Oxygen Reduction Reaction Activity Research Articles

Activating colloidal synthesized Au catalyst by the electrochemical strategy: Gas atmosphere, electrolyte and electrochemical technique

Organic ligands are necessarily used to stabilize nanoparticles (NPs) in colloid synthesis, and the presence of these ligands in most cases can have adverse effects on heterogeneous nanocatalysis. Therefore, it is crucial to develop efficient methods to remove ligands and study the removal mechanism. In this article, we developed a combined electrochemical method (chronoamperometry (CA) + cyclic voltammetry (CV)), which can completely and efficiently remove thiol ligand from Au NPs to produce cleaned Au/C catalyst. Using the oxygen reduction reaction (ORR) activity as the evaluation criterion for ligand removal, we found that gas atmosphere (O2) plays an important role in the removal process, while the acidity and alkalinity of electrolyte have no effect on the removal efficiency. A proposed thiol ligand removal mechanism along with Au degradation is presented. The results of CA activation at an oxidation constant potential (1.7 V) indicate that oxidation of thiol alone cannot remove thiol ligand. Only if a reduction constant potential of 0.2 V is further applied, the ORR activity of Au/C catalyst will increase, indicating that both the oxidation and reduction processes of Au NPs are crucial for ligand removal. Although the CA method (with an upper potential of 1.7 V and a lower potential of 0.2 V) can efficiently remove the majority of thiol ligand, complete removal of thiol ligand requires further CV activation. Based on the relevant results, a combined electrochemical method (CA + CV) is established. Developing standardized methods for removing ligands on the surface of catalysts is important for obtaining efficient catalysts and is also important for the reproducibility of catalytic results.

Accordion-like multilayered titanium nitride enables FeN4-O axial coordination of iron phthalocyanine as efficient catalysts for oxygen reduction reaction

The susceptibility of MXenes to oxidation leads to rapid chemical degradation and functional loss, and hence limits their diverse applications. In this study, we develop a scalable strategy to transform blocky, condensed titanium nitride (TiN) into accordion-like leafy titanium nitride (M-TiN), which exhibits enhanced chemical stability and an increased surface area. When functionalized with iron phthalocyanine (FePc), the resulting M-TiN/FePc composite displays a remarkable electrocatalytic activity towards the oxygen reduction reaction (ORR) due to the formation of FeN4-O axial coordination and a low-to-intermediate Fe spin state, as confirmed by spectroscopy and magnetic measurements. This leads to electron filling in the antibonding orbitals composed of Fe 3dz2 and O2 π* orbitals, significantly improving O2 activation and ORR activity. Significantly, with the M-TiN/FePc composite as the air cathode catalyst, a zinc-air battery achieves a superior power density of 270.31 mW cm−2 and enhanced cyclability compared to that with commercial Pt/C. Results from this study highlight the significance of morphological engineering of TiN in regulating the atomic configuration of adsorbed metal active centers and hence their catalytic activity, in particular, in harsh oxidative conditions.

Large-Scale Atomic Strain Defects on Palladium Surfaces for Enhanced Oxygen Reduction and Zinc-Air Batteries.

Designing nano-electrocatalysts rich in surface defects is critical to improve their catalytic performance. However, prevailing synthesis techniques rely heavily on complex procedures that compromise defect extensiveness and uniformity, casting a high demand for methods capable of synthesizing large-scale crystalline defects. An innovative design strategy is herein proposed that induces ample strain/dislocation defects during the growth of palladium (Pd), which is well-known as a good oxygen reduction reaction (ORR) catalyst. The controlled defect engineering on Pd core is achieved by the tensile stress exerted from an intentionally applied Fe3O4 skin layer during synthesis, which changes the surface free energy of Pd to stabilize the defect presence. With such large-scale crystalline defects, this Pd catalyst exhibits significantly higher ORR activity than commercial Pt/C, enabling its promising future in zinc-air battery catalysis. Additionally, the protective Fe3O4 skin covering the catalyst also enhances its catalytic stability. Theoretical calculations show that the superior catalytic property of such defect-engineered Pd is associated with the correspondingly modified adsorption energy of *O intermediates onto its surface, which further improves the reaction rate and thus boosts ORR kinetics. Findings here are expected to provide a paradigm for designing efficient and stable metal catalysts with plentiful large-scale strain defects.

