Catalyst For Reaction Research Articles

Catalytic Refining Lignin-derived Monomers: Seesaw Effect between Nanoparticle and Single-Atom Pt.

Pt automatically adsorbed on oxygen vacancy of TiO2 via an in-situ interfacial redox reaction, resulting in atomically dispersion of Pt on TiO2.In the upgrading of lignin-derived 4-propylguaiacol, single-atom catalyst (SAC) Pt/TiO2-H achieved a conversion of 96.9% and a demethoxylation selectivity of 93.3% under 3 MPa H2 at 250 °C for 3 h, markedly different from the performance of nanoparticle counterpart that gave deep deoxygenation selectivity over 99.0%. The high demethoxylation activity of SAC Pt/TiO2-H is mainly attributed to its weak hydrogen spillover capacity that suppressed the benzene ring hydrogenation and the deep deoxygenation. Additionally, SAC Pt/TiO2-H reduced the energy barrier of CAr-OCH3 bond cleavage and accordingly lowered the Gibbs free energy of the demethoxylation reaction. This facile method could fabricate single-atom Au, Pd, Ir, and Ru supported on TiO2-H, demonstrating the generality of this strategy for the establishment of a library of SACs. Moreover, SAC exhibited versatile capacity in demethoxylation of different lignin-derived monomers and high stability.This study showcases the superiority of atomically dispersed metal catalysts for selective demethoxylation reactions and proposes a renewable alternative to fossil-based 4-alkylphenols through upgrading of lignin-derived monomers.

MIL-101(Cr)/aminoclay nanocomposites for conversion of CO2 into cyclic carbonates.

We present the use of an amine functionalized two-dimensional clay i.e., aminoclay (AC), in the chemistry of a three-dimensional metal-organic framework (MOF) i.e., MIL-101(Cr), to prepare MIL-101(Cr)/AC composites, which are exploited as catalysts for efficient conversion of CO2 gas into cyclic carbonates under ambient reaction conditions. Three different MOF nanocomposites, denoted as MIL-101(Cr)/AC-1, MIL-101(Cr)/AC-2, and MIL-101(Cr)/AC-3, were synthesized by an in situ process by adding different amounts of AC to the precursor solutions of the MIL-101(Cr). The composites were characterized by various techniques such as FT-IR, PXRD, FESEM, EDX, TGA, N2 adsorption, as well as CO2 and NH3-TPD measurements. The composites were exploited as heterogeneous catalysts for CO2 cycloaddition reactions with different epoxides and the catalytic activity was investigated at atmospheric pressure under solvent-free conditions. Among all the materials, MIL-101(Cr)/AC-2 shows the best catalytic efficiency under the optimized conditions and exhibits enhanced efficacy compared to various MIL-101(Cr)-based MOF catalysts, which typically need either high temperature and pressure or a longer reaction time or a combination of all the parameters. The present protocol using MIL-101(Cr)/AC-2 as the heterogeneous catalyst gives 99.9% conversion for all the substrates into the products at atmospheric pressure.

Investigation of Doping Effects on the Local Electrochemical Activity of Transition Metal Dichalcogenides 2D Materials

AbstractFinding strategies to enhance catalysts’ electrochemical activity is based on controlling the material design. Bidimensional materials (2DM) such as MoS2 are explored as catalysts for the hydrogen evolution reaction (HER). A comprehensive study of the effects of doping 2D materials with transition metals based on theoretical predictions in tandem with experimental investigation correlates the doping type to the changes in the electronic and electrochemical activity. Localized electrochemical maps obtained by scanning electrochemical cell microscopy (SECCM) reveal that Ti‐doping induces a heterogeneous increase in 2H‐MoS2 basal plane electrochemical activity, while Ni‐doping induces a homogeneous decrease. Additionally, Kelvin probe microscopy provides insight into Ti‐doping, showcasing a decline in the 2H‐MoS2 work function, therefore confirming the predictions from density functional theory simulations. In essence, the findings underscore the potential of transition metal coordination on the 2H‐MoS2 surface as an attractive method for locally doping 2D materials with minimal damage to the crystalline lattice, consequently enhancing the electrochemical activity on the material's basal plane.

