High-performance Oxygen Reduction Reaction Research Articles

Water hyacinth root derived hybrid metal oxides/nitrogen doped porous carbon as an efficient non-precious metal oxygen reduction reaction electrocatalyst in alkaline media

A biomass derived hybrid metal oxides/nitrogen doped porous carbon (NC) electrocatalyst is fabricated by direct pyrolysis of the water hyacinth root (WHR) mixed ZnCl2 raw materials at 600 °C (WHR600), 700 °C (WHR700) and 800 °C (WHR800) under autogenic pressure conditions. XRD analysis presents a novel Zn(Al1.8Fe0.2)O4 compound combined with hematite quart and muscovite phases for WHR700 and WHR800 samples. In addition, the WHR700 sample accounts for the maximum pyridinic N content incorporated into carbon framework (NC). Electrochemically, the WHR700 catalyst displays the highest oxygen reduction reaction (ORR) performance in alkaline media. The high ORR performance for WHR700 catalyst is significantly a result of the presence of the Zn(Al1.8Fe0.2)O4 phase and the pyridinic N species. Furthermore, an accelerate durability test for WHR700 sample over 5000 cycles exhibits only 8 mV half-wave potential reduction. The WHR700 catalyst is also extremely stable to the methanol poisoning during ORR operation.

Trifunctional electrocatalysts of single transition metal atom doped g-C4N3 with high performance for OER, ORR and HER

With the rapid development of renewable energy technologies, the quest for efficient and cost-effective trifunctional catalysts capable of simultaneously driving the Hydrogen Evolution Reaction (HER), Oxygen Reduction Reaction (ORR), and Oxygen Evolution Reactions (OER) has become a focal point of research. In this study, we employed first-principles calculations to investigate the catalytic activities of the synthetic material g-C4N3 as an electrocatalyst for HER, OER, and ORR by incorporating various transition metal atoms into the numerous 3 N vacancies (TM@g-C4N3) naturally occurring in its primitive structure. Our calculations reveal that Cu@g-C4N3 holds promise as a trifunctional electrocatalyst, exhibiting low OER/ORR overpotentials (ηOER = ηORR = 0.44 V) and a |ΔG∗H| value of only 0.08 eV. Furthermore, Ni@g-C4N3_S1N2 exhibits a lower OER overpotential (ηOER = 0.34 V). Bader charge analysis, charge density difference calculations, and D-band center investigations confirm that the catalytic performance is fundamentally rooted in the electronic properties of these materials. Thus, g-C4N3 embedded with transition metal atoms shows promise as an efficient electrocatalyst for OER/ORR/HER, with implications for the development of high-efficiency trifunctional electrocatalysts.

Nitrogen-doped carbon/graphitic CQDs composites with 98.8% microporosity as a highly stable electrocatalyst for oxygen reduction

Designing micropore-rich carbon materials with large specific surface area (SSA) as a carbon-based oxygen reduction reaction (ORR) electrocatalyst is still frontier but remains challenging in catalysis of zinc-air batteries. Here we propose a new strategy for synthesis of nitrogen atoms co-doped carbon sheets and carbon quantum dots (N-C@CQDs) with an SSA of 1485.3 m2 g−1 and 98.8 % micro-porosity from α-cellulose via using a complex salt (ZnCl2-NH4Cl) with low eutectic point (179 °C) as a pore regulator and K2FeO4 as a graphitization catalyst, which can serve as an active and stable carbon-based ORR electrocatalyst. The role of K2FeO4 not only promotes graphitization but also oxidizes the large-sized graphitic carbon particles into a huge amount of uniformly distributed CQDs. This catalyst has exhibited a comparable ORR activity and superior stability to the Pt/C, but a Zn-air battery assembled with the former has delivered a higher peak power density (214 mW cm−2) and a larger gravimetric energy density (ED) of (959 Wh kgZn-1), especially in which it also displays an outstanding catalytic durability with 98.7 % ED retention during a ∼110 h continuous discharge. This work provides a new pathway for design of high-performance carbon-based ORR catalysts in various energy devices.