Construction of atom-scale Co/Fe/Ni M-N-C active sites within nitrogen-doped carbon spheres for high-performance bifunctional oxygen catalysts in rechargeable zinc-air batteries

Developing carbon-based catalysts with metal‑nitrogen‑carbon (M-N-C) active sites as efficient and low-cost bifunctional catalysts to replace precious metal catalysts for rechargeable zinc-air batteries devices has garnered significant attention. Herein, nitrogen-doped submicron carbon-based spherical bifunctional electrocatalysts (CNPD-CoFeNi) with abundant atom-scale Co/Fe/Ni M-N-C active sites and defects were synthesized. The introduction of massive amounts of Zn species increases the spatial distance of Co/Fe/Ni metal sites to prevent aggregation during pyrolysis, and the evaporation of Zn at high temperatures creates defects synergizing with M-N-C. Consequently, CNPD-CoFeNi possesses a stable carbon-based spherical structure, high electrical conductivity, rich nitrogen content, abundant atom-scale Co/Fe/Ni M-N-C active sites, and defects, displaying outstanding durability, oxygen reduction reaction (ORR) activity with a half-wave potential of 0.87 V, and satisfactory OER performance, surpassing or comparable with the state-of-art Pt/C and RuO2, respectively. Notably, liquid Zn-air batteries with CNPD-CoFeNi catalyst exhibit an exceptional high peak power density of 146.5 mW cm−2 and stable charge-discharge cycling over 270 h, outperforming Pt/C-RuO2 based devices. Additionally, the all-solid-state Zn-air battery also displays satisfactory practicability and stability. The synthesis strategy and its remarkable results provide valuable guidance and inspiration for the future advancement of precious metal substitutes in ORR/OER and rechargeable zinc-air batteries.

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.

MOF-Derived Ni/NiO-C Nanocomposites as Bifunctional Electrocatalysts Capable of Driving Both ORR and OER.

Bifunctional electrocatalysts, capable of efficiently driving both the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER), are crucial for advancing electrochemical processes. While noble-metal-based catalysts are widely recognized for their role in oxygen processes, current state-of-the-art designs are limited to either ORR or OER activity, presenting a notable research gap. In addressing this challenge, we have developed a novel Ni/NiO-C nanocomposite catalyst derived from a nickel-based metal-organic framework (Ni-SKU-5). For the ORR, the Ni/NiO-C catalyst exhibits an onset potential of 0.95 V vs RHE in a 1.0 M KOH solution, coupled with a Tafel slope of -99 mV dec-1 at 1600 rpm. Moreover, the catalyst displays excellent stability, maintaining a performance of over 90% after 10 h of continuous reaction. Furthermore, the catalyst proves effective in the OER, boasting an overpotential of 370 mV (at 10 mA cm-2) and a Tafel slope of 114 mV dec-1, highlighting its bifunctionality. The bifunctional overpotential of the Ni/NiO-C composite is measured at 820 mV, surpassing that of the 20% Pt/C electrocatalyst (860 mV), highlighting its potential for practical applications. Comparative experiments establish the origin of the robust bifunctional reactivity toward the conformal hybrid structure, porous framework, and the synergistic effect operating among the constituents of the nanocomposite.

Synergistic effect of Fe-Ru alloy and Fe-N-C sites on oxygen reduction reaction

In the pursuit of optimizing Fe-N-C catalysts for the oxygen reduction reaction (ORR), the incorporation of alloy nanoparticles has emerged as a prominent strategy. In this work, we effectively synthesized the FeRu-NC catalyst by anchoring Fe-Ru alloy nanoparticles and FeN4 single atom sites onto carbon nanotubes. The FeRu-NC catalyst exhibits significantly enhanced ORR activity and long-term stability, with a high half-wave potential of 0.89 V (vs. RHE) in alkaline conditions, and the half-wave potential remains nearly unchanged after 5000 cycles. The zinc-air battery (ZAB) assembled with FeRu-NC demonstrates a power density of 169.1 mW cm−2, surpassing that of commercial Pt/C. Density functional theory (DFT) calculations reveal that the synergistic interaction between the Fe–Ru alloy and FeN4 single atoms alters the electronic structure and facilitates charge transfer at the FeN4 sites, thereby modulating the adsorption and desorption of ORR intermediates. This enhancement in catalytic activity for the ORR process underscores the potential of this approach for refining M-N-C catalysts, providing novel insights into their optimization strategies.