Post-treatment induced anisotropic growth of MOF-derived surface modified heterogeneous catalyst for efficient oxygen evolution reaction

The advancement of electrocatalysts exhibiting outstanding performance in the oxygen evolution reaction (OER), crucial for hydrogen production, holds immense significance in addressing energy shortages and mitigating environmental pollution. In this study, a novel approach to synthesizing Co-MOF (Metal-Organic Framework) directly immobilized onto a Ni foam substrate through hydrothermal synthesis is presented. In contrast to conventional methods employing powder-based synthesis with binders, our direct attachment method offers a unique and efficient means of creating robust Co-MOF at Ni foam (Co-MOF@NF) hybrid catalysts. Subsequently, a chemical reduction approach utilizing sodium borohydride was employed to introduce surface modification into the Co-MOF structure. The resulting material, sodium borohydride treated Co-MOF@NF (Red. 1 h Co-MOF@NF), exhibited a remarkable enhancement in OER activity compared to the pristine Co-MOF@NF sample. Notably, Red.1 h Co-MOF@NF demonstrated a substantially reduced overpotential of 235 mV to achieve a current density of 10 mA cm⁻2, in contrast to the 300 mV overpotential required by the pristine Co-MOF@NF under the same conditions. Furthermore, the Red.1 h Co-MOF@NF catalyst displayed exceptional stability, sustaining a current density of 50 mA cm⁻2 for over 48 h, highlighting its promising potential for practical applications. The synergistic effects of direct hydrothermal attachment, surface modification, and improved OER performance make this study a significant contribution to the advancement of efficient and stable electrocatalysts for energy conversion applications.

Construction and catalysis role of a kinetic promoter based on lithium-insertion technology and proton exchange strategy for lithium-sulfur batteries

The high theoretical energy density and specific capacity of lithium-sulfur (Li-S) batteries have garnered considerable attention in the prospective market. However, ongoing research on Li-S batteries appears to have encountered a bottleneck, with unresolved key technical challenges such as the significant shuttle effect and sluggish reaction kinetics. This investigation explores the catalytic efficacy of three catalysts for Li-S batteries and elucidates the correlation between their structure and catalytic impacts. The results suggest that the combined utilization of lithium-insertion technology and a proton exchange approach for δ-MnO2 can optimize its electronic structure, resulting in an optimal catalyst (H/Li inserted δ-MnO2, denoted as HLM) for the sulfur reduction reaction. The replacement of Mn sites in δ-MnO2 with Li atoms can enhance the structural stability of the catalyst, while the introduction of H atoms between transition metal layers contributes to the satisfactory catalytic performance of HLM. Theoretical calculations demonstrate that the bond length of Li2S4 adsorbed by the HLM molecule is elongated, thereby facilitating the dissociation process of Li2S4 and enhancing the reaction kinetics in Li-S batteries. Consequently, the Li-S battery utilizing HLM as a catalyst achieves a high areal specific capacity of 4.2 mAh cm−2 with a sulfur loading of 4.1 mg cm−2 and a low electrolyte/sulfur (E/S) ratio of 8 μL mg−1. This study introduces a methodology for designing effective catalysts that could significantly advance practical developments in Li-S battery technology.

Atomically dispersed Iridium on Mo2C as an efficient and stable alkaline hydrogen oxidation reaction catalyst

Hydroxide exchange membrane fuel cells (HEMFCs) have the advantages of using cost-effective materials, but hindered by the sluggish anodic hydrogen oxidation reaction (HOR) kinetics. Here, we report an atomically dispersed Ir on Mo2C nanoparticles supported on carbon (IrSA-Mo2C/C) as highly active and stable HOR catalysts. The specific exchange current density of IrSA-Mo2C/C is 4.1 mA cm−2ECSA, which is 10 times that of Ir/C. Negligible decay is observed after 30,000-cycle accelerated stability test. Theoretical calculations suggest the high HOR activity is attributed to the unique Mo2C substrate, which makes the Ir sites with optimized H binding and also provides enhanced OH binding sites. By using a low loading (0.05 mgIr cm−2) of IrSA-Mo2C/C as anode, the fabricated HEMFC can deliver a high peak power density of 1.64 W cm−2. This work illustrates that atomically dispersed precious metal on carbides may be a promising strategy for high performance HEMFCs.

