Fe Active Sites Research Articles

Construction of Fe(III) Active Sites on Phenanthroline-Grafted g-C3N4: Reduced Work Function and Enhanced Intramolecular Charge Transfer for Efficient N2 Photofixation.

Photocatalytic nitrogen fixation is one of the important pathways for green and sustainable ammonia synthesis, but the extremely high bonding energy of the N≡N triple bond makes it difficult for conventional nitrogen fixation photocatalysts to directly activate and hydrogenate. Given this, we covalently grafted the phenanthroline unit onto graphitic carbon nitride nanosheets (CN) by the simple thermal oxidation method and complexed it with transition metal Fe3+ ions to obtain stable dispersed Fe active sites, which can significantly improve the photocatalytic activity. The Fe(III)-4-P-CN photocatalyst morphology consists of porous lamellar structures internally connected by nanowires. The special morphology of the catalysts gives them excellent nitrogen fixation performance, with an average NH3 yield of 492.9 μmol g-1 h-1, which is 6.5 times higher than that of the pristine CN, as well as better photocatalytic cycling stability. Comprehensive experiments and density-functional theory results show that Fe(III)-4-P-CN is more favorable than pristine CN for *N2 activation, effectively lowering the reaction energy barrier. Moreover, other byproducts (such as nitrate and H2O2) are also produced during the photocatalytic nitrogen fixation process, which also provides a new way for nitrogen-fixing photocatalysts to achieve multifunctional applications.

Cu, Fe, N‐doped Carbon Nanotubes Prepared through Silica Coating for Selective Oxygen Reduction to Water in Acidic Media

AbstractWe report Cu, Fe, N‐doped carbon nanotubes, (Cu,Fe)−N−CNT, as electrocatalysts for the oxygen reduction reaction (ORR) in acidic media. (Cu,Fe)−N−CNT was prepared using a silica coating method in pyrolysis to minimize the formation of carbon‐coated metal oxide or carbide nanoparticles, which are known to be inactive for the H2O2 reduction. (Cu,Fe)−N−CNT shows a turnover frequency of 0.66 e− site−1 s−1 at +0.8 V vs. RHE and H2O2 yields of <1 % for the ORR with a utilization factor of active sites of 82 %. Kinetic analysis reveals that 4e− transfer rates for (Cu,Fe)−N−CNT are higher than those of a monometallic counterpart of Fe−N−CNT. In situ X‐ray absorption spectroscopy enables us to determine redox potentials: E°’(FeIII/FeII)=0.65 V vs. RHE and E°’(CuII/CuI)=0.45 V for (Cu,Fe)−N−CNT, and E°’(FeIII/FeII)=0.65 V for Fe−N−CNT. These results indicate that bimetallic doping into carbon nanotubes gives the effect on kinetic parameters but not on thermodynamic ones. In other words, there is no direct electronic interactions between the Cu and Fe active sites for (Cu,Fe)‐N‐CNT because such interactions should modulate their redox potentials.

Enhancing Electrocatalytic CO2-to-CO Conversion by Weakening CO Binding through Nitrogen Integration in the Metallic Fe Catalyst.

Metallic iron (Fe) typically demonstrates the unfavorable catalytic activity for the CO2 reduction reaction (CO2RR), mainly attributed to the excessively strong binding of CO products on Fe sites. Toward this end, we employed an effective approach involving electronic structure modulation through nitrogen (N) integration to enhance the performance of the CO2RR. Here, an efficient catalyst has been developed, composed of N-doped metallic iron (Fe) nanoparticles encapsulated in a porous N-doped carbon framework. Notably, this N-integrated Fe catalyst displays significantly enhanced performance in the electrocatalytic reduction of CO2, yielding the highest CO Faradaic efficiency of 97.5% with a current density of 6.68 mA cm-2 at -0.7 V versus the reversible hydrogen electrode. The theoretical calculations, combined with the in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy study, reveal that N integration modulates the electron density around Fe, resulting in the weakening of the binding strength between the Fe active sites and *CO intermediates, consequently promoting the desorption of CO and the overall CO2RR process.