Shape and composition evolution of Pt and Pt3M nanocrystals under HCl chemical etching

Controlling the shape and composition of Pt-based nanocrystals is essential to improve electrocatalytic performance. In this work, we have carefully investigated the evolution process of morphology and composition for Pt and Pt3M (M = Ni, Co) nanocrystals by hydrochloric acid (HCl) etching. As a result, only Pt3Ni nanocrystals successfully formed unsaturated step-like atoms on the surface and then constructed high-index facets (HIFs), while Pt and Pt3Co preserved a good octahedron shape. Density functional theory (DFT) calculation suggests that Cl− ions can be tightly adsorbed on the surface of Pt3Ni rather than other nanocrystals, which hinders the deposition of newly-reduced atoms and thus regulating the surface morphology. Besides, the etching of surface transitional metals further accelerates the formation of HIFs. Boosted by the active sites on the surface, HCl-Pt-Ni exhibited a ∼10.8 and ∼11.3 times higher oxygen reduction reaction (ORR) mass and specific activities than commercial Pt/C catalyst, and possessed a good durability after 10,000 cycles test. This work gives a deep insight into the design of high-performance Pt-based ORR catalysts.

Zn Single Atoms/Clusters/Nanoparticles Embedded in the Hybrid Carbon Aerogels for High-Performance ORR Electrocatalysis.

Carbon-supported zinc single-atom catalysts have received considerable attention in the electrocatalytic oxygen reduction reaction (ORR) owing to the strong reduction capacity of zinc atoms and the abundant reserves of zinc elements. The common preparation method has been limited to the high-temperature pyrolysis of nitrogen-rich organic molecules and zinc ions, which makes it difficult to further improve the ORR performance. Herein, we first prepared ZnO/PNT/rGO aerogels as precursors via a simple hydrothermal method combined with freeze-drying, in which reduced graphene oxides (rGO) and polypyrrole nanotubes (PNT) together assembled into three-dimensional frames and numerous ZnO nanoparticles were anchored in the three-dimensional skeletons. Then, ZnO/PNT/rGO aerogels were calcined at 800 °C in the argon atmosphere, in which PNT/rGO were derived carbon aerogels, ZnO nanoparticles were reduced to Zn0 by carbon, and generating zinc single atoms were captured by the surrounding nitrogen atoms or aggregated into Zn clusters/nanoparticles in the carbon substrates. The obtained products were Zn single atoms/clusters/nanoparticles embedded into PNT/rGO-derived carbon aerogels, named Zn/NC catalysts. Zn/NC catalysts display a much higher half-wave potential and a larger limiting current density than pure rGO aerogels, NC, and Zn/C catalysts, indicating the synergy of excellent electronic transportation, high mass efficiency from outstanding porosity, and several active centers. Tailoring the quantity of zinc acetate can provide the optimal ORR performance with the Eonset of 0.96 V, the E1/2 of 0.845 V, and remarkable durability. This work exploits a novel strategy of carbon thermal reduction to construct high-performance Zn-based low-dimensional ORR catalysts.

Use of biogenic silver nanoparticles on the cathode to improve bioelectricity production in microbial fuel cells.

To date, research on microbial fuel cells (MFCs) has. focused on the production of cost-effective, high-performance electrodes and catalysts. The present study focuses on the synthesis of silver nanoparticles (AgNPs) by Pseudomonas sp. and evaluates their role as an oxygen reduction reaction (ORR) catalyst in an MFC. Biogenic AgNPs were synthesized from Pseudomonas aeruginosa via facile hydrothermal synthesis. The physiochemical characterization of the biogenic AgNPs was conducted via scanning electron microscopy (SEM), X-ray diffraction (XRD), and UV-visible spectrum analysis. SEM micrographs showed a spherical cluster of AgNPs of 20-100nm in size. The oxygen reduction reaction (ORR) ability of the biogenic AgNPs was studied using cyclic voltammetry (CV). The oxygen reduction peaks were observed at 0.43V, 0.42V, 0.410V, and 0.39V. Different concentrations of biogenic AgNPs (0.25-1.0mg/cm2) were used as ORR catalysts at the cathode in the MFC. A steady increase in the power production was observed with increasing concentrations of biogenic AgNPs. Biogenic AgNPs loaded with 1.0mg/cm2 exhibited the highest power density (PDmax) of 4.70W/m3, which was approximately 26.30% higher than the PDmax of the sample loaded with 0.25mg/cm2. The highest COD removal and Coulombic efficiency (CE) were also observed in biogenic AgNPs loaded with 1.0mg/cm2 (83.8% and 11.7%, respectively). However, the opposite trend was observed in the internal resistance of the MFC. The lowest internal resistance was observed in a 1.0mg/cm2 loading (87Ω), which is attributed to the high oxygen reduction kinetics at the surface of the cathode by the biogenic AgNPs. The results of this study conclude that biogenic AgNPs are a cost-effective, high-performance ORR catalyst in MFCs.