Recent Advances in Denitrogenative Organic Transformations of 1,2,3‐Benzotriazin‐4(3H)‐ones

AbstractDenitrogenative organic transformations and related reactions are a class of significant approaches for carrying out unusual C−C/C‐heteroatom (C−O, C−N, C−S) bond‐forming reactions that are usually promoted by Ru, Ir, Pd, Ni, and Cu metal catalysts. In this trait, numerous methods were adopted to synthesize several pharmaceutically valuable N‐ and O‐containing heteroaromatics using 1,2,3‐benzotriazin‐4(3H)‐one as an electrophilic coupling partner. This review involves the recent achievements related to the metal/organo‐catalyzed thermal and visible‐light mediated denitrogenative approaches with 1,2,3‐benzotriazin‐4(3H)‐ones towards the synthesis of imperative N‐heteroaromatic compounds. In addition, metal and oxidant‐free ortho‐functionalization of benzotriazinones by using suitable nucleophilic partners have been discussed. In particular, the most novel methods employing Ni and Pd metal catalysts that have emerged are exhibited. Specific attention has been paid to offering the detailed mechanistic pathway to explain the role of metal catalysts and the mechanism in the absence of metal catalysts in the denitrogenative reactions under a thermal/visible light medium.

Non-precious Electrocatalysts for the Hydrogen Evolution Reaction

The development of non-precious metal-based catalysts for the hydrogen evolution reaction (HER) is a promising research area with the potential to advance water electrolysis and enable the widespread use of hydrogen as a clean energy source. While noble metals like Pt and Pd exhibit excellent HER activity, their limited availability and high cost present significant challenges. Non-precious transition metals such as Fe, Co, and Ni have emerged as alternative catalyst materials due to their natural abundance. However, these metals often encounter obstacles related to their hydrogen adsorption behavior. This commentary highlights the various strategies employed to optimize the electronic structures of non-precious metal-based catalysts to enhance the HER performance. The outlook of non-precious metal-based catalysts is bright, with ongoing and future research activities mainly focusing on improving their properties, integrating these catalysts into commercial water electrolysis systems, and improving the scalability for large-scale hydrogen production. The development of high-performance non-precious metal-based catalysts for HER is crucial to future sustainable and efficient hydrogen production in the transition from fossil fuels to clean energy.

Influence of Oxygen Vacancies in La0.4Sr0.6FeO3-δ Perovskite Oxide Nanoparticles for the Oxygen Evolution Reaction

Oxygen vacancies are important factors to tune the performance of oxide catalysts for the oxygen evolution reaction (OER). However, it remains challenging how to control the concentration of the oxygen vacancies and decouple their effects on OER from other factors. In this work, we use a specific composition/phase La0.4Sr0.6FeO3- d perovskite oxide as an example to tailor the oxygen vacancies of their nanoparticulate using a modified molten salt synthesis and ozone treatment. The OER performance of the resulting La0.4Sr0.6FeO3- d nanoparticles with different degree of oxygen vacancies ranging from 0 to 25% are compared. The OER reactivity increases with increased oxygen vacancies in the materials, but the change is nonlinear. The OER stability, on the other hand, has a bimodal distribution. The activities of fully oxidized sample and the most oxygen-deficient sample degrade slower than the two samples in the middle. The results suggest that it is feasible to design catalysts with oxygen vacancy to be the most OER active and stable. Further investigation into the oxygen vacancy – active site relation would offer guiding principle to design and synthesize high OER performance oxide catalysts.

A new nickel-based δ-isomer Anderson-type polyoxometalates: Synthesis, crystal structure and catalytic activity in 1,2,3-triazoles production

In this study, we present a novel organic hybrid Ni-based δ-isomer of Anderson-type polyoxometalates (POMs), namely, δ-[C6H12Mo6N2NiO24]4− (1), as an efficient catalyst for the cycloaddition reaction between alkynes, halides, and sodium azide. Synthesis of the catalyst was performed using a facile one-pot method followed by characterization using single crystal, powder XRD, SEM, and FT-IR techniques. After optimizing reaction conditions for a model reaction (T = 80 °C, time = 6 h, and solvent = 2 mL H2O), the catalytic activity of this compound was examined for the preparation of diversely substituted 1,2,3-triazoles under ambient atmospheric and additive-free conditions, achieving moderate to good yields. Catalyst 1 could reuse up to four sequential cycles without significant loss in its catalytic activity. Additionally, the true heterogeneity of the catalyst was determined by the hot-filtration test.

High-Entropy La(FeCuMnMgTi)O3 Nanoparticles as Heterogeneous Catalyst for CO2 Electroreduction Reaction.