Organic-inorganic hybrid interfaces with π-d electron coupling for preventing metal and sulfur leaching toward enhanced oxygen evolution reaction

Transition metal sulfides (TMSs) catalysts with high catalytic oxygen evolution reaction (OER) activity have been extensively studied, especially Fe and Co-based sulfides. Fe and Co active sites with a strong synergistic effect, which can adjust the electron density distribution and effectively improve the electrocatalytic OER activity. However, TMSs have poor stability in alkaline environment caused by metal ions and sulfur elements are facilitated to dissolve. In this work, TMSs was modified by polyaniline (PANI) to inhibit the precipitation of iron, cobalt, and sulfur elements and enhance its stability under alkaline conditions. Moreover, π-d structure can also be formed by the coating of PANI, which can further adjust its own electronic structure on the basis of stabilizing the TMSs structure, so as to improve the electrochemical performance, rendering them to stably operate at harsh environment for more than 90 h. These findings offer new guidance for improving the electrocatalytic stability of TMSs.

Coexisting single-atomic Fe and Fe2O3 on nitrogen-deficient g-C3N4 with enriched Fenton-like oxidation and photocatalytic performances for tetracycline degradation: DFT calculation, degradation mechanism and toxicity evaluation

The regulation of heterogeneous material properties to strengthen the peroxymonosulfate activation to destroy refractory pharmaceuticals remains a challenge. Herein, a promising nitrogen-deficient catalyst (FeCN) with single atom Fe and Fe2O3 nanoparticles dispersing on g-C3N4 matrix was synthesized and applied as a competent peroxydisulfate (PDS) activator for tetracycline (TC) degradation under visible light. The K-edge X-ray absorption fine structures and 57Fe Mössbauer measurements confirmed the unique configuration of Fe2O3 and single atom Fe active sites (pyrrolic and pyridinic FeN4) induced by the neighbouring nitrogen vacancies. The theory calculations and experiments provided a deep insight into the PDS activation and TC degradation via radical and non-radical pathways. The pyrrolic FeN4 active sites dominated the electron transfer, while the pyridinic FeN4 and Fe2O3 decomposed PDS to produce free radicals. The synergistic effect between the Fenton-like oxidation and photocatalysis is responsible for efficient TC degradation. This study offers a new strategy by integrating novel catalysts and advanced oxidation technology for effective wastewater purification.

Iron catalysts enhanced by ultrasound for methane decomposition and hydrogen generation

Clean hydrogen production offers a viable alternative in the transition to a greener and more sustainable energy future. This study introduces a novel method for enhancing Fe/Al2O3 catalysts using La2O3 and CeO2 doping, aimed at improving hydrogen production via methane decomposition. It addresses the critical challenge of modulating metal-support interaction. Employing ultrasonication in the catalyst preparation, we observed through XRD, H2-TPR, H2 chemisorption, Raman spectroscopy, TGA, and TPO analyses that La2O3 addition prevents FeAl2O4 formation and increases Fe reduction and active sites. Catalysts assisted by ultrasound outperform traditional methods, exhibiting a consistent and significant increase in conversion and yield efficiencies. The La2O3-modified catalysts outperformed the standard Fe/Al2O3 catalyst in methane decomposition. At 800 °C, they demonstrated enhanced activity and stability under demanding conditions, achieving a methane conversion of 93% and hydrogen yield of 84%. This approach boosts hydrogen production and contributes to the development of sustainable and efficient energy solutions.

A High-Entropy Single-Atom Catalyst Toward Oxygen Reduction Reaction in Acidic and Alkaline Conditions.

The design of high-entropy single-atom catalysts (HESAC) with 5.2 times higher entropy compared to single-atom catalysts (SAC) is proposed, by using four different metals (FeCoNiRu-HESAC) for oxygen reduction reaction (ORR). Fe active sites with intermetallic distances of 6.1Å exhibit a low ORR overpotential of 0.44V, which originates from weakening the adsorption of OH intermediates. Based on density functional theory (DFT) findings, the FeCoNiRu-HESAC witha nitrogen-doped sample were synthesized. The atomic structures are confirmed with X-ray photoelectron spectroscopy (XPS), X-ray absorption (XAS), and scanning transmission electron microscopy (STEM). The predicted high catalytic activity is experimentally verified, finding that FeCoNiRu-HESAC has overpotentials of 0.41and 0.37V with Tafel slopes of 101 and 210mVdec-1 at the current density of 1mAcm-2 and the kinetic current densities of 8.2 and 5.3mAcm-2, respectively, in acidic and alkaline electrolytes. These results are comparable with Pt/C. The FeCoNiRu-HESAC is used for Zinc-air battery applications with an open circuit potential of 1.39V and power density of 0.16Wcm-2. Therefore, a strategy guided by DFT is provided for the rational design of HESAC which can be replaced with high-cost Pt catalysts toward ORR and beyond.

