CO Tolerance Research Articles

Elucidating the effects of nitrogen and phosphorus co-doped carbon on complex spinel NiFe2O4 towards oxygen reduction reaction in alkaline media

The study presents for the first time complex spinel NiFe2O4 nanoparticles supported on nitrogen and phosphorus co-doped carbon nanosheets (NPCNS) prepared using sol gel and the carbonization of graphitic carbon nitride with lecithin as a highly active and durable electrocatalyst for oxygen reduction reaction. The physicochemical properties of complex spinel NiFe2O4 on NPCNS and subsequent nanomaterials were investigated using techniques such as X-ray diffraction, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and transmission electron microscopy. The electrochemical activity of the electrocatalysts was evaluated using hydrodynamic linear sweep voltammetry, cyclic voltammetry, electrochemical impedance spectroscopy, and chronoamperometry. The electrocatalytic performance of the NiFe2O4/NPCNS nanohybrid electrocatalyst is dominated by the 4e− transfer mechanism, with an onset potential of 0.92 V vs. RHE, which is closer to that of the Pt/C, and a current density of 7.81 mA/cm2 that far exceeds that of the Pt/C. The nanohybrid demonstrated the best stability after 14 400 s, outstanding durability after 521 cycles, and the best ability to oxidize methanol and remove CO from its active sites during CO tolerance studies. This improved catalytic activity can be attributed to small nanoparticle sizes of the unique complex spinel nickel ferrite structure, N-Fe/Ni coordination of nanocomposite, high dispersion, substantial ECSA of 47.03 mF/cm2, and synergy caused by strong metal-support and electronic coupling interactions.

PtPdAg nanotrees with low Pt content for high CO tolerance within formic acid and methanol electrooxidation

PtPdAg nanotrees with low Pt content for high CO tolerance within formic acid and methanol electrooxidation

Impact of Fe2(MoO4)3 and ZnMoO4 on CO Tolerance of Pt/C catalysts for enhanced methanol electrooxidation efficiency

Success of Pt/C catalyst in electrooxidation of methanol is highly influenced by its ability to withstand the poisoning effects of carbonaceous species adsorbed on the catalytic surface. Covalently bonded CO molecules occlude the active sites of the catalytic surface, impeding methanol adsorption. In this study, Pt/C-based nanocomposite catalysts were synthesized incorporating Fe2(MoO4)3 and ZnMoO4 to form heterojunctions through intermittent microwave-assisted polyol method to augment the CO oxidation pathway by introducing hydroxy groups adsorbed on their surfaces. Thorough characterization of the catalysts elucidated their chemical and phase purity, bonding configurations, and oxidation states, with various electroanalytical techniques employed to probe the mechanism of activity enhancement. Furthermore, the distinctive electron density profiles of these molybdate species have been identified as potential facilitators of methanol adsorption on the platinum surface. Equimolar composition in formulating the composite catalysts yielded a fivefold increase in catalytic activity (with ZnMoO4) and a 1.5-fold increase (with Fe2(MoO4)3). This approach demonstrates promise for tailoring Pt/C catalysts to develop industrially viable CO-tolerant and highly stable electrocatalysts.

Fluorine atoms incorporation strengthens the strong metal-support interaction of PtNi@NFGC for enhanced methanol oxidation reaction performance under alkaline media

The regulatory mechanism of strong metal-support interaction (SMSI) is of great significance in improving the electrocatalytic performance for supported electrocatalysts. Here, PtNi alloy nanoparticles were deposited on N, F-codoped graphene-like carbon nanosheets (PtNi@NFGC) to construct a highly active interface for efficient methanol oxidation reaction (MOR), which solves the problems of high cost, poor activity and easy aggregation of Pt-based catalysts. Due to the high electrophilicity, F atoms doping into the carbon lattice can not only manipulate the electron structure and the state of the carbon skeleton, but also further trigger the stronger charge transfer between metal atoms and carbon support. Compared with single-doped PtNi@NGC, N, F-codoped PtNi@NFGC possesses a lower onset potential and methanol oxidation potential, higher methanol oxidation current and stronger CO tolerance. The results of the partial density of state (PDOS) simulation display that N, F-codoping promotes the electron transfer from Pt atoms to NFGC support, and leads to the d-band center shift upward, thus strengthening the oxidation degree of Pt active sites and increasing the composition of high-valent Ptx+. In-situ Raman analysis and density functional theory (DFT) results expound that F atoms embedding observably enhances the adsorption energy of Pt active centers to *OH intermediates, which not only significantly improves MOR catalytic activity, but also achieves efficient methanol dehydrogenation and alleviates CO poisoning. This customization of metal-support interface interaction by heteroatom doping strategy opens up opportunities for designing efficient supported catalysts.

