SACs for the ORR are summarized. Emphasis is given to the regulation of the coordination configuration of heteroatom-doped M–N–C SACs.

Coupling Nano-Fe3o4 with Oxygen Vacancies on a Hypercrosslinked Iron Porphyrin-Coated Zif-8 as a High-Efficiency Oxygen Reduction Reaction Electrocatalyst

Coupling Nano-Fe3o4 with Oxygen Vacancies on a Hypercrosslinked Iron Porphyrin-Coated Zif-8 as a High-Efficiency Oxygen Reduction Reaction Electrocatalyst

A Simple Synthesis of Fe2P Nanoparticles Encapsulated Doped Carbon Nanotube as Electrocatalysts for Oxygen Reduction Reaction and Zinc‐Air Battery

The design and application of high efficiency, low cost, and nonprecious metal oxygen reduction reaction (ORR) catalyst is a prerequisite for the commercialization of energy conversion devices. Here, a simple method is proposed to prepare Fe2P nanoparticles encapsulated in nitrogen‐doped carbon nanotubes (Fe2P@NPCNTs) through a self‐growth strategy. In addition, it is worth noting that Fe2P@NPCNTs have high catalytic activity and good stability as ORR catalysts due to the unique structure of the material, the synergy between the components, and the large specific surface area. As expected, the catalyst has a half‐wave potential (0.827 V) close to commercial Pt/C and a lower Tafel slope (54.17 mV dec−1) compared to other samples. Meanwhile, the zinc‐air battery with Fe2P@NPCNTs as catalysts exhibits high open‐circuit voltage, good maximum power density, and excellent stability. Therefore, this cheap and simple method is generally available for the synthesis of other non‐noble metal catalysts for various energy systems.

Synergistic Binary Fe-Co Nanocluster Supported on Defective Tungsten Oxide as Efficient Oxygen Reduction Electrocatalyst in Zinc-Air Battery.

Rational design of metal oxide supported non‐precious metals is essential for the development of stable and high‐efficiency oxygen reduction reaction (ORR) electrocatalysts. Here, an efficient ORR catalyst consisting of binary Fe/Co nanoclusters supported by defective tungsten oxide and embedded N‐doped carbon layer (NC) with a 3D ordered macroporous architecture (3DOM Fe/Co@NC‐WO2− x ) is developed. The oxygen deficient 3DOM WO2− x not only serves as a porous and stable support, but also enhances the conductivity and ensures good dispersion of the binary Fe/Co nanocluster, benefiting its ORR catalytic activity. Theoretical calculation shows that there exists a synergistic effect of electron transfer from Fe to Co in the supported binary Fe/Co cluster, promoting the ORR reaction energetics. Accordingly, the 3DOM Fe/Co@NC‐WO2− x catalyst exhibits excellent ORR activity in alkaline medium with a half wave potential (E 1/2) of 0.87 V higher than that of Pt/C (0.85 V). The zinc–air batteries assembled by 3DOM Fe/Co@NC‐WO2− x cathode deliver a higher power density and specific capacity than that of Pt/C. A new strategy of combining synergistic binary‐metal nanoclusters and conductive metal oxide support design is provided here to develop efficient and durable ORR electrocatalyst.

Coordination regulated pyrolysis synthesis of ultrafine FeNi/(FeNi)9S8 nanoclusters/nitrogen, sulfur-codoped graphitic carbon nanosheets as efficient bifunctional oxygen electrocatalysts

Design of advanced carbon nanomaterials with high-efficiency oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activities is still imperative yet challenging for searching green and renewable energies. Herein, we synthesized ultrafine FeNi/(FeNi)9S8 nanoclusters encapsulated in nitrogen, sulfur-codoped graphitic carbon nanosheets (FeNi/(FeNi)9S8/N,S-CNS) by coordination regulated pyrolyzing the mixture of the metal precursors, dithizone and g-C3N4 at 800 °C. The as-prepared FeNi/(FeNi)9S8/N,S-CNS exhibited distinct electrocatalytic activity and stability for the ORR with positive onset (Eonset) and half-wave (E1/2) potentials (Eonset = 0.97 V; E1/2 = 0.86 V) and OER with the small overpotential (η = 283 mV) at 10 mA cm−2 in the alkaline media, outperforming commercial Pt/C and RuO2 catalysts. This research provides some constructive guidelines for preparing efficient, low-cost and stable nanocatalysts for electrochemical energy devices.

Mesoporous N-P Codoped Carbon Nanosheets as Superior Cathodic Catalysts of Neutral Metal-Air Batteries.