Aminotriazine derived N-doped mesoporous carbon with a tunable nitrogen content and their improved oxygen reduction reaction performance.

The electrocatalytic activity of carbon materials is highly dependent on the controlled modulation of their composition and porosity. Herein, mesoporous N-doped carbon with different amounts of nitrogen was synthesized through a unique strategy of using a high nitrogen containing CN precursor, 3-amino 1,2,4 triazine (3-ATZ) which is generally used for the preparation of carbon nitrides, integrated with the combination of a templating method and high temperature treatment. The nitrogen content and the graphitisation of the prepared materials were finely tuned with the simple adjustment of the carbonisation temperature (800-1100 °C). The optimised sample as an electrocatalyst for oxygen reduction reaction (ORR) exhibited an onset potential of 0.87 V vs. RHE with a current density of 5.1 mA cm-2 and a high kinetic current density (Jk) of 33.1 mA cm-2 at 0.55 V vs. RHE. The characterisation results of the prepared materials indicated that pyridinic and graphitic nitrogen in the carbon framework promoted ORR activity with improved four-electron selectivity and excellent methanol tolerance and stability. DFT calculations demonstrated that the structural and planar defects in the N-doped carbon regulated the surface electronic properties of the electrocatalyst, leading to a reduction in the energy barrier for the ORR activity. This strategy has the potential to unlock a platform for designing a series of catalysts for electrochemical applications.

Strong Electronic Metal-Support Interactions Enable the Increased Spin State of Co-N4 Active Sites and Performance for Acidic Oxygen Reduction Reaction.

Nonprecious metal catalysts, particularly M-N-C catalysts, are widely recognized as promising contenders for the oxygen reduction reaction (ORR). However, a notable performance gap persists between M-N-C catalysts and Pt-based catalysts under acidic conditions. In this study, hybrid catalysts comprising single Co atoms and ultralow concentrations of Pt3Co intermetallic nanoparticles (NPs) are introduced to enhance ORR performance. Under acidic conditions, these hybrid catalysts demonstrate ORR efficiency with a half-wave potential of 0.895 V, negligible decay even after 80 000 cycles, and a high maximum power density of 1.34 W cm-2 in fuel cells. This performance surpasses those of Co-N-C and Pt/Co-N-C catalysts. Both experimental findings and theoretical computations suggest that the heightened ORR activity stems from an increase in the spin density of Co sites induced by noble metal NPs, facilitating the activation of O-O bonds via side-on overlapping and enabling a transition in the reaction pathway from associative to dissociative processes. This research offers a promising avenue for the systematic design of M-N-C cathodes with an enhanced performance for acidic fuel cells.

Boosting oxygen reduction performance by copper-iron co-doped on ZIF-derived N-doped carbon nanotubes

Developing high-efficiency non-noble metal catalysts for the oxygen reduction reaction (ORR) is paramount for sustainable energy conversion. In this study, we proposed a Cu, Fe co-doped zeolite imidazole framework (ZIF)-derived nitrogen-doped carbon nanotubes catalyst (Cu–Fe@CNTs/NC) obtained by hydrothermal method and pyrolysis. The electrochemical results showed that Cu–Fe@CNTs/NC exhibited favorable oxygen reduction performance and good stability under alkaline electrolyte. The incorporation of Cu and Fe bimetallic dopants promoted the carbon nanotubes growth on ZIF nanosheets, and the collaborative action of Cu and Fe enhanced its ORR catalytic activity. These findings provide an innovative way to prepare high active non-platinum ORR catalysts.

Formation Characteristics of Pt-Ni Alloy Nanoparticles Fabricated by Nanolamination of Atomic Layer Deposition in Hydrogen.