In this work, La(FeCuMnMgTi)O3 HEO nanoparticles with a perovskite-type structure are synthesized and used in the electrocatalytic CO2 reduction reaction (CO2RR). The catalyst demonstrates high performance as an electrocatalyst for the CO2RR, with a Faradaic efficiency (FE) of 92.5% at a current density of 21.9 mA cm-2 under -0.75 V vs a saturated calomel electrode (SCE). Particularly, an FE above 54% is obtained for methyl isopropyl ketone (C5H10O, MIPK) at a partial current density of 16 mA cm-2, overcoming all previous works. Besides, the as-prepared HEO catalyst displays robust stability in the CO2RR. The excellent catalytic performance of La(FeCuMnMgTi)O3 is ascribed to the synergistic effect between the electronic effects associated with five cations occupying the high-entropy sublattice sites and the oxygen vacancies within the perovskite structure of the HEO. Finally, DFT calculations indicate that Cu plays a vital role in the catalytic activity of the La(FeCuMnMgTi)O3 HEO nanoparticles toward C2+ products.

One-Step Synthesis of High-Efficiency Oxygen Evolution Reaction Catalyst FeSx(Y/MB) with High Temperature Resistance and Strong Alkali

Given the energy crisis and escalating environmental pollution, the imperative for developing clean new energy is evident. Hydrogen has garnered significant attention owing to its clean properties, high energy density, and ease of storage and transportation. This study synthesized four types of catalysts—FeS(DI/MB), FeS(ET/MB), Fe(DI/MB), and Fe(ET/MB)—using two distinct solution systems: DI/MB and ET/MB. The FeS(DI/MB) catalyst, synthesized using the layered solution system (DI/MB), demonstrates a uniformly distributed and dense nanosheet structure, exhibiting excellent resistance to strong bases and superior catalytic properties. The FeS(DI/MB) electrode showed OER overpotentials of 460 mV and 318 mV in 1 M and 6 M, respectively, at current densities of up to 500 mA cm−2. Under industrial electrolysis test conditions, the FeS(DI/MB) electrode required only 262 mV to achieve a current density of 500 mA cm−2, operating in a high-temperature, strong alkaline environment of 6 M at 60 °C. Furthermore, the FeS(DI/MB) electrode exhibited excellent OER catalytic activity and stability, as evidenced by a 60 h stability test These findings provide valuable insights into the preparation of iron nickel sulfide-based catalysts, and further in-depth and comprehensive exploration is anticipated to yield the excellent catalytic performance of these catalysts in the realm of electrolytic water hydrogen production.

A first-principles prediction of the structural, electronic, transport and photocatalytic properties of GaGeX3 (X = S, Se, Te) monolayers.

The discovery of new 2D materials with superior properties motivates scientists to make breakthroughs in various applications. In this study, using calculations based on density functional theory (DFT), we have comprehensively investigated the geometrical characteristics and stability of GaGeX3 monolayers (X = S, Se, or Te), determining their electronic and transport properties, and some essential optical and photocatalytic properties. AIMD simulations show that these materials are highly structurally and thermodynamically stable. Notably, the GaGeSe3 monolayer is a semiconductor with a band gap of 1.9 eV and has a high photon absorption coefficient of up to 1.1 × 105 cm-1 in the visible region. The calculated solar-to-hydrogen conversion efficiency of the GaGeSe3 monolayer is 11.33%, which is relatively high compared to some published 2D materials. Furthermore, the electronic conductivity of the GaGeSe3 monolayer is 790.65 cm2 V-1 s-1. Our findings suggest that the GaGeSe3 monolayer is a new promising catalyst for the solar water-splitting reaction to give hydrogen and a potential new 2D material for electrical devices with high electron mobility.

Tuning Two-Dimensional Phthalocyanine Dual Site Metal-Organic Framework Catalysts for the Oxygen Reduction Reaction.

Metal-organic frameworks (MOFs) offer an interesting opportunity for catalysis, particularly for metal-nitrogen-carbon (M-N-C) motifs by providing an organized porous structural pattern and well-defined active sites for the oxygen reduction reaction (ORR), a key need for hydrogen fuel cells and related sustainable energy technologies. In this work, we leverage electrochemical testing with computational models to study the electronic and structural properties in the MOF systems and their relationship to ORR activity and stability based on dual transitional metal centers. The MOFs consist of two M1 metals with amine nodes coordinated to a single M2 metal with a phthalocyanine linker, where M1/M2 = Co, Ni, or Cu. Co-based metal centers, in particular Ni-Co, demonstrate the highest overall activity of all nine tested MOFs. Computationally, we identify the dominance of Co sites, relative higher importance of the M2 site, and the role of layer M1 interactions on the ORR activity. Selectivity measurements indicate that M1 sites of MOFs, particularly Co, exhibit the lowest (<4%), and Ni demonstrates the highest (>46%) two-electron selectivity, in good agreement with computational studies. Direct in situ stability characterization, measuring dissolved metal ions, and calculations, using an alkaline stability metric, confirm that Co is the most stable metal in the MOF, while Cu exhibits notable instability at the M1. Overall, this study reveals how atomistic coupling of electronic and structural properties affects the ORR performance of dual site MOF catalysts and opens new avenues for the tunable design and future development of these systems for practical electrochemical applications.