Morphological and microstructural engineering of Mn-N-C with strengthened Mn-N bond for efficient electrochemical oxygen reduction reaction

Revealing the correlation between the micro–macro structures and active sites of transition metal-nitrogen-carbon (M−N−C) for electrochemical oxygen reduction reaction (ORR) is essential to develop non-precious metal catalyzed fuel cells and metal-air batteries. Herein, Mn-N-C catalysts with various morphologies and microstructures were prepared using Mn2+ coordinated bis(imino)-pyridine-based polymer with N-rich content as a new platform of precursor, which was synthesized via a condensation reaction of 1H-1, 2, 4-Triazole-3, 5-Diamine and 2, 6-Diacetylpyridine. Results demonstrate that morphologies and fine structures (pore structure, N dopants, surface area, and atomic Mn-N bond length, etc.) of Mn-N-C catalysts are strongly dependent on the growth of the specific precursor with and without NaCl as a template and the secondary calcination temperature can further optimize the bond length of Mn-Nx moieties, resulting in significant activity differences between correspondingly derived Mn-N-C catalysts for ORR. Compared to Mn-N-C derived from the synthesized precursor without NaCl, Mn-N-C obtained by the precursor grown directly on NaCl features an ultra-thin nanosheet-like structure with a hierarchical pore distribution and a shorter Mn-N bond, presenting high ORR performance with a half-wave potential of 0.88 V in 0.1 M KOH and a tiny potential loss of 11 mV after 30 K cycles, which is also proved by high-performance practical single Zn-Air battery (139 mW·cm−2) and proton exchange membrane fuel cell (400 mW·cm−2). This work provides a new understanding of the critical role of morphology and Mn-N bonding length of M−N−C for enhancing ORR and a new route of developing non-Fe/Co-based M−N−C catalysts for electrocatalysis.

Constructing Nitrogen-Doped Carbon Hierarchy Structure Derived from Metal-Organic Framework as High-Performance ORR Cathode Material for Zn-Air Battery.

The development of efficient and low-cost catalysts for cathodic oxygen reduction reaction (ORR) in Zn-air battery (ZAB) is a key factor in reducing costs and achieving industrialization. Here, a novel segregated CoNiPt alloy embedded in N-doped porous carbon with a nanoflowers (NFs)-like hierarchy structure is synthesized through pyrolyzing Hofmann-type metal-organic frameworks (MOFs). The unique hierarchical NFs structure exposes more active sites and facilitates the transportation of reaction intermediates, thus accelerating the reaction kinetics. Impressively, the resulting 15% CoNiPt@C NFs catalyst exhibits outstanding alkaline ORR activity with a half-wave potential of 0.93V, and its mass activity is 7.5 times higher than that of commercial Pt/C catalyst, surpassing state-of-the-art noble metal-based catalysts. Furthermore, the assembled CoNiPt@C+RuO2 ZAB demonstrates a maximum power density of 172mW cm-2 , which is superior to that of commercial Pt/C+RuO2 ZAB. Experimental results reveal that the intrinsic ORR mass activity is attributed to the synergistic interaction between oxygen defects and pyrrolic/graphitic N species, which optimizes the adsorption energy of the intermediate species in the ORR process and greatly enhances catalytic activity. This work provides a practical and feasible strategy for synthesizing cost-effective alkaline ORR catalysts by optimizing the electronic structure of MOF-derived catalysts.

Selectively oxygen reduction reaction and strongly suppressed CO poisoning on PtZn nanoalloys decorated on N-doped carbon sphere