Forced-flow atomic layer deposition nanolamination is employed to fabricate Pt-Ni nanoparticles on XC-72, with the compositions ranging from Pt94Ni6 to Pt67Ni33. Hydrogen is used as a co-reactant for depositing Pt and Ni. The growth rate of Pt is slower than that using oxygen reactant, and the growth exhibits preferred orientation along the (111) plane. Ni shows much slower growth rate than Pt, and it is only selectively deposited on Pt, not on the substrate. Higher ratios of Ni would hinder subsequent stacking of Pt atoms, resulting in lower overall growth rate and smaller particles (1.3-2.1nm). Alloying of Pt with Ni causes shifted lattice that leads to larger lattice parameter and d-spacing as Ni fraction increases. From the electronic state analysis, Pt 4f peaks are shifted to lower binding energies with increasing the Ni content, suggesting charge transfer from Ni to Pt. Schematic of the growth behavior is proposed. Most of the alloy nanoparticles exhibit higher electrochemical surface area and oxygen reduction reaction activity than those of commercial Pt. Especially, Pt83Ni17 and Pt87Ni13 show excellent mass activities of 0.76 and 0.59AmgPt -1, respectively, higher than the DOE target of 2025, 0.44AmgPt -1.

New Morphology Modifier Enables the Preparation of Ultra-Long Platinum Nanowires Excluding Mo Component for Efficient Oxygen Reduction Reaction Performance.

The structural tailoring of Pt-based catalysts into 1D nanowires for oxygen reduction reactions (ORR) has been a focus of research. Mo(CO)6 is commonly used as a morphological modifier to form nanowires, but it is found that it inevitably leads to Mo doping. This doping introduces unique electrochemical signals not seen in other Pt-based catalysts, which can directly reflect the stability of the catalyst. Through experiments, it is demonstrated that Mo doping is detrimental to ORR performance, and theoretical calculations have shown that Mo sites that are inherently inactive also poison the ORR activity of the surrounding Pt. Therefore, a novel gas-assisted technique is proposed to replace Mo(CO)6 with CO, which forms ultrafine nanowires with an order of magnitude increase in length, ruling out the effect of Mo. The catalyst performs at 1.24 A mgPt -1, 7.45 times greater than Pt/C, demonstrating significant ORR mass activity, and a substantial improvement in stability. The proton exchange membrane fuel cell using this catalyst provides a higher power density (0.7W cm-2). This study presents a new method for the preparation of ultra-long nanowires, which opens up new avenues for future practical applications of low-Pt catalysts in PEMFC.

BaFe12O19 Functional Porous Carbon Nanocomposite as an Electrocatalyst of the Oxygen Reduction Reaction

AbstractIt is crucial to develop a non‐precious metal catalyst with high efficiency, affordable cost, and minimal environmental impact for conducting research on the oxygen reduction reaction (ORR) in fuel cells. In this study, BaFe12O19 functional porous carbon (BaFe12O19/PC) nanocomposite was successfully prepared using Fe2O3, BaCO3 and glucose as precursors. Meanwhile, the BaFe12O19/PC catalyst‐modified glassy carbon electrode, carbon rod, and Hg/HgO electrode were used as the working electrode, counter electrode, and reference electrode, respectively, to investigate the electrochemical behavior. The uniform distribution of nano‐scale BaFe12O19 particles in a porous carbon framework was confirmed by field emission scanning electron microscopy characterization. In addition, a double‐layer interface (Fe/Fe3C) was formed between the porous carbon and the nano‐sized BaFe12O19 particles. Fe/Fe3C has a synergistic effect with C, facilitating the migration and transfer of electrons from BaFe12O19 to porous carbon. The BaFe12O19/PC nanocomposite exhibited a four‐electron pathway for electrocatalytic kinetics, showcasing a significantly elevated half‐wave potential of 0.77 V, an impressively reduced Tafel slope of 84.95 mV/dec, and exceptional tolerance towards methanol. It is important to highlight that the BaFe12O19/PC nanocomposite not only possess high catalytic activity for oxygen reduction reactions (ORR), but also demonstrate excellent stability. Consequently, this synthesized BaFe12O19/PC nanocomposite hold promising prospects as cost‐effective and efficient catalysts in fuel cell applications.