A Vacuum Vapor Deposition Strategy to Fe Single-Atom Catalysts with Densely Active Sites for High-Performance Zn-Air Battery.

Iron single-atom catalysts (SACs) have garnered increasing attention as highly efficient catalysts for the oxygen reduction reaction (ORR), yet their performance in practical devices remains suboptimal due to the low density of accessible active sites. Anchoring iron single atoms on 2D support is a promising way to increase the accessible active sites but remains difficult attributing to the high aggregation tendency of iron atoms on the 2D support. Herein, a vacuum vapor deposition strategy is presented to fabricate an iron SAC supported on ultrathin N-doped carbon nanosheets with densely active sites (FeSAs-UNCNS). Experimental analyses confirm that the FeSAs-UNCNS achieves densely accessible active sites (1.11×1020sitesg-1) in the configuration of Fe─N4O. Consequently, the half-wave potential of FeSAs-UNCNS in 0.1m KOH reaches a remarkable value of 0.951V versus RHE. Moreover, when employed as the cathode of various kinds of Zn-air batteries, FeSAs-UNCNS exhibits boosting performances by achieving a maximum power density of 306mWcm-2 and long cycle life (>180h) at room temperature, surpassing both Pt/C and reported SACs. Further investigations reveal that FeSAs-UNCNS facilitates the mass and charge transfer during catalysis and the atomic configuration favors the desorption of *OH kinetically.

Accelerating the Screening of Modified MA2Z4 Catalysts for Hydrogen Evolution Reaction by Deep Learning‐Based Local Geometric Analysis

Machine learning (ML) integrated with density functional theory (DFT) calculations have recently been used to accelerate the design and discovery of single‐atom catalysts (SACs) by establishing deep structure–activity relationships. The traditional ML models are always difficult to identify the structural differences among the single‐atom systems with different modification methods, leading to the limitation of the potential application range. Aiming to the structural properties of several typical two‐dimensional MA2Z4‐based single‐atom systems (bare MA2Z4 and metal single‐atom doped/supported MA2Z4), an improved crystal graph convolutional neural network (CGCNN) classification model was employed, instead of the traditional machine learning regression model, to address the challenge of incompatibility in the studied systems. The CGCNN model was optimized using crystal graph representation in which the geometric configuration was divided into active layer, surface layer, and bulk layer (ASB‐GCNN). Through ML and DFT calculations, five potential single‐atom hydrogen evolution reaction (HER) catalysts were screened from chemical space of 600 MA2Z4‐based materials, especially V1/HfSn2N4(S) with high stability and activity (ΔGH* is 0.06 eV). Further projected density of states (pDOS) analysis in combination with the wave function analysis of the SAC‐H bond revealed that the SAC‐dz2 orbital coincided with the H‐s orbital around the energy level of −2.50 eV, and orbital analysis confirmed the formation of σ bonds. This study provides an efficient multistep screening design framework of metal single‐atom catalyst for HER systems with similar two‐dimensional supports but different geometric configurations.

Competitive coordination-induced assembling of Ni-mof/NiFe-ldh heterostructure for enhanced electrocatalytic methanol oxidation

Direct methanol fuel cells (DMFCs) can permit the utilization of noble-metal-free electrocatalysts, which certainly reduces the cost and accelerates their practical implementation. With the exploration of efficient and economical methanol oxidation reaction (MOR) catalysts, Ni-based nanostructures have been recognized as the most promising MOR catalysts in alkaline media. Herein, we construct a novel heterojunction MOR electrocatalyst composed of Ni-based metal-organic framework (Ni-MOF) and NiFe-based layered double hydroxides (LDHs) through a coordination-induced self-assembly strategy. Owing to the synergic effect between Ni and Fe sites, coupled with the effect of hetero-interface, the resultant Ni-MOF/NiFe-LDH composite exhibits remarkable MOR activity in 0.1 M KOH electrolyte with the oxidation current density (32.66 mA cm−2) is 2.65 and 2.44 times higher than that of the primitive NiFe-LDH and Ni-MOF. The excellent stability of the Ni-MOF/NiFe-LDH electrocatalyst has also been confirmed by long-term chronoamperometry (CA) analysis. Our work paves a facile controllable way for fabricating MOF/LDH heterostructure targets on MOR and underlines its potential to boost energy conversion efficiency through the manipulation of synergic components.