Tailoring Oxygen Reduction Reaction Kinetics of Fe-N-C Catalyst via Spin Manipulation for Efficient Zinc-Air Batteries.

The interaction between oxygen species and metal sites of various orbitals exhibits intimate correlation with the oxygen reduction reaction (ORR) kinetics. Herein, a new approach for boosting the inherent ORR activity of atomically dispersed Fe-N-C matrix is represented by implanting Featomic clusters nearby. The as-prepared catalyst delivers excellent ORR activity with half-wave potentials of 0.78 and 0.90V in acidic and alkaline solutions, respectively. The decent ORR activity can also be validated from the high-performance rechargeable Zn-air battery. The experiments and density functional theory calculations reveal that the electron spin-state of monodispersed Fe active sites is transferred from the low spin (LS, t2g 6 eg 0) to the medium spin (MS, t2g 5 eg 1) due to the involvement of Fe atomic clusters, leading to the spin electron filling in σ∗ orbit, by which it favors OH- desorption and in turn boosts the reaction kinetics of the rate-determining step. This work paves a solid way for rational design of high-performance Fe-based single atom catalysts through spin manipulation.

Visible-light photocatalytic O2-to-H2O2 via nitrogen-graphene quantum dots-modified Bi2Fe4O9 for synchronizing the reduction of Cr(VI) and oxidation of organic contaminants: Kinetics, mechanism, and performance

Synergistic coexistence of toxic chromium and organic contaminants in wastewater has made treatments highly complicated. As solar-driven wastewater treatments become increasingly environmentally and economically attractive, a photocatalyst (denoted as N-GQDs/Bi2Fe4O9) is developed for photocatalytic reduction of Cr(VI) and simultaneous oxidation of organic contaminants in wastewater. Incorporating N-GQDs (as electron reservoir) into Bi2Fe4O9 modulates the band structure (from 2.40 to 2.24 eV), facilitating charge transfer and electron accumulation at N-GQDs. Due to the photo-Fenton synergistic reaction between N-GQDs/Bi2Fe4O9 photocatalysis process, N-GQDs/ Bi2Fe4O9 demonstrates excellent H2O2 generation (1.64 μM min−1) and H2O2 activation (0.0063 min−1) performance, leading to generation of more highly reactive species (i.e., OH radicals), achieving BPA removal of 99.9 % under visible-light irradiation for 100 min. Interestingly, the photo-Fenton synergistic reaction enhances the reduction of Cr(VI) (99.8 %), while the Fe(II) active sites on the N-GQDs/Bi2Fe4O9 can also promote the synchronized Cr(VI) reduction. Also, the accumulated electron around N-GQDs enhances redox cycles of Fe(II)/Fe(III) reactions to realize the sustainable photo-Fenton catalytic reaction. This new N-GQDs/Bi2Fe4O9 photocatalyst demonstrates the feasibility of concurrent reduction of toxic Cr(VI)-to-Cr(III) and oxidation of organic contaminants in wastewater with a simple process via nearly unlimited solar energy.

Regulated Dual Defects of Bridging Organic and Terminal Inorganic Ligands in Iron-based Metal-Organic Framework Nodes for Efficient Photocatalytic Ammonia Synthesis.

Engineering advantageous defects to construct well-defined active sites in catalysts is promising but challenging to achieve efficient photocatalytic NH3 synthesis from N2 and H2O due to the chemical inertness of N2 molecule. Here, we report defective Fe-based metal-organic framework (MOF) photocatalysts via a non-thermal plasma-assisted synthesis strategy, where their NH3 production capability is synergistically regulated by two types of defects, namely, bridging organic ligands and terminal inorganic ligands (OH- and H2O). Specially, the optimized MIL-100(Fe) catalysts, where there are only terminal inorganic ligand defects and coexistence of dual defects, exhibit the respective 1.7- and 7.7-fold activity enhancement comparable to the pristine catalyst under visible light irradiation. As revealed by experimental and theoretical calculation results, the dual defects in the catalyst induce the formation of abundant and highly accessible coordinatively unsaturated Fe active sites and synergistically optimize their geometric and electronic structures, which favors the injection of more d-orbital electrons in Fe sites into the N2 π* antibonding orbital to achieve N2 activation and the formation of a key intermediate *NNH in the reaction. This work provides a guidance on the rational design and accurate construction of porous catalysts with precise defective structures for high-performance activation of catalytic molecules.