A new highly active and CO2-stable heterostructure cathode material for solid oxide fuel cells developed from bismuth ion-modified cation-deficient Nd0.9BaCo2O5+δ

Efficient oxygen reduction kinetics as well as excellent stability are the main goals of current electrode materials for solid oxide fuel cells (SOFCs). Here, we present the latest findings regarding the augmentation of performance in SOFC through utilization of a novel heterogeneous cathode, consisting of an excess cation-deficient double perovskite Nd0.9BaCo2O5+δ (NBC90) backbone and in situ exsolved BaCo1-yBiyO3-x nanoparticles modified by bismuth (NBC90+B). The anisotropic growth of such self-assembled nanoparticles and the formation of multiple heterointerfaces exhibit an extremely strong activation effect. The in situ formed BaCo1-yBiyO3-x nanoparticles and cation-deficient NBC90 parental perovskite significantly enhance the catalytic activity and durability of the cathode toward oxygen reduction. The structural stability and CO2 tolerance of the cathode are greatly enhanced, which is attributed to the penetration of the high acidic Bi ions in the separated phase and the synergistic effect of the two-phase interface. The results unequivocally demonstrate the exceptional stability and efficiency of the NBC90+B composite as a promising cathode candidate for SOFCs.

A-site alkali metal-doped SrTi0.3Fe0.7O3-δ: A highly stable symmetrical electrode material for solid oxide electrochemical cells

To addresses the limitations in electrode performance observed at temperatures ≤700 °C, attributed to the low oxygen surface exchange coefficient primarily caused by high Sr surface segregation, we developed an electrode performance enhancement strategy involving A-site alkali metal doping to SrTi1-xFexO3-δ (STF)-based perovskite. Here, we present the symmetrical electrode material for solid oxide electrochemical cells (SOCs), Sr0.95Mg0.05Ti0.3Fe0.7O3-δ (SMTF), demonstrating a unique combination of excellent symmetrical electrode performance and long-term stability. A-site Mg doping reduces the Sr surface segregation and improves the conductivity but also significantly enhances its electrochemical performance. At 700 °C, the performance of SMTF symmetric cell in both fuel cell and electrolysis modes is 1.5 times higher than that of STF. Moreover, under air atmosphere, SMTF demonstrates stable performance (>1000 h) at 1 A cm−2, with no degradation observed after 400 h testing under humidified hydrogen conditions. Additionally, SMTF exhibits excellent CO2 tolerance in CO2-rich atmospheres.

Halogen Tailoring of Platinum Electrocatalyst with High CO Tolerance for Methanol Oxidation Reaction

The catalytic activity of platinum for the CO oxidation depends on the interaction of electron donation and back‐donation at the platinum center. Here we demonstrate that the platinum bromine nanoparticles with electron‐rich properties on bromine bonded with sp‐C in graphdiyne (PtBr NPs/Br‐GDY), which is formed by bromine ligand and constitutes an electrocatalyst with a high CO‐resistant for methanol oxidation reaction (MOR). The catalyst showed peak mass activity for MOR as high as 10.4 A mgPt−1, which is 20.8 times higher than the 20% Pt/C. The catalyst also showed robust long‐term stability with slight current density decay after 100 hours at 35 mA cm−2. Structural characterization, experimental, and theoretical studies show that the electron donation from bromine makes the surface of platinum catalysts highly electron‐rich, and can strengthen the adsorption of CO as well as enhance π back‐donation of Pt to weaken the C−O bond to facilitate CO electrooxidation and enhance catalytic performance during MOR. The results highlight the importance of electron‐rich structure among active sites in Pt‐halogen catalysts and provide detailed insights into the new mechanism of CO electrooxidation to overcome CO poisoning at the Pt center on an orbital level.

