Fe Single-atom Catalysts Research Articles

Electron transfer mediated activation of periodate by contaminants to generate 1O2 by charge-confined single-atom catalyst.

The electron transfer process (ETP) is able to avoid the redox cycling of catalysts by capturing electrons from contaminants directly. However, the ETP usually leads to the formation of oligomers and the reduction of oxidants to anions. Herein, the charge-confined Fe single-atom catalyst (Fe/SCN) with Fe-N3S1 configuration was designed to achieve ETP-mediated contaminant activation of the oxidant by limiting the number of electrons gained by the oxidant to generate 1O2. The Fe/SCN-activate periodate (PI) system shows excellent contaminant degradation performance due to the combination of ETP and 1O2. Experiments and DFT calculations show that the Fe/SCN-PI* complex with strong oxidizing ability triggers the ETP, while the charge-confined effect allows the single-electronic activation of PI to generate 1O2. In the Fe/SCN + PI system, the 100% selectivity dechlorination of ETP and the ring-opening of 1O2 avoid the generation of oligomers and realize the transformation of large-molecule contaminants into small-molecule biodegradable products. Furthermore, the Fe/SCN + PI system shows excellent anti-interference ability and application potential. This work pioneers the generation of active species using ETP's electron to activate oxidants, which provides a perspective on the design of single-atom catalysts via the charge-confined effect.

Selenic Acid Etching Assisted Atomic Engineering for Designing Metal-Semimetal Dual Single-Atom Catalysts for Enhanced CO2 Electroreduction.

Single-atom catalysts are promising for electrocatalytic CO2 conversion but face challenges in controllable syntheses. Herein, a facile selenic acid etching-assisted strategy has been developed to fabricate a hybrid metal-semimetal dual single-atom catalyst for electrocatalytic CO2 reduction. This strategy enables the simultaneous generation of monodisperse active sites and hierarchical morphologies with hollow nanostructures. The as-obtained catalyst with Fe-Se dual single-atom sites supported by porous nitrogen-doped carbon (FeSe-NC) shows exceptional catalytic activity and CO selectivity, delivering a Faradaic efficiency (FE) of >97% with industrially comparable jCO, superior to the Fe single-atom catalyst. Moreover, the FeSe-NC-based rechargeable Zn-CO2 battery delivers a high power density (2.01 mW cm-2) and outstanding FECO (>90%), as well as excellent cycling stability. Experimental results together with theoretical calculations reveal that the etching-induced defects and the Se-modulated Fe centers with asymmetrical polarized charge distributions synergistically facilitate the key intermediate *CO desorption and thus accelerate the CO2-to-CO conversion.

Coordination dependent photocatalytic peroxymonosulfate activation on biomass derived Fe single atom catalysts for atrazine degradation

Challenges associated with uncontrollable metal coordination structures in biomass-derived single-atom catalysts (SACs) and their intricate impacts on photocatalytic peroxymonosulfate (PMS) activation pose significant hurdles for the application of photo-Fenton technology towards wastewater treatment. Herein, we employed a co-pyrolysis strategy using Enteromorpha prolifera (E. prolifera) to synthesize Fe SACs with varying Fe–NX coordination, i.e., Fe–N5 and Fe–N6. Fe–N6-based SAC achieved over 80% atrazine (ATZ) degradation in 15 min, with a degradation rate of 0.13 min−1, representing 2.6-fold improvement over SAC with Fe–N5 structure. Experimental and simulation results revealed that Fe–N6 active sites acted as electron donors, enhancing the delocalization of π-electrons and improving photocatalytic PMS activation. This SAC also exhibited high selectivity for 1O2 degradation pathway and impressive ATZ degradation in seawater, with notable chlorine resistance, underscoring its potential in environmental pollutant remediation. This work unveils the catalyst structure-photocatalytic PMS activation performance relationship, offering avenue for developing more sustainable and efficient biomass-derived SACs for wastewater treatment.

Manipulating the Electronic Properties of an Fe Single Atom Catalyst via Secondary Coordination Sphere Engineering to Provide Enhanced Oxygen Electrocatalytic Activity in Zinc-Air Batteries.