Regulated Dual Defects of Bridging Organic and Terminal Inorganic Ligands in Iron‐based Metal‐Organic Framework Nodes for Efficient Photocatalytic Ammonia Synthesis

AbstractEngineering advantageous defects to construct well‐defined active sites in catalysts is promising but challenging to achieve efficient photocatalytic NH3 synthesis from N2 and H2O due to the chemical inertness of N2 molecule. Here, we report defective Fe‐based metal‐organic framework (MOF) photocatalysts via a non‐thermal plasma‐assisted synthesis strategy, where their NH3 production capability is synergistically regulated by two types of defects, namely, bridging organic ligands and terminal inorganic ligands (OH− and H2O). Specially, the optimized MIL‐100(Fe) catalysts, where there are only terminal inorganic ligand defects and coexistence of dual defects, exhibit the respective 1.7‐ and 7.7‐fold activity enhancement comparable to the pristine catalyst under visible light irradiation. As revealed by experimental and theoretical calculation results, the dual defects in the catalyst induce the formation of abundant and highly accessible coordinatively unsaturated Fe active sites and synergistically optimize their geometric and electronic structures, which favors the injection of more d‐orbital electrons in Fe sites into the N2 π* antibonding orbital to achieve N2 activation and the formation of a key intermediate *NNH in the reaction. This work provides a guidance on the rational design and accurate construction of porous catalysts with precise defective structures for high‐performance activation of catalytic molecules.

Inter-site structural heterogeneity induction of single atom Fe catalysts for robust oxygen reduction

Metal-nitrogen-carbon catalysts with hierarchically dispersed porosity are deemed as efficient geometry for oxygen reduction reaction (ORR). However, catalytic performance determined by individual and interacting sites originating from structural heterogeneity is particularly elusive and yet remains to be understood. Here, an efficient hierarchically porous Fe single atom catalyst (Fe SAs-HP) is prepared with Fe atoms densely resided at micropores and mesopores. Fe SAs-HP exhibits robust ORR performance with half-wave potential of 0.94 V and turnover frequency of 5.99 e−1s−1site−1 at 0.80 V. Theoretical simulations unravel a structural heterogeneity induced optimization, where mesoporous Fe-N4 acts as real active centers as a result of long-range electron regulation by adjacent microporous sites, facilitating O2 activation and desorption of key intermediate *OH. Multilevel operando characterization results identify active Fe sites undergo a dynamic evolution from basic Fe-N4 to active Fe-N3 under working conditions. Our findings reveal the structural origin of enhanced intrinsic activity for hierarchically porous Fe-N4 sites.

Acid treatment enhances the methane combustion activity of LaFeO3 perovskite catalyst

The catalytic combustion of methane has gained much attention as a sustainable technology, due to concerns about the environmental impact of unburnt methane emissions from the natural gas vehicles. Researchers have explored alternatives to precious metal catalysts for methane combustion, with a focus on perovskite oxides known for their excellent activity and sintering-resistance capacity. In this study, LaFeO3 perovskite material was synthesized and subsequently subjected to a nitric acid etching treatment to modify its surface. It was found that the acid preferentially dissolved La cations from LaFeO3 surface while the perovskite phase was unchanged, as a consequence, the etched LaFeO3 shows improvement in methane combustion activity. The best performance was achieved in the sample with one-hour surface etched treatment, which suggests that the appropriate surface reconstruction induced by acid treatment promotes the formation of more active Fe sites on the surface and reduces the energic barriers of methane activation. This work presents a straightforward and effective approach to tailor the exposed surface properties of perovskites, thereby enhancing their activity in hydrocarbon combustion reactions.