Rationally Designed L12-Pt2RhFe Intermetallic Catalyst with High CO-Tolerance for Alkaline Methanol Electrooxidation.

It is a grand challenge to deep understanding of and precise control over functional sites for the rational design of highly efficient catalysts for methanol electrooxidation. Here, an L12-Pt2RhFe intermetallic catalyst with integrated functional components is demonstrated, which exhibits exceptional CO tolerance. The Pt2RhFe/C achieves a superior mass activity of 6.43 A mgPt -1, which is 2.23-fold and 3.53-fold higher than those of PtRu/C and Pt/C. Impressively, the Pt2RhFe/C exhibits a significant enhancement in durability owing to its high CO-tolerance and stability. Density functional theory calculations reveal that high performance of Pt2RhFe intermetallic catalyst arises from the synergistic effect: the strong OH binding energy (OHBE) at Fe sites induce stably adsorbed OH species and thus facilitate the dehydrogenation step of methanol via rapid hydrogen transfer, while moderate OHBE at Rh sites promote the formation of the transition state (Pt-CO···OH-Rh) with a low activation barrier for CO removal. This work provides new insights into the role of OH binding strength in the removal of CO species, which is beneficial for the rational design of highly efficient catalysts.

Electrochemical behaviour of redox-robust electrode in contact with protonic electrolyte: Case of double-layered Sr2Fe1.5Mo0.5O6-δ - Ce0.8Sm0.2O2-δ composite

Electrochemical devices based on proton-conducting oxides offer a significant potential for implementation in a variety of high-temperature electrochemical applications. It is a well-known fact that electrochemical devices require active electrodes to function optimally. Over the last few years, Sr2Fe1.5Mo0.5O6-δ has received much attention as an effective redox-robust electrode for oxygen conducting electrolytes. This study presents, for the first time, the results of investigations on a double-layered composite electrode based on Sr2Fe1.5Mo0.5O6-δ in contact with a barium-free proton-conducting electrolyte La0.9Sr0.1ScO3-δ. It was found that the investigated electrode exhibits low polarization resistance about 0.15 and 0.22 Ohm cm2 in wet air and wet hydrogen at 600 °C, respectively. In addition, the electrode exhibits acceptable redox stability and CO2 tolerance. Also, the results of electrochemical impedance spectra analysis and a discussion on the parallel pathways of hydrogen oxidation and oxygen reduction reactions and the nature of rate-determining steps are presented in the manuscript. The obtained results show the high prospects for a Sr2Fe1.5Mo0.5O6-δ - based composite electrode for protonic ceramic electrochemical cells.

Composites of Titanium-Molybdenum Mixed Oxides and Non-Traditional Carbon Materials: Innovative Supports for Platinum Electrocatalysts for Polymer Electrolyte Membrane Fuel Cells.

TiO2-based mixed oxide-carbon composite support for Pt electrocatalysts provides higher stability and CO tolerance under the working conditions of polymer electrolyte membrane fuel cells compared to traditional carbon supports. Non-traditional carbon materials like graphene nanoplatelets and graphite oxide used as the carbonaceous component of the composite can contribute to its affordability and/or functionality. Ti(1-x)MoxO2-C composites involving these carbon materials were prepared through a sol-gel route; the effect of the extension of the procedure through a solvothermal treatment step was assessed. Both supports and supported Pt catalysts were characterized by physicochemical methods. Electrochemical behavior of the catalysts in terms of stability, activity, and CO tolerance was studied. Solvothermal treatment decreased the fracture of graphite oxide plates and enhanced the formation of a reduced graphene oxide-like structure, resulting in an electrically more conductive and more stable catalyst. In parallel, solvothermal treatment enhanced the growth of mixed oxide crystallites, decreasing the chance of formation of Pt-oxide-carbon triple junctions, resulting in somewhat less CO tolerance. The electrocatalyst containing graphene nanoplatelets, along with good stability, has the highest activity in oxygen reduction reaction compared to the other composite-supported catalysts.