Oxygen reduction and evolution reactions are two key processes in electrochemical energy conversion technologies. Synthesis of nonprecious metal, carbon-based electrocatalysts with high oxygen bifunctional activity and stability is a crucial, yet challenging step to achieving electrochemical energy conversion. Here, an approach to address this issue: synthesis of an atomically dispersed Fe electrocatalyst (Fe1/NCP) over a porous, defect-containing nitrogen-doped carbon support, is described. Through incorporation of a phosphorus atom into the second coordination sphere of iron, the activity and durability boundaries of this catalyst are pushed to an unprecedented level in alkaline environments, such as those found in a zinc-air battery. The rationale is to delicately incorporate P heteroatoms and defects close to the central metal sites (FeN4P1-OH) in order to break the local symmetry of the electronic distribution. This enables suitable binding strength with oxygenated intermediates. In situ characterizations and theoretical studies demonstrate that these synergetic interactions are responsible for high bifunctional activity and stability. These intrinsic advantages of Fe1/NCP enable a potential gap of a mere 0.65V and a high power density of 263.8mWcm-2 when incorporated into a zinc-air battery. These findings underscore the importance of design principles to access high-performance electrocatalysts for green energy technologies.

Constructing Asymmetric Fe-Nb Diatomic Sites to Enhance ORR Activity and Durability.

Iron-nitrogen-carbon (Fe-N-C) materials have been identified as a promising class of platinum (Pt)-free catalysts for the oxygen reduction reaction (ORR). However, the dissolution and oxidation of Fe atoms severely restrict their long-term stability and performance. Modulating the active microstructure of Fe-N-C is a feasible strategy to enhance the ORR activity and stability. Compared with common 3d transition metals (Co, Ni, etc.), the 4d transition metal atom Nb has fewer d electrons and more unoccupied orbitals, which could potentially forge a more robust interaction with the Fe site to optimize the binding energy of the oxygen-containing intermediates while maintaining stability. Herein, an asymmetric Fe-Nb diatomic site catalyst (FeNb/c-SNC) was synthesized, which exhibited superior ORR performance and stability compared with those of Fe single-atom catalysts (SACs). The strong interaction within the Fe-Nb diatomic sites optimized the desorption energy of key intermediates (*OH), so that the adsorption energy of Fe-*OH approaches the apex of the volcano plot, thus exhibiting optimal ORR activity. More importantly, introducing Nb atoms could effectively strengthen the Fe-N bonding and suppress Fe demetalation, causing an outstanding stability. The zinc-air battery (ZAB) and hydroxide exchange membrane fuel cell (HEMFC) equipped with our FeNb/c-SNC could deliver high peak power densities of 314 mW cm-2 and 1.18 W cm-2, respectively. Notably, the stable operation time for ZAB and HEMFC increased by 9.1 and 5.8 times compared to Fe SACs, respectively. This research offers further insights into developing stable Fe-based atomic-level catalytic materials for the energy conversion process.

Iron nanoparticles enhance the efficiency of single-atom Fenton-like catalyst by boosting Fe-NX activity

Single-atom catalysts (SACs) have been widely employed for the removal of organic contaminants via advanced oxidation processes (AOPs). The underlying principle involves central metal atoms that interact synergistically with surrounding atoms in specific ensembles to adsorb reactants and facilitate catalytic reactions. However, comprehensive studies exploring the ensemble effect of SACs in combination with metal nanoparticles relatively rare. In this study, we have synthesized a highly active iron single-atom catalyst (Fe@BC), which features both Fe-Nx coordination sites and iron nanoparticles. Fe@BC exhibits remarkable adsorption and degradation capabilities for bisphenol A across a wide pH range from 3.0 to 11.0. Scavenging experiments coupled with electron paramagnetic resonance analysis have revealed that •OH and O2•− are the key reactive oxygen species within the Fe@BC/PAA system, with •OH playing a crucial role in the removal of bisphenol A (BPA). Our comprehensive characterization analysis has validated the simultaneous presence of Fe nanoparticles and Fe-Nx sites, which are crucial for the catalyst's high activity. Furthermore, our experimental data highlight the importance of the synergistic effect between these two components. Density Functional Theory calculations have provided additional insights, showing that the presence of iron nanoparticles significantly boosts the Fe-Nx sites' activity. This enhancement is achieved by increasing adsorption energy, promoting electron transfer to peracetic acid (PAA), and decreasing the energy barrier for the formation of active species. These findings are vital for the strategic refinement of Fe single-atom catalysts for PAA-based advanced oxidation processes.