Boosting selective hydrogenation of α,β-unsaturated aldehydes through constructing independent Pt and Fe active sites on support

The alloy catalysts usually exhibited excellent catalytic synergy owing to the electronic and ensemble effect. However, the process of alloying makes the displacement of the d-band center from the Fermi level, decreasing the adsorption strength of reactant molecules. Herein, we constructed the spatial separation catalyst in which the independent Pt and FeOx nanoparticles were uniformly distributed on SBA-15 support (denoted as Pt = Fe/SBA-15), which exhibits remarkable efficiency in the hydrogenation of α,β-unsaturated aldehydes, i.e. with a 4 fold higher than the corresponding alloy catalyst in reaction rate, and a 4 fold increase in selectivity for cinnamalcohol production compared to the single Pt catalyst. It is found that Pt primarily catalyzes the H2 dissociative adsorption into H*, while FeOx mainly catalyzes the reaction between H* and aldehydes, forming alcohols. Assuming that the rate-determining-step is the H-spillover from Pt to Fe, the two cascade reactions are interconnected. To confirm this mechanism, we employ a physical mixture catalyst of Pt/SBA-15 and FeOx/SBA-15, where its catalytic activity lies between Pt = Fe/SBA-15 and alloy materials. The catalysts’ structures are well characterized by STEM and EDS mapping analysis, and the mechanism is supported by experimental data and DFT calculations. The research we conducted offers a new perspective into the cooperative catalysis, achieved by coupling independent active centers in thermos-hydrogenation reactions.

Unraveling Valence Electron Number Dependent Excitonic Effects over M1-N3C1 Sites in Single-Atom Catalysts.

Excitonic effects significantly influence the selective generation of reactive oxygen species and photothermal conversion efficiency in photocatalytic reactions; however, the intrinsic factors governing excitonic effects remain elusive. Herein, a series of single-atom catalysts with well-defined M1-N3C1 (M = Mn, Fe, Co, and Ni) active sites are designed and synthesized to investigate the structure-activity relationship between photocatalytic materials and excitonic effects. Comprehensive characterization and theoretical calculations unveil that excitonic effects are positively correlated with the number of valence electrons in single metal atoms. The single Mn atom with 5.93 valence electrons exhibits the weakest excitonic effects, which dominate superoxide radical (O2•-) generation through charge transfer and enhance photothermal conversion efficiency. Conversely, the single Ni atom with 9.27 valence electrons exhibits the strongest excitonic effects, dominating singlet oxygen (1O2) generation via energy transfer while suppressing photothermal conversion efficiency. Based on the valence electron number dependent excitonic effects, a reaction environment with hyperthermia and abundant cytotoxic O2•- is designed, achieving efficient and stable water disinfection. This work reveals single metal atom dependent excitonic effects and presents an atomic-level methodology for catalytic application targeted reaction environment tailoring.

Pre-adsorption effect of salicylhydroxamic acid on the separation performance and mechanism of chlorite and specularite

In this study, salicylhydroxamic acid (SHA) was added before the depressant dextrin during flotation process as a pre-adsorbent to pre-adsorb chlorite subordinating elements (Al) and hinder the subsequent adsorption of depressants on chlorite, which utilizing reverse flotation to separate specularite from chlorite and reveal the mechanisms behind it. Single-mineral flotation test results indicated that dextrin and starch have comparable depression effect, while dextrin exhibits better selectivity towards specularite than starch. Chlorite's high floatability can be maintained under the same experimental conditions by adding 9 mg/L SHA and there is an effective separation achieved. Zeta potential data, FT-IR and X-ray photoelectron spectroscopy demonstrated that SHA forms four or five membered ring chelates with Al sites and a few Fe sites on the surface of chlorite through O-O bonding, which forms steric hindrance the adsorption of dextrin, and then forms electrostatic attraction with DDA to improve the floatability of chlorite. In addition, the active Fe sites on specularite surface were sufficiently depressed by dextrin, resulting in the selective separation of chlorite from specularite.