Dilute RuCo Alloy Synergizing Single Ru and Co Atoms as Efficient and CO‐Resistant Anode Catalyst for Anion Exchange Membrane Fuel Cells

AbstractRuthenium (Ru) is considered a promising candidate catalyst for alkaline hydroxide oxidation reaction (HOR) due to its hydrogen binding energy (HBE) like that of platinum (Pt) and its much higher oxygenophilicity than that of Pt. However, Ru still suffers from insufficient intrinsic activity and CO resistance, which hinders its widespread use in anion exchange membrane fuel cells (AEMFCs). Here, we report a hybrid catalyst (RuCo)NC+SAs/N‐CNT consisting of dilute RuCo alloy nanoparticles and atomically single Ru and Co atoms on N‐doped carbon nanotubes The catalyst exhibits a state‐of‐the‐art activity with a high mass activity of 7.35 A mgRu−1. More importantly, when (RuCo)NC+SAs/N‐CNT is used as an anode catalyst for AEMFCs, its peak power density reaches 1.98 W cm−2, which is one of the best AEMFCs properties of noble metal‐based catalysts at present. Moreover, (RuCo)NC+SAs/N‐CNT has superior long‐time stability and CO resistance. The experimental and density functional theory (DFT) results demonstrate that the dilute alloying and monodecentralization of the exotic element Co greatly modulates the electronic structure of the host element Ru, thus optimizing the adsorption of H and OH and promoting the oxidation of CO on the catalyst surface, and then stimulates alkaline HOR activity and CO tolerance of the catalyst.

Dilute RuCo Alloy Synergizing Single Ru and Co Atoms as Efficient and CO-Resistant Anode Catalyst for Anion Exchange Membrane Fuel Cells.

Ruthenium (Ru) is considered a promising candidate catalyst for alkaline hydroxide oxidation reaction (HOR) due to its hydrogen binding energy (HBE) like that of platinum (Pt) and its much higher oxygenophilicity than that of Pt. However, Ru still suffers from insufficient intrinsic activity and CO resistance, which hinders its widespread use in anion exchange membrane fuel cells (AEMFCs). Here, we report a hybrid catalyst (RuCo)NC+SAs/N-CNT consisting of dilute RuCo alloy nanoparticles and atomically single Ru and Co atoms on N-doped carbon nanotubes The catalyst exhibits a state-of-the-art activity with a high mass activity of 7.35 A mgRu -1. More importantly, when (RuCo)NC+SAs/N-CNT is used as an anode catalyst for AEMFCs, its peak power density reaches 1.98 W cm-2, which is one of the best AEMFCs properties of noble metal-based catalysts at present. Moreover, (RuCo)NC+SAs/N-CNT has superior long-time stability and CO resistance. The experimental and density functional theory (DFT) results demonstrate that the dilute alloying and monodecentralization of the exotic element Co greatly modulates the electronic structure of the host element Ru, thus optimizing the adsorption of H and OH and promoting the oxidation of CO on the catalyst surface, and then stimulates alkaline HOR activity and CO tolerance of the catalyst.

A-site cation deficient SrTa0.1Fe0.9O3-δ as a bi-functional cathode for both oxygen ion- and proton-conducting solid oxide fuel cells

In order to accelerate the widespread application of solid oxide fuel cells (SOFCs), especially proton-conducing solid oxide fuel cells (PCFCs), it is crucial to develop a cathode material with high activity for the oxygen reduction reaction (ORR), excellent long-term stability and CO2 tolerance. Herein, an A-site deficient cobalt-free (Co-free) perovskite oxide Sr0.95Ta0.1Fe0.9O3-δ (S0.95TF) is prepared by introducing cation deficiencies into SrTa0.1Fe0.9O3-δ (STF), and it proves to be a highly active cathode. The increased oxygen vacancies, the decreased thermal expansion coefficient (TEC) value and improved CO2 tolerance, efficiently enhance electrochemical performance and durability during long-term stability testing. As a result, the area specific resistance (ASR) values of S0.95TF at 600 °C are only 0.095 and 0.42 Ω cm2 with the Sm0.2Ce0.8O1.9 (SDC) and BaZr0.1Ce0.7Y0.1Yb0.1O3-δ (BZCYYb) electrolytes, respectively. In addition, both of the single cells with S0.95TF cathodes, based on different electrolytes, can function stably for 200 h without obvious performance decrease. These results clearly demonstrate that S0.95TF is a highly promising candidate for both oxygen ion-conducting SOFCs and PCFCs.