Inflammation-free electrochemical in vivo sensing of dopamine with atomic-level engineered antioxidative single-atom catalyst

Electrochemical methods with tissue-implantable microelectrodes provide an excellent platform for real-time monitoring the neurochemical dynamics in vivo due to their superior spatiotemporal resolution and high selectivity and sensitivity. Nevertheless, electrode implantation inevitably damages the brain tissue, upregulates reactive oxygen species level, and triggers neuroinflammatory response, resulting in unreliable quantification of neurochemical events. Herein, we report a multifunctional sensing platform for inflammation-free in vivo analysis with atomic-level engineered Fe single-atom catalyst that functions as both single-atom nanozyme with antioxidative activity and electrode material for dopamine oxidation. Through high-temperature pyrolysis and catalytic performance screening, we fabricate a series of Fe single-atom nanozymes with different coordination configurations and find that the Fe single-atom nanozyme with FeN4 exhibits the highest activity toward mimicking catalase and superoxide dismutase as well as eliminating hydroxyl radical, while also featuring high electrode reactivity toward dopamine oxidation. These dual functions endow the single-atom nanozyme-based sensor with anti-inflammatory capabilities, enabling accurate dopamine sensing in living male rat brain. This study provides an avenue for designing inflammation-free electrochemical sensing platforms with atomic-precision engineered single-atom catalysts.

Sublimation Transformation Synthesis of Dual-Atom Fe Catalysts for Efficient Oxygen Reduction Reaction.

Dual-atom catalysts (DACs) have garnered significant interest due to their remarkable catalytic reactivity. However, achieving atomically precise control in the fabrication of DACs remains a major challenge. Herein, we developed a straightforward and direct sublimation transformation synthesis strategy for dual-atom Fe catalysts (Fe2/NC) by utilizing in situ generated Fe2Cl6(g) dimers from FeCl3(s). The structure of Fe2/NC was investigated by aberration-corrected transmission electron microscopy and X-ray absorption fine structure (XAFS) spectroscopy. As-obtained Fe2/NC, with a Fe-Fe distance of 0.3 nm inherited from Fe2Cl6, displayed superior oxygen reduction performance with a half-wave potential of 0.90 V (vs. RHE), surpassing commercial Pt/C catalysts, Fe single-atom catalyst (Fe1/NC), and its counterpart with a common and shorter Fe-Fe distance of ~0.25 nm (Fe2/NC-S). Density functional theory (DFT) calculations and microkinetic analysis revealed the extended Fe-Fe distance in Fe2/NC is crucial for the O2 adsorption on catalytic sites and facilitating the subsequent protonation process, thereby boosting catalytic performance. This work not only introduces a new approach for fabricating atomically precise DACs, but also offers a deeper understanding of the intermetallic distance effect on dual-site catalysis.

Construction of N-Fe-S bridge in atomic iron catalyst for boosting Fenton-like reactions

Constructing the coordination environment of single-atom catalysts (SACs) can be an attractive technical strategy to regulate the generation of reactive oxygen species for Fenton-like reactions. Herein, we have constructed an asymmetric coordination of Fe single-atom catalyst (FeSA-NS-PCNS) with abundant N-Fe-S bridge (FeSA-N3S1) for robust Fenton-like reactions. 82.5 % of singlet oxygen (1O2) selectivity and high turnover frequency of bisphenol A degradation (0.568 min−1) were achieved at mild conditions. Experimental works and theoretical analyses illustrated that S doping breaks the inert environment of the original N-Fe-N symmetric coordination equilibrium and modulates the electron density of the atomic Fe center, which is beneficial for boosting PMS adsorption and reducing the energy barriers of vital *OH and *O intermediates. The coupling between the FeSA-N3S1 interface and peroxymonosulfate molecule boosts in-situ electron transfer through the N-Fe-S bridge, which induces more electron flow from the low valence Fe to OH* on the surface of Fe-*O-H, forming a high yield of 1O2. Moreover, we designed the Fenton-like reactions by FeSA-NS-PCNS membrane reactor for an efficient contaminant removal rate of over 90 % even after 11 cycles. This work provides a novel perspective on developing SACs with asymmetric coordination to regulate reactive oxygen species for the treatment of organic contaminants in water bodies.

Nonmetal Doping Modulates Fe Single-Atom Catalysts for Enhancement in Peroxidase Mimicking via Symmetry Disruption, Distortion, and Charge Transfer.