Construction of electron rich Fe active sites by FeCu alloy anchoring on carbon nitride for photocatalytic nitrogen reduction

Construction of electron rich Fe active sites by FeCu alloy anchoring on carbon nitride for photocatalytic nitrogen reduction

Iron containing sludge-derived carbon towards efficient peroxymonosulfate activation: Active site synergy, performance and alternation mechanism

Converting industrial sludge into catalytic materials for water purification is a promising approach to simultaneously realize effective disposal of sludge and resource of water. However, manipulating the high efficiency remains a huge challenge due to the difficulty in the active sites control of the sludge. Herein, we proposed a constitutive modulation strategy by the combination of hydrothermal and pyrolysis (HTP) for the fabrication of defects-assistant Fe containing sludge-derived carbon catalysts on upgrading performance in peroxymonosulfate (PMS) activation for pollutant degradation. Adjustable defects on dyeing sludge-derived carbon catalysts (DSCC) were achieved by introducing oxygen or nitrogen functional precursors (hydroquinone or p-phenylenediamine) during hydrothermal processes and by further pyrolysis, where O was detrimental while N was beneficial to defect generation. Compared to the DSCC with less defects (DHSC-O), the defect-rich sample (DHSC-2N) exhibited superior catalytic performance of PMS activation for bisphenol A (BPA) elimination (k = 0.45 min−1, 2.52 times of DHSC-O), as well as 81.4% total organic carbon (TOC) removal. Meanwhile, the degradation capacity was verified in wide pH range (2.1–8.1) and various aqueous matrices, reflecting the excellent adaptability and anti-interference performance. Furthermore, the continuous-flow experiments on industrial wastewater showed synchronous BPA and chemical oxygen demand (COD) removal, implying great potential for practical application. Solid electron paramagnetic resonance (EPR) and 57Fe Mösssbauer spectra analysis indicated that the defects acted as secondary active sites for Fe sites, which were beneficial to accelerating the electron transfer process. The only Fe active sites preferred the radical pathway. The controllable reaction tendency provides possibilities for the on-demand design of sludge-based catalysts to meet the requirements of practical wastewater treatment under Fenton-like reaction.

Atomically Dispersed Iron Active Sites on Covalent Organic Frameworks for Artificial Photosynthesis of Hydrogen Peroxide

AbstractArtificial photosynthesis has been regarded as a promising solution toward solar energy conversion, generating storable and transportable chemical fuels such as hydrogen (H2) and hydrogen peroxide (H2O2). However, the design of robust catalytic sites not only affects the activity, but also identify the atomic‐level correlation between active sites and natural photosynthesis performance. Herein, a synthesis method of single‐atomic Iron (Fe) active sites anchored on novel covalent organic framework (COF) for the production of H2O2 under visible light irradiation. When benzyl alcohol is the most sacrificial agent, the state‐of‐the‐art Fe‐based COF exhibits an excellent H2O2 generation rate of 4130 µmol g−1 h−1, over 5.3 times higher than that of pristine COF, achieving an apparent quantum yield of 6.4% at 420 nm. The enhanced photocatalytic performance is ascribed to the synergistic effect of atomically dispersed Fe sites and COF hosts, reducing the reaction energy barrier for the formation of *OOH intermediates and optimizing the adsorption of O2 and thus promoting two‐electron oxygen reduction reaction (ORR). This work establishes an atomic‐level engineering approach to build atomically dispersed Fe active sites on COF photocatalysts and provides in‐depth insight upon the ORR mechanism for promising artificial photosynthesis of H2O2.

Density Functional Theory Study of Mechanism of Reduction of N2O by CO over Fe-ZSM-5 Zeolites

Nitrous oxide (N2O) is an industrial waste gas (e.g., from the production of adipic acid), which damages the ozone layer and causes the greenhouse effect. Density functional theory calculations were employed to investigate the mechanism of direct catalytic decomposition of N2O and selective catalytic reduction (SCR) of N2O by CO over Fe-ZSM-5 zeolites. Two stable Fe-active sites with six-membered ring structures on Fe-ZSM-5 were considered. The calculations indicate that the decomposition of N2O is affected by the coordination environment around Fe and can occur through two reaction pathways. However, there is invariably a more considerable energy hurdle for the initiation of the second stage of N2O decomposition. When CO participated in the reaction, it showed good reactivity and stability, the reaction energy barriers of the rate-limiting step were reduced by roughly 20.57 kcal/mol compared to the direct catalytic decomposition of N2O. CO exhibited a superior electron-donating ability and orbital hybridization performance during the reaction, which enhanced the cyclicity of the N2O reduction catalytic process. Our calculations confirmed the significant role of CO in N2O reduction over Fe-ZSM-5 observed in previous studies. This study provides a valuable theoretical reference for exploring CO-SCR methods for N2O reduction over Fe-based zeolite catalysts.