The development of a high-performance oxygen reduction reaction (ORR) catalyst with a low Pt content, high activity, and long-term durability is crucial as it can become a core item in the fuel cell market. In this study, the amount of Pt used in the catalyst is reduced by more than three-fold compared with commercial catalysts. Concurrently, a PtZn alloy, which does not use expensive transition metals, is introduced as an active species. Nitrogen-doped carbon sphere (CS), which serves as an electron sink, is used as a support; it acts as a Lewis base site and facilitates H+ adsorption during the ORR. The analytical results reveal that the introduction of Zn is significantly more favorable for the ORR compared with N-doping. O2-pulse temperature-programmed desorption (TPD) reveals that most of the O2 molecules are adsorbed on Zn, and CO-pulse TPD demonstrates that Zn suppresses CO poisoning in the PtZn alloys. The mass and specific activities of the Pt1Zn1/N-CS electrode at 0.9 V are 5.94 A mg–1 and 0.79 mA cm–2, respectively, and a rotational frequency of 2.5 e-site–1 s–1 is achieved. The electrochemical performance remains unchanged even after 5000 cycles. The ORR on the Pt1Zn1/N-CS electrode does not occur randomly on Pt and Zn; Pt and Zn selectively attract and reduce *O, *OH, or *OOH which generated as intermediates.

TiO/Ti3O5-Decorated Electrospun Carbon Nanofibers as High-Performance Oxygen Reduction Reaction Electrocatalysts

TiO/Ti₃O₅-Decorated Electrospun Carbon Nanofibers as High-Performance Oxygen Reduction Reaction Electrocatalysts

Mn-Doped Zn Metal-Organic Framework-Derived Porous N-Doped Carbon Composite as a High-Performance Nonprecious Electrocatalyst for Oxygen Reduction and Aqueous/Flexible Zinc-Air Batteries.

Developing low-cost, efficient, and stable oxygen reduction reaction (ORR) electrocatalysts is crucial for the commercialization of energy conversion devices such as metal-air batteries. In this study, we report a Mn-doped Zn metal-organic framework-derived porous N-doped carbon composite (30-ZnMn-NC) as a high-performance ORR catalyst. 30-ZnMn-NC exhibits excellent electrocatalytic activity, demonstrating a kinetic current density of 9.58 mA cm-2 (0.8 V) and a half-wave potential of 0.83 V, surpassing the benchmark Pt/C and most of the recently reported non-noble metal-based catalysts. Moreover, the assembled zinc-air battery with 30-ZnMn-NC demonstrates high peak power densities of 207 and 66.3 mW cm-2 in liquid and flexible batteries, respectively, highlighting its potential for practical applications. The excellent electrocatalytic activity of 30-ZnMn-NC is attributed to its unique porous structure, the strong electronic interaction between metal Zn/Mn and adjacent N-doped carbon, as well as the bimetallic Mn/Zn-N active sites, which synergistically promote faster reaction kinetics. This work offers a controllable design strategy for efficient electrocatalysts with porous structures and bimetallic active sites, which can significantly enhance the performance of energy conversion devices.

Building Atomic Scale and Dense Fe─N4 Edge Sites of Highly Efficient Fe─N─C Oxygen Reduction Catalysts Using a Sacrificial Bimetallic Pyrolysis Strategy.

Replacing high-cost and scarce platinum (Pt) with transition metal and nitrogen co-doped carbon (M/N/C, M = Fe, Co, Mn, and so on) catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells has largely been impeded by the unsatisfactory ORR activity of M/N/C due to the low site utilization and inferior intrinsic activity of the M─N4 active center. Here, these limits are overcome by using a sacrificial bimetallic pyrolysis strategy to synthesize Fe─N─C catalyst by implanting the Cd ions in the backbone of ZIF-8, leading to exposure of inaccessible FeN4 edge sites (that is, increasing active site density (SD)) and high fast mass transport at the catalyst layer of cathode. As a result, the final obtained Fe(Cd)─N─C catalyst has an active site density of 33.01 µmol g-1 (with 33.01% site utilization) over 5.8 times higher than that of Fe─N─C catalyst. Specially, the optimal catalyst delivers a high ORR performance with a half-wave potential of 0.837 (vs RHE) in a 0.1 m HClO4 electrolyte, which surpasses most of Fe-based catalysts.

Facile synthesis of PtCo nanoparticles/three-dimensional graphene hybrid material as a highly active and stable electrocatalyst for oxygen reduction reaction

To further promote the widespread commercialization of proton exchange membrane fuel cells (PEMFCs), high performance oxygen reduction reaction (ORR) catalysts with high activity and stability must be developed to accelerate its sluggish kinetic process. Here, we report a successful synthesis of a novel hybrid material - highly synergistic PtCo nanoparticles (NPs) attached to three-dimensional graphene (PtCo @3DG). The PtCo @3DG exhibits excellent ORR performance, and the mass activity and specific activity measured at 0.9 V vs. RHE were 0.801 A/mgPt and 1.250 mA/cm2 respectively, which are 6.8 and 6.2 times higher than commercial Pt/C. High stability of this new material is achieved, which has demonstrated a loss of only 1.87% after an extensive 10,000 cycles test. The superior performance of PtCo @3DG can be primarily attributed to several key features, including its ultrathin size, a high Pt utilization, and a beneficial alloy effect. Additionally, the 3D graphene possesses an open and interconnected porous structure that facilitates efficient charge and mass transfer, which accelerates the desorption process of intermediates and exposes more active sites.