Development of high-efficiency oxygen reduction reaction (ORR) catalysts under neutral conditions has made little research progress. In this work, we synthesized a three-dimensional porous N/P codoped carbon nanosheet composites (CNP@PNS) by high-temperature thermal treatment of dicyandiamide, starch, and triphenylphosphine and subsequent porous structure-making treatment using the NaCl molten salt template. In the neutral solution, the electrocatalytic performance of the CNP@PNS-4 catalyst exhibits an onset potential of 0.98 V (vs reversible hydrogen electrode) and a half-wave potential of 0.91 V for ORR, which greatly surpasses commercial Pt/C (40%). Three kinds of neutral metal-air batteries (Zn-air, Al-air, and Fe-air) using the prepared samples as cathodic catalysts were constructed, corresponding to the maximum power density of 120.2, 78.3, and 18.9 mW·cm-2, respectively. Also, they reveal outstanding discharge stability under different current densities. The density functional theory calculation depicts the reduction of the free energy of the determining step and subsequent decline of the overpotential for ORR.

Boron modulating electronic structure of FeN4C to initiate high-efficiency oxygen reduction reaction and high-performance zinc-air battery

The biggest challenge is to develop a low cost and readily available catalyst to replace expensive commercial Pt/C for efficient electrochemical oxygen reduction reaction (ORR). In this research, closo-[B12H12]2− and 1,10-phenanthroline-iron complexes were introduced into the porous metal-organic framework by impregnation method, and further annealing treatment achieved the successful anchoring of single-atom-Fe in B-doped CN Matrix (FeN4CB). The ORR activity of FeN4CB is comparable to the widely used commercial 20 wt% Pt/C. Where the half-wave potential (E1/2) in alkaline medium up to 0.84 V, and even in the face of challenging ORR in acidic medium, the E1/2 of ORR driven by FeN4CB is still as high as 0.81 V. When FeN4CB was used as air cathode, the open circuit voltage of Zn-air battery reaches 1.435 V, and the power density and specific capacity are as high as 177 mW cm−2 and 800 mAh gZn−1 (theoretical value: 820 mAh gZn−1), respectively. The dazzling point of FeN4CB also appears in the high ORR stability, whether in alkaline or acidic media, E1/2 and limiting current density are still close to the initial value after 5000 times cycles. After continuously running the charge-discharge test for 220 h, the charge voltage and discharge voltage of the rechargeable zinc-air battery with FeN4CB as the air cathode maintained the initial state. Density functional theory calculations reveals that introducing B atom to Fe–N4–C can adjust the electronic structure to easily break O = O bond and significantly reduce the energy barrier of the rate-determining step resulting in an improved ORR activity.

Tunable nano-distribution of Pt on TiO2 nanotubes by atomic compression control for high-efficient oxygen reduction reaction

Achieving cost-competitive catalysts with low Pt utilization and improving the durability caused by the corrosion of supports in the catalysts must be solved for the high activity in the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). Here, we show an innovative technique to synthesize unique nanotube supports for the ORR catalysts based on the combination of experimental and theoretical studies. The method precisely controls the atomic morphology of TiO2 nanotubes by a small amount of atomic substitution, maximizing their efficiency as catalyst supports. The spontaneous change in the size and dispersibility of the Pt nanoparticles appears by only small lattice contraction on the metal-doped TiO2 (M-TiO2) nanotubes. To study this phenomenon, various dopants such as V, Nb, and Cr were added to the M-TiO2 nanotubes. The compression arising out of each metal-support interaction resulted in the diverse shape of the nanoparticles on similar supports, which is revealed based on the X-ray absorption fine structure (XAFS) and the density-functional-theory (DFT) calculations. Based on a comprehensive understanding of inter-and intracrystal interactions in the small substitution doping process, we can control the size and dispersibility of the Pt nanoparticles, catalytic activity, and durability of catalysts for ORR.

Zn, Co, and Fe Tridoped N-C Core-Shell Nanocages as the High-Efficiency Oxygen Reduction Reaction Electrocatalyst in Zinc-Air Batteries.

Transition metal-nitrogen-carbon (TM-N-C) nanomaterials are promising platinum-based substitutes for the oxygen reduction reaction (ORR). However, large-scale commercial production of high-efficiency, durable TM-N-C catalysts remains a formidable challenge. In this work, a facile ″ZIF-on-ZIF″ strategy is first adopted to design ZIF-8@ZIF-67 core-shell polyhedral nanocages, and then, ferrocene (Fc) is added to form ZIF-8@ZIF-67@Fc double-layer encapsulating polyhedral nanocages. Finally, Zn, Co, and Fe tridoped N-C nanocages (ZnCoFe-N-C) as the high-efficiency ORR electrocatalyst are prepared through high-temperature annealing. Benefiting from the trimetal, nitrogen and carbon species bond to each other to form highly efficient active sites, and the material exhibits outstanding performance in 0.1 M KOH, onset potential and half-wave potential of up to 0.95 and 0.878 V (vs RHE), respectively, and long-term durability and methanol tolerance. Furthermore, when utilizing as a zinc-air battery (ZAB) air electrode, it exhibits wonderful indicators, reflected in an open circuit voltage of 1.525 V, power density of 350.2 mW cm-2, and specific capacity of 794.7 mAh gzn-1, which outperforms the benchmark Pt/C catalyst. This work provides a facile and effective strategy to obtain a highly efficient and stable TM-N-C electrocatalyst for the ORR in ZABs.