Calcium-doped double perovskite PrBaFe2O5+δ as a high-performance cathode for solid oxide fuel cells

Fe-based double perovskites represent a significant category of cobalt-free materials and exhibit promise as cathodes for solid oxide fuel cells (SOFCs) because of their lower thermal expansivity and reduced cost. However, they often encounter challenges associated with poor oxygen reduction reactivity stemming from intrinsic low electronic and oxygen-ion conductivity. In this investigation, Ca was introduced as a dopant for the first time to improve the electrochemical properties of PrBaFe2O5+δ (PBFO). The findings unveiled effective adjustments in the formation of oxygen vacancy by introducing Ca into PBFO. Therefore, the oxygen adsorption, dissociation, and charge transfer processes were modulated considerably. At 800 °C, PrBa0.9Ca0.1Fe2O5+δ (PBCFO) exhibited a Rp of 0.027 Ω cm2, representing a 78.1 % reduction in comparison with PBFO. Concurrently, the output power density of the PBCFO increased by 17.3 %. These results underscore the potential of Ca doping to elevate the ORR kinetics and CO2 tolerance of PBFO.

First principles calculation and experimental study of Ln0.125Sr0.875Co0.875Ta0.125O3-δ(Ln = La, Sm, and Nd) as potential cathode materials for intermediate-temperature solid oxide fuel cells

Solid oxide fuel cells (SOFCs), as important energy equipment, have excellent characteristics, including low pollution and high catalytic activity. The cathode, which is the key component of an SOFC, plays a vital role in practical applications. Herein, we study the properties of Ln0.125Sr0.875Co0.875Ta0.125O3-δ (Ln = La, Sm, and Nd, abbreviated as LSCT, SSCT, and NSCT, respectively) cathode materials both theoretically and experimentally. The conductivity of LnSCT gradually decreased with decreasing Ln3+ ionic radius. Density of states (DOS) analysis indicated that LSCT has the highest conductivity owing to the band center of Co 3d being closer to O 1s. Density functional theory (DFT) calculations showed that the SSCT sample has the lowest oxygen vacancy formation energy, which facilitated the formation of oxygen vacancies. The binding energy results show that SSCT and NSCT have relatively good structural stability compared to LSCT. The polarization impedance values of LSCT, SSCT, and NSCT at 700 °C are 0.105, 0.069, and 0.304 Ω cm2, respectively. The CO2 sensitivity of LSCT, SSCT, and NSCT was evaluated by calculating the CO2 adsorption energy and performing impedance tests under different CO2 concentrations. These results indicate that LSCT and SSCT have better CO2 tolerance than NSCT. At 700 °C, for Ln = La, Sm, and Nd, the maximum power of NiCu-SDC/SDC/LSGM/LnSCT electrolyte-supported fuel cell reached 430, 462, and 382 mW cm−2, respectively. These findings provide a reference for the future design and development of SOFCs cathode material.

A medium-entropy engineered double perovskite oxide for efficient and CO2-tolerant cathode of solid oxide fuel cells

Developing highly active and robust cathodes remains challenging for solid oxide fuel cells (SOFCs). Therefore, we report an A-site medium-entropy double perovskite oxide PrBa0.5Sr0.25Ca0.2Ce0.05Co2O5+δ (PBSCCC) and its electrocatalytic activity and CO2 tolerance property are systematically probed. The PBSCCC cathode exhibits excellent oxygen reduction reaction (ORR) activity with a low polarization resistance of 0.027 Ω cm2 at 700 °C. More importantly, compared to PrBaCo2O5+δ (PBC) and PrBa0.8Ca0.2Co2O5+δ (PBCC) oxides, its CO2 resistance is prominently enhanced with significantly less BaCO3 and Co3O4 impurities formed. The superior ORR performance and structure stability are mainly attributed to its high electrical conductivity and significantly reduced surface cation segregations. Our results show that the potential of PBSCCC as a cathode material for SOFCs is enormous and also prove the rationality and feasibility of entropy engineering for cathode development.