N and S dual-coordinated Fe single-atoms in hierarchically porous hollow nanocarbon for efficient oxygen reduction

Fe-, and N-co-doped carbon (FeNC) electrocatalysts are promising alternatives to Pt-based catalysts for oxygen reduction reaction (ORR); however, simultaneously enhancing their intrinsic activity and exposure of Fe active sites remains challenging. Herein, we report S-modified Fe single-atom catalysts (SACs) anchored on N,S-co-doped hollow porous nanocarbon (Fe/NS-C) for ORR. The unique hollow structure and large surface area of the SACs are favorable for mass/electron transport and exposure of Fe single-atom active sites. The as-prepared Fe/NS-C electrocatalysts display a high-efficiency ORR activity with a half-wave potential of 0.893 V versus the reversible hydrogen electrode and exceed that of the benchmark commercial Pt/C catalyst as well as most reported transition-metal based SACs. Impressively, the Fe/NS-C-based Al-air battery (AAB) displays a high open circuit voltage of 1.48 V, a maximum power density of 140.16 mW cm−2, and satisfactory durability, outperforming commercial Pt/C-based AAB. Furthermore, Fe/NS-C exhibits considerable potential as a cathode catalyst for application in direct methanol fuel cells. Experimental and theoretical calculation results reveal that the excellent ORR performance of Fe/NS-C can be contributed to the highly active FeN3S sites and the unique hollow structure. This work provides new insights into the rational design and synthesis high-performance ORR electrocatalysts for energy conversion and storage devices. of employing ZIF-8 as precursors.

Spatial confinement of zeolitic imidazolate framework deposits by porous carbon nanospheres for dual-atom catalyst towards high-performance oxygen reduction reaction

Spatial confinement of zeolitic imidazolate framework deposits by porous carbon nanospheres for dual-atom catalyst towards high-performance oxygen reduction reaction

Soft‐Pyrolysis Co–N‐Implanted Polymer to Gain High‐Density Co–Nx Sites on Carbons for Efficient Oxygen Reduction in Zn–Air Batteries

A soft‐pyrolysis strategy by heating Co–N‐implanted covalent organic polymer combining on carbon nanotubes at ≤500 °C has been developed to obtain efficient Co–N–C electrocatalysts for oxygen reduction reaction (ORR). The prepared Co–N–C is highly active for ORR with a half‐wave potential of 0.91 V versus RHE in 0.1 m KOH electrolyte, superior to most of previously reported Co‐based electrocatalysts. When employing it as cathode electrocatalyst, the homemade Zn–air battery shows a peak power density of 304.2 mW cm−2, comparable to the parallel power density (250 mW cm−2) of Zn–air battery with Pt/C (20 wt%) electrocatalyst at cathode. The soft‐pyrolysis strategy not only helps to generate high density Co–Nx active sites on carbons but also facilitates the optimizing balance between active site densities, graphitization degree, and pore structure of Co–N–C catalysts. Herein, a simple and energy‐effective low‐temperature pyrolysis strategy to obtain high‐performance ORR electrocatalyst is provided.

Molten-Salt Electrochemical Deoxidation Synthesis of Platinum-Neodymium Nanoalloy Catalysts for Oxygen Reduction Reaction.