Developing biomimetic catalysts with excellent peroxidase (POD)-like activity has been a long-standing goal for researchers. Doping nonmetallic atoms with different electronegativity to boost the POD-like activity of Fe-N-C single-atom catalysts (SACs) has been successfully realized. However, the introduction of heteroatoms to regulate the coordination environment of the central Fe atom and thus influence the activation of the H2O2 molecule in the POD-like reaction has not been extensively explored. Herein, the effect of different doping sites and numbers of heteroatoms (P, S, B, and N) on the adsorption and activation of H2O2 molecules of Fe-N sites is thoroughly investigated by density functional theory (DFT) calculations. In general, alternation in the catalytic efficiency directly depends on the transfer of electrons and the geometrical shifts near the Fe-N site. First, the symmetry disruption of the Fe-N4 site by P, S, and B doping is beneficial to the activation of H2O2 due to a significant reduction in the adsorption energies. In some cases, without Fe-N4 site disruption, the configurations fail to modulate the adsorption behavior of H2O2. Second, Fe-N-P/S configurations exhibit a stronger affinity for H2O2 molecules due to the significant out-of-plane distortions induced by larger atomic radii of P and S. Moreover, the synergistic effects of Fe and doping atoms P, S, and B with weaker electronegativity than that of N atoms promote electron donation to generated oxygen-containing intermediates, thus facilitating subsequent electron transfer with other substrates. This work demonstrates the critical role of tuning the coordinating environment of Fe-N active centers by heteroatom doping and provides theoretical guidance for controlling the types by breaking the symmetry of SACs to achieve optimal POD-like catalytic activity and selectivity.

Development of Iron‐Based Single Atom Materials for General and Efficient Synthesis of Amines

AbstractEarth abundant metal‐based heterogeneous catalysts with highly active and at the same time stable isolated metal sites constitute a key factor for the advancement of sustainable and cost‐effective chemical synthesis. In particular, the development of more practical, and durable iron‐based materials is of central interest for organic synthesis, especially for the preparation of chemical products related to life science applications. Here, we report the preparation of Fe‐single atom catalysts (Fe‐SACs) entrapped in N‐doped mesoporous carbon support with unprecedented potential in the preparation of different kinds of amines, which represent privileged class of organic compounds and find increasing application in daily life. The optimal Fe‐SACs allow for the reductive amination of a broad range of aldehydes and ketones with ammonia and amines to produce diverse primary, secondary, and tertiary amines including N‐methylated products as well as drugs, agrochemicals, and other biomolecules (amino acid esters and amides) utilizing green hydrogen.

Development of Iron-Based Single Atom Materials for General and Efficient Synthesis of Amines.

Earth abundant metal-based heterogeneous catalysts with highly active and at the same time stable isolated metal sites constitute a key factor for the advancement of sustainable and cost-effective chemical synthesis. In particular, the development of more practical, and durable iron-based materials is of central interest for organic synthesis, especially for the preparation of chemical products related to life science applications. Here, we report the preparation of Fe-single atom catalysts (Fe-SACs) entrapped in N-doped mesoporous carbon support with unprecedented potential in the preparation of different kinds of amines, which represent privileged class of organic compounds and find increasing application in daily life. The optimal Fe-SACs allow for the reductive amination of a broad range of aldehydes and ketones with ammonia and amines to produce diverse primary, secondary, and tertiary amines including N-methylated products as well as drugs, agrochemicals, and other biomolecules (amino acid esters and amides) utilizing green hydrogen.

Modulation of Photocatalytic CO2 Reduction by n-p Codoping Engineering of Single-Atom Catalysts.

Transition metal (TM) single-atom catalysts (SACs) have been widely applied in photocatalytic CO2 reduction. In this work, n-p codoping engineering is introduced to account for the modulation of photocatalytic CO2 reduction on a two-dimensional (2D) bismuth-oxyhalide-based cathode by using first-principles calculation. n-p codoping is established via the Coulomb interactions between the negatively charged TM SACs and the positively charged Cl vacancy (VCl) in the dopant-defect pairs. Based on the formation energy of charged defects, neutral dopant-defect pairs for the Fe, Co, and Ni SACs (PTM0) and the -1e charge state of the Cu SAC-based pair (PCu-1) are stable. The electrostatic attraction of the n-p codoping strengthens the stability and solubility of TM SACs by neutralizing the oppositely charged VCl defect and TM dopant. The n-p codoping stabilizes the electron accumulation around the TM SACs. Accumulated electrons modify the d-orbital alignment and shift the d-band center toward the Fermi level, enhancing the reducing capacity of TM SACs based on the d-band theory. Besides the electrostatic attraction of the n-p codoping, the PCu-1 also accumulates additional electrons surrounding Cu SACs and forms a half-occupied dx2-y2 state, which further upshifts the d-band center and improves photocatalytic CO2 reduction. The metastability of Cl multivacancies limits the concentration of the n-p pairs with Cl multivacancies (PTM@nCl (n > 1)). Positively charged centers around the PTM@nCl (n > 1) hinders the CO2 reduction by shielding the charge transfer to the CO2 molecule.