Modulating Spin of Atomic Manganese Center for High-Performance Oxygen Reduction Reaction.

Single atom catalysts (SACs) are promising non-precious catalysts for oxygen reduction reaction (ORR). Unfortunately, the ORR SACs usually suffer from unsatisfactory activity and in particular poor stability. Herein, we report atomically dispersed manganese (Mn) embedded on nitrogen and sulfur co-doped graphene as an efficient and robust electrocatalyst for ORR in alkaline electrolyte, realizing a half-wave potential (E1/2) of 0.883 V vs. reversible hydrogen electrode (RHE) with negligible activity degradation after 40,000 cyclic voltammetry (CV) cycles in 0.1 M KOH. Introducing sulfur (S) to form Mn-S coordination changes the spin state of single Mn atom from high-spin to low-spin, which effectively optimizes the oxygen intermediates adsorption over the single Mn atomic sites and thus greatly improves the ORR activity.

Inclusion Strategy for Constructing S/N Orbital Hybridization-Regulated sp3/sp2 Carbon toward Boost Electrocatalysis.

Metal-free carbon-based electrocatalysts have gained significant attention in the field of zinc-air batteries (ZABs) due to their affordability, good conductivity and chemical stability. However, unmodified carbon materials typically fall short in adsorbing and activating the substrates and intermediates involved in oxygen reduction reactions (ORR). Here, a metal-free carbon-based electrocatalyst with S atom p orbital hybrid modified N-sp3/sp2 carbon structure (C/NS) were prepared by cyclodextrins inclusion. The catalyst demonstrates impressive ORR activity (E1/2=0.885 V vs. RHE) and robust ZABs performance with a power density of 171.3 mW cm-2 and a specific capacity of 781.2 mAh g-1. Density functional theory (DFT) calculation reveals that S atom effectively regulates the charge distribution and p-band center of active site carbon atom in the N-sp3/sp2 carbon structure. This modification prompts the adsorption and dissociation of O2 and intermediates, resulting in higher reactive activity. This work provides a valuable and practical strategy for preparing cost-effective metal-free carbon-based electrocatalysts for ORR with high performance.

Modulating Spin of Atomic Manganese Center for High‐Performance Oxygen Reduction Reaction

Single atom catalysts (SACs) are promising non‐precious catalysts for oxygen reduction reaction (ORR). Unfortunately, the ORR SACs usually suffer from unsatisfactory activity and in particular poor stability. Herein, we report atomically dispersed manganese (Mn) embedded on nitrogen and sulfur co‐doped graphene as an efficient and robust electrocatalyst for ORR in alkaline electrolyte, realizing a half‐wave potential (E1/2) of 0.883 V vs. reversible hydrogen electrode (RHE) with negligible activity degradation after 40,000 cyclic voltammetry (CV) cycles in 0.1 M KOH. Introducing sulfur (S) to form Mn‐S coordination changes the spin state of single Mn atom from high‐spin to low‐spin, which effectively optimizes the oxygen intermediates adsorption over the single Mn atomic sites and thus greatly improves the ORR activity.

Steam Gasification of PEMFC Catalysts: An Endothermal Process to Create Accessible Carbon Support Morphologies

Platinum catalysts supported on porous carbons are considered state-of-the-art for proton-exchange membrane fuel cells (PEMFCs) due to their ability to protect Pt nanoparticles within the internal pores of the primary carbon particles. This shielding enables high oxygen reduction reaction (ORR) activity by separating the Pt particles from ionomer contact and endows them with greater resilience against voltage cycling-induced degradation. However, the pore enclosure impedes oxygen diffusion to internal platinum particles at high current densities, incurring significant voltage losses particularly at low cathode loadings (∼0.07 mgPt cm−2). Such transport bottlenecks can be mitigated by localized oxidation, a thermal post-treatment enabling Pt particles to etch open the surrounding pore space via Pt-catalyzed carbon oxidation. The strong exothermicity of this reaction, however, is challenging for process scale-up. We explore Pt-catalyzed steam gasification of Pt/Ketjenblack as an endothermal, but otherwise functionally similar post-treatment to increase catalyst accessibility. Connecting physico- and electrochemical characterizations of steam-gasified catalysts, we identify the generation of mesopore volume to be crucial for high current density performance and efficient oxygen transport. Ultimately, locally oxidized and steam-gasified catalysts reveal subtle differences in their respective etching mechanisms, resulting in marginally less efficient pore opening, but also better ORR activity retention for steam gasification.