N‐Doped Carbon Nanofibers and Carbon Nanotubes‐Encapsulated CoNi Alloy as Highly Active Oxygen Reduction Catalysts for Direct Methanol Fuel Cells

The slow oxygen reduction kinetics of direct methanol fuel cell (DMFCs) are one of the limiting factors affecting its application. Therefore, exploring nonprecious catalysts with high activity and methanol resistance is urgently needed. Herein, zeolitic imidazolate framework‐8 particles are first blended with different proportions of metal salts (Ni as well as Co) and further electrospun to obtain a nanofiber precursor. After pyrolysis treatment, a composite catalyst (CoNi@N‐CNFs) with a highly dispersed CoNi alloy phase supported by porous N‐doped carbon nanofiber and carbon nanotube is prepared. The surface electronic structure can be reasonably adjusted by optimizing the doping ratio of Ni and Co. The CoNi@N‐CNFs shows high oxygen reduction activity and methanol resistance. Half‐wave potential and the onset potential of Co1Ni1@N‐CNFs (Co: Ni mole ratio = 1:1) are 0.79 and 0.87 V. Additionally, Co1Ni1@N‐CNF‐modified DMFC endows a high power density (24.07 mW cm−2), which is close to Pt/C‐based DMFC (27.59 mW cm−2). Rich active sites, large specific surface area, and synergy between CoNi alloy and N configuration of CoNi@N‐CNFs effectively accelerate electron transfer, resulting in the superior catalytic activity. This work provides a new strategy to design effective 1D oxygen reduction reaction catalysts in fuel cells.

Recent Advancements in Ascribing Several Platinum Free Electrocatalysts Pertinent to Hydrogen Evolution from Water Reduction.

The advancement of a sustainable and scalable catalyst for hydrogen production is crucial for the future of the hydrogen economy. Electrochemical water splitting stands out as a promising pathway for sustainable hydrogen production. However, the development of Pt-free electrocatalysts that match the energy efficiency of Pt while remaining economical poses a significant challenge. This review addresses this challenge by highlighting latest breakthroughs in Pt-free catalysts for the hydrogen evolution reaction (HER). Specifically, we delve into the catalytic performance of various transition metal phosphides, metal carbides, metal sulphides, and metal nitrides toward HER. Our discussion emphasizes strategies for enhancing catalytic performance and explores the relationship between structural composition and the performance of different electrocatalysts. Through this comprehensive review, we aim to provide insights into the ongoing efforts to overcome barriers to scalable hydrogen production and pave the way for a sustainable hydrogen economy.

Instantaneous Thermal Energy for Swift Synthesis of Single-Atom Catalysts for Unparalleled Performance in Metal-Air Batteries and Fuel Cells.

Based on experimental and computational evidence, phthalocyanine (Pc) compounds in the form of quaternary bound metal-nitrogen (N) atoms are the most effective catalysts for oxygen reduction reaction (ORR). However, the heat treatment process used in their synthesis may compromise the ideal structure, causing the agglomeration of transition metals. To overcome this issue, we developed a novel method for synthesizing iron (Fe) single-atom catalysts with ideal structures supported by thermally exfoliated graphene oxide (GO). This was achieved through a short heat-treatment of only 2.5min involving FePc and N,N-dimethylformamide in the presence of GO. According to the synthesis mechanism revealed by this study, carbon monoxide acts as a strong linker between the single Fe atoms and graphene. It facilitates the formation of a structure containing oxygen species between FeN4 and graphene, which provides high activity and stability for the ORR. These catalysts possess an enormous number of active sites and exhibit enhanced activity towards the alkaline ORR. They have demonstrated excellent performance when applied to real electrochemical devices, such as zinc-air batteries and anion exchange membrane fuel cells. We expect that the instantaneous heat treatment method developed in our study will aid in the development of high-performing single-atom catalysts. This article is protected by copyright. All rights reserved.