Nanoarchitectonics of Fe single-atom catalyst modified with flexible wearable patch for sweat biomarker analysis

In personalized medical diagnostics and health monitoring, the analysis of biomarkers in sweat, such as uric acid (UA) and dopamine (DA), offers valuable insights into metabolic states. This study introduces a flexible wearable patch based on Fe single-atom catalysts (FeSAs) to simultaneously detect UA and DA in sweat for comprehensive health assessment. Our wearable patch demonstrated linear response ranges of 1–800 μM for UA and 1–500 μM for DA, with detection limits of 2.68 μM and 3.76 μM, and sensitivities of 0.015 μA μM−1 cm−2 and 0.0176 μA μM−1 cm−2, respectively. Additionally, we integrated agarose hydrogel into the wearable patches, optimizing sweat collection efficiency at agarose concentrations ranging from 2 % to 3.8 %. This innovation enables effective biomarker enrichment directly from the skin surface. In conclusion, our study presents an innovative FeSAs-based electrocatalyst capable of simultaneous detection of low-concentration UA and DA biomarkers.

Atomically dispersed Fe-N5 sites with optimized electronic structure for sustainable wastewater purification via efficient Fenton-like catalysis

Herein, a single-atom catalyst (SAC) featuring Fe-N5 sites (FeNC) with optimized electronic structures was constructed and applied to activate peroxymonosulfate (PMS) for wastewater purification. The high-coordinated Fe-N5 sites was obtained by creating a high-nitrogen gas environment around fully exposed Fe atomic sites on chitosan surface during pyrolysis. The FeNC/PMS system demonstrated excellent decontamination capability, superior anti-pH interference ability, while also exceptional durability in a continuous-flow catalytic filtration reactor. Experiments and density functional theory calculations unveiled that Fe-N5 site was the active center. Meaningfully, neighboring carbonyl groups narrowed the gap between d-band center of Fe 3d and Fermi level, which increased the adsorption energy of PMS on Fe-N5 sites, thus lowering the energy barrier for singlet oxygen generation. This study brings a vivid electronic structure optimization strategy for enhancing the catalytic activity of Fe SAC as well as guiding the selection of desirable catalysts for wastewater purification by Fenton-like chemistry.

Atomically dispersed Fe–N4 sites activated 3D-on-2D derived porous carbon structure toward superior oxygen reduction reaction

The oxygen reduction reaction (ORR) is a crucial step in the energy transformation devices, which requires the fabrication of a cost-effective and energy-efficient Fe single-atom catalyst (SAC) to substitute platinum. However, achieving a controllable synthesis of Fe SAC is a formidable challenge. In this study, a Fe SAC with a novel 3D-on-2D architecture was fabricated by coating 3D metal-organic frameworks (MOFs) over the surface of 2D reduced graphene oxide (rGO). In-situ combining MOF and rGO in a composite structure by adjusting their weight proportion is a key to preparing an active 3D-on-2D structured catalyst with FeN4 active sites. Thanks to the favorable conductivity of the 2D rGO-derived carbon structure and the 3D MOF structure exposing an enhanced density of FeN4 sites, FeNC@rGO-2 demonstrates exceptional ORR activity. It performs more effectively than commercial Pt/C, exhibiting excellent half-wave potentials of 0.887, 0.705, and 0.741 V in alkaline, neutral, and acidic solutions respectively. Impressively, FeNC@rGO-2 exhibits excellent stability and methanol tolerance. When FeNC@rGO-2 is assembled as cathode catalyst in Zinc-air batteries (ZAB) and microbial fuel cells (MFC), FeNC@rGO-2-ZAB reveals outstanding power density (393 mW cm−2) and good charge/discharge cycling stability. Amazingly, FeNC@rGO-2-MFC also shows superior power density (2810 ± 19 mW m−2) and efficiency of electron recovery. This study reveals that FeNC@rGO-2 has extremely high application value in energy conversion devices oriented for alkaline and neutral electrolytes.