CO2- tolerant CuFe2O4 as Bifunctional Electrocatalyst for Transition from Rechargeable Li-O2 to Li-CO2 Batteries

CO2-tolerant rechargeable Lithium-Air batteries are seen as a high-performing alternative to Li-ion batteries. They utilize O2 from the air, reducing it at the cathode to form lithium peroxide (Li2O2) during discharge which is then oxidized to form lithium-metal and freeing O2 during charging. Most of the present studies involve pure O2 as the cathode material instead of aerial O2, which has a stiff-challenge due to atmospheric CO2 which produces Li2CO3 during discharge, posing a resistive load on the battery if not re-oxidized on charging. Ideally, presence of CO2 should enhance the charge-storage capacity if it is cycled reversibly. Thus, present research aims at taking advantage of both O2 and CO2 by employing metallic Cu on CuFe2O4 catalyst, synthesized from a one-step auto-combustion route. The Cu metal present in the catalyst leads to a low surface-area, yet the catalyst demonstrates excellent oxygen reduction reaction and moderate oxygen evolution reaction activity. excellent CO2 reduction reaction activity, oxidizing both the Li2O2 and the Li2CO3 during charge in both 10% CO2 and 100% CO2 atmospheres. The fabricated Li-CO2 battery operates for practical application, suggesting the suitability of the catalyst for the transition from practical Li-O2 battery to Li-Air battery.

Enhanced oxygen reduction reaction with rare-earth metal-based Ce-N-C catalyst

An atomically dispersed single atom catalyst based on rare-earth metal, Cerium embedded into the porous N-doped carbon (Ce-N-C), has been synthesized by using metal-organic framework method. The Ce-N-C catalyst have been physiochemically and electrochemically characterized in detail. Transmission electron microscope studies revealed atomically dispersed Ce atoms on the N-doped carbon support. The electrochemical oxygen reduction reaction (ORR) kinetics of Ce-N-C-3 catalyst revealed an admirable activity with a half-wave potential of 0.89 V, nearly equal to state-of-the-art Pt/C catalyst. The K-L plots and RRDE measurements revealed a nearly direct 4 electron reduction of O2 to H2O by Ce-N-C-3 catalyst. In addition, the chronoamperometry studies with a simulated H2O2 environments clearly revealed the significance of Ce3+/Ce4+ redox couple in deactivating hydrogen peroxide and/or hydroperoxide radicals. The commendable ORR activity, stability and peroxide resistance of Ce-N-C-3 catalysts is credited to the high surface area, atomically dispersed Ce atoms, formation of Ce-N4-C active sites in the catalysts, evidenced from the XPS analysis, in addition to the significance of Ce3+/Ce4+ redox couple in the catalyst. Most importantly, chronoamperometric studies revealed clear evidence of Ce3+/Ce4+ couple significance, helping in effectively mitigating the peroxide related detrimental effects to the ORR catalyst.

Laser driven generation of single atom Fe-N-C catalysts for the oxygen reduction reaction

Single-Atom Catalysts (SACs) have emerged as the ultimate solutions in challenging systems bridging the gap between homogeneous and heterogeneous catalysts. However, feasible synthesis methods are necessary to stabilize single metal atoms, increase catalyst loadings and scale up the synthesis. Due to its sluggish kinetics, the oxygen reduction reaction (ORR) is the main source of irreversibility in proton exchange membrane fuel cells (PEMFC). The most promising candidates to replace Pt-based catalysts for the ORR in fuel cells are the so-called Fe-N/C catalysts. These catalysts display high ORR activity in acidic and alkaline electrolytes. In this work, we propose a laser-driven pyrolysis approach to generate Fe-N/C SACs that involves decomposition of aerosolized iron-phthalocyanines. The resulting catalyst displays ORR activity in acidic and alkaline electrolytes, with competitive half-potential and kinetic current density values in comparison with state-of-the-art electrocatalysts.