Platinum-rare earth metal (Pt-RE) nanoalloys are regarded as a potential high performance oxygen reduction reaction (ORR) catalyst. However, wet chemical synthesis of the nanoalloys is a crucial challenge because of the extremely high oxygen affinity of RE elements and the significantly different standard reduction potentials between Pt and RE. Here, this paper presents a molten-salt electrochemical synthetic strategy for the compositional-controlled preparation of platinum-neodymium (Pt-Nd) nanoalloy catalysts. Carbon-supported platinum-neodymium (Ptx Nd/C) nanoalloys, with distinct compositions of Pt5 Nd and Pt2 Nd, are obtained through molten-salt electrochemical deoxidation of platinum and neodymium oxide (Pt-Nd2 O3 ) precursors supported on carbon. The Ptx Nd/C nanoalloys, especially the Pt5 Nd/C exhibit a mass activity of 0.40Amg-1 Pt and a specific activity of 1.41mAcm-2 Pt at 0.9V versus RHE, which are 3.1 and 7.1 times higher, respectively, than that of commercial Pt/C catalyst. More significantly, the Pt5 Nd/C catalyst is remarkably stable after undergoing 20000 accelerated durability cycles. Furthermore, the density-functional-theory (DFT) calculations confirm that the ORR catalytic performance of Ptx Nd/C nanoalloys is enhanced by compressive strain effect of Pt overlayer, causing a suitable weakened binding energies of O* and .

Use of Fe-H3BTC and GO Compounds To Prepare N/Fe-Doped Carbon for a High-Performance Oxygen Reduction Reaction Catalyst.

Zinc-air batteries (ZABs), as a new type of energy storage and conversion device, have received lots of attention due to their high energy density and low cost. The electrode material is a key factor for improving the performance of ZABs. Here, a facile strategy for the fabrication of N-rich porous carbon is reported. H3BTC and GO are selected as carbon precursors, histidine and Fe(NO3)3 are used as ligands, and urea is used as a N source and template. After the conventional drying of the complex and following carbonization process, serial N-doped carbon materials are prepared. The composition and structure of the material are characterized, and the effect of the ligand is studied. The hierarchical porous structure facilitates the full exposition of N and trace of Fe active sites and benefits the transportation of electrolytes, thus improving the oxygen reduction reaction (ORR). The ORR performances show that the porous carbon has a positive initial and half-wave potential, good limiting current density, a near four-electron transfer process, and better methanol resistance and durability. The assembled ZAB exhibits high specific capacity (880.4 mAh gZn-1), excellent open-circuit voltage (1.54 V), and superior cycling stability, which further provides the significant potential for its application.

Three-dimensional porous nitrogen-doped carbon nanosheets with ultra-high surface area for high-performance oxygen reduction reaction electrocatalysts

A series of three-dimensional (3D) porous nitrogen-doped carbon nanosheets (PNCNs) have been successfully fabricated via a high-pressure carbonization followed by high-temperature thermal treatment. With the prolonging of thermal treatment time, the 3D PNCNs demonstrate several remarkable advantages for oxygen reduction reaction (ORR) electrocatalysts, including ultra-high specific surface area (more than 2100 m2/g−1), unique 3D porous structure, abundant defects, and suitable configuration of nitrogen. With these merits, the N-C-2 h based electrocatalyst exhibits outstanding ORR activities with a comparable onset potential of −40 mV (vs. Ag/AgCl), half-wave potential of −120 mV (vs. Ag/AgCl), satisfactory electron transfer number (4) and superior stability to those of commercial 20% Pt/C. The excellent electrochemical behaviors of 3D PNCNs are confirmed to be dominated by structural characteristics, which can be optimized by varying thermal treatment time. Our work offers a promising way for controllably constructing carbon-based materials with optimized ORR performance.

Zinc-Mediated Template Synthesis of Hierarchical Porous N-Doped Carbon Electrocatalysts for Efficient Oxygen Reduction.

The development of highly active and low-cost catalysts for use in oxygen reduction reaction (ORR) is crucial to many advanced and eco-friendly energy techniques. N-doped carbons are promising ORR catalysts. However, their performance is still limited. In this work, a zinc-mediated template synthesis strategy for the development of a highly active ORR catalyst with hierarchical porous structures was presented. The optimal catalyst exhibited high ORR performance in a 0.1 M KOH solution, with a half-wave potential of 0.89 V vs. RHE. Additionally, the catalyst exhibited excellent methanol tolerance and stability. After a 20,000 s continuous operation, no obvious performance decay was observed. When used as the air-electrode catalyst in a zinc-air battery (ZAB), it delivered an outstanding discharging performance, with peak power density and specific capacity as high as 196.3 mW cm-2 and 811.5 mAh gZn-1, respectively. Its high performance and stability endow it with potential in practical and commercial applications as a highly active ORR catalyst. Additionally, it is believed that the presented strategy can be applied to the rational design and fabrication of highly active and stable ORR catalysts for use in eco-friendly and future-oriented energy techniques.