Unveiling structural evolution of Fe single atom catalyst in nitrate reduction for enhanced electrocatalytic ammonia synthesis

Unveiling structural evolution of Fe single atom catalyst in nitrate reduction for enhanced electrocatalytic ammonia synthesis

Creation of intrinsic defects on ZIF-8 particles to facilitate electrochemical reduction of CO2 over Fe single-atom catalyst

The fabrication of various defects on the surface of metal single-atom catalysts can improve their electrochemical CO2 reduction reaction (CO2RR) ability, and the current mainstream research focuses on the defect modification of heteroatom doping, while there are fewer studies on intrinsic defects on carbon substrates. Herein, a series of catalysts with both Fe-N4 sites and intrinsic defects were synthesized on the ZIF-8 surface by pyrolytic etching at a suitable temperature under ammonia atmosphere. Electrochemical tests in an H-cell showed that the catalyst achieved CO Faradaic efficiency (FECO) of 96.9 % and CO partial current density (JCO) of 9.088 mA cm−2 at −0.6 V. Through further studies, we introduced a “585” ring structure to describe these intrinsic defects and found that these intrinsic defects on the carbon-based surface can act as active sites to promote CO2RR along with the Fe-N4 sites. This work provides a reference for the study of intrinsic defect-modified single atomic materials.

Boosting Electrochemiluminescence Performance of a Dual-Active Site Iron Single-Atom Catalyst-Based Luminol-Dissolved Oxygen System via Plasmon-Induced Hot Holes.

Due to the commonly low content of biomarkers in diseases, increasing the sensitivity of electrochemiluminescence (ECL) systems is of great significance for in vitro ECL diagnosis and biodetection. Although dissolved O2 (DO) has recently been considered superior to H2O2 as a coreactant in the most widely used luminol ECL systems owing to its improved stability and less biotoxicity, it still has unsatisfactory ECL performance because of its ultralow reactivity. In this study, an effective plasmonic luminol-DO ECL system has been developed by complexing luminol-capped Ag nanoparticles (AgNPs) with plasma-treated Fe single-atom catalysts (Fe-SACs) embedded in graphitic carbon nitride (g-CN) (pFe-g-CN). Under optimal conditions, the performance of the resulting ECL system could be markedly increased up to 1300-fold compared to the traditional luminol-DO system. Further investigations revealed that duple binding sites of pFe-g-CN and plasmonically induced hot holes that disseminated from AgNPs to g-CN surfaces lead to facilitate significantly the luminous reaction process of the system. The proposed luminol-DO ECL system was further employed for the stable and ultrasensitive detection of prostate-specific antigen in a wide linear range of 1.0 fg/mL to 1 μg/mL, with a pretty low limit of detection of 0.183 fg/mL.

In Situ Symbiosis of Cerium Oxide Nanophase for Enhancing the Oxygen Electrocatalysis Performance of Single-Atom Fe─N─C Catalyst with Prolonged Stability for Zinc-Air Batteries.

The Fenton reaction, induced by the H2O2 formed during the oxygen reduction reaction (ORR) process leads to significant dissolution of Fe, resulting in unsatisfactory stability of the iron-nitrogen-doped carbon catalysts (Fe-NC). In this study, a strategy is proposed to improve the ORR catalytic activity while eliminating theeffectof H2O2 by introducing CeO2 nanoparticles. Transmission electron microscopy and subsequent characterizations reveal that CeO2 nanoparticles are uniformly distributed on the carbon substrate, with atomically dispersed Fe single-atom catalysts (SACs) adjacent to them. CeO2@Fe-NC achieves a half-wave potential of 0.89V and a limiting current density of 6.2mAcm-2, which significantly outperforms Fe-NC and commercial Pt/C. CeO2@Fe-NC also shows a half-wave potential loss of only 1% after 10000 CV cycles, which is better than that of Fe-NC (7%). Further, H2O2 elimination experiments show that the introduction of CeO2 significantly accelerate the decomposition of H2O2. In situ Raman spectroscopy results suggest that CeO2@Fe-NC significantly facilitates the formation of ORR intermediates compared with Fe-NC. The Zn-air batteries utilizing CeO2@Fe-NC cathodes exhibit satisfactory peak power density and open-circuit voltage. Furthermore, theoretical calculations show that the introduction of CeO2 enhances the ORR activity of Fe-NC SAC. This study provides insights for optimizing SAC-based electrocatalysts with high activity and stability.