A highly oxygen reduction reaction active and CO2 durable high-entropy cathode for solid oxide fuel cells

One big obstacle for the oxygen reduction reaction (ORR) electrode in solid oxide fuel cells (SOFCs) is the poor reaction activity and fast degradations caused by CO2 poisoning. Here we report our design of an active A-site Ca-rich high-entropy Pr0.1875Ba0.1875Sr0.1875La0.1875Ca0.25CoO3-δ (PBSLC25C) electrode, guided by the O p-band theory. When applied as a cathode in solid oxide fuel cells (SOFCs), it demonstrates high ORR activity and excellent CO2 tolerance under realistic operating conditions. Ni-YSZ-based anode-supported cells with PBSLC25C cathodes demonstrate excellent peak power densities of 1.14 W cm−2, 1.04 W cm−2, and 0.77 W cm−2 in the air with 1%, 5%, and 10% CO2, respectively, at 750 °C. The engineered high-entropy PBSLC25C effectively diminishes the CO2 poisoning effect and maintains active surfaces for fast oxygen exchange, as confirmed by the cell durability test in air containing CO2 (5 and 10 vol%), Raman spectroscopy, and density functional theory calculations.

Preparation of high-performance multiphase heterostructures IT-SOFC cathode materials by Pr-induced in situ assembly

Here, in situ assembly in La0.6Sr0.4Co0.2Fe0.8O3-δ and CoFe2O4 composite (LSCFC) cathode was induced by Pr to form La0.6Sr0.4CoxFeyO3-δ/PrCoO3/Co3O4/PrO2 (LSCFC-PI) multiphase heterostructures. The surface of LSCFC-PI forms uniform nanoparticles, and the unique core-shell structure prevents Sr segregation, thereby enhancing CO2 tolerance and increasing oxygen reduction reaction (ORR) active sites. Furthermore, compared with LSCFC, LSCFC-PI increases the oxygen vacancy content of the cathode due to the existence of multiphase heterostructure, improves the ORR kinetics, and the conductivity is also greatly improved. The peak power density (PPD) of LSCFC-PI as a single-cell cathode at 700 ℃ reached 1.51 W cm−2, which was 2.65 times higher than that of LSCFC's 0.57 W cm−2, and in the long-term stability test at a constant voltage ∼0.8 V for 100 hours, showing excellent stability. In situ assembly of multiphase heterostructures is expected to become a new strategy for developing high-performance IT-SOFC cathodes.

Facile Synthesis of PtP2 Nanocrystals as Highly Active Electrocatalysts for Methanol Oxidation.

Although significant efforts have been made in the past few decades, the development of affordable, durable, and effective electrocatalysts for direct methanol fuel cells (DMFCs) remains a formidable challenge. Herein, we present a facile and efficient phosphorization approach for synthesizing PtP2 intermetallic nanocrystals and utilize them as electrocatalysts in the methanol oxidation reaction (MOR). Impressively, the synthesized PtP2 nanocatalysts exhibit a mass activity of 2.14 mA μg-1 and a specific activity of 6.28 mA cm-2, which are 5.1 and 9.5 times higher than those achieved by the current state-of-the-art commercial Pt/C catalyst, respectively. Moreover, the PtP2 nanocatalysts demonstrate improved stability toward acidic MOR by retaining 92.1% of its initial mass activity after undergoing 5000 potential cycles, far surpassing that of the commercial Pt/C (38%). Further DMFC tests present a 2.7 times higher power density than that of the commercial Pt/C, underscoring their potential for application in methanol fuel cells. Density functional theory calculations suggest that the accelerated MOR kinetics and improved CO tolerance on PtP2 can be attributed to the attenuated binding strength of CO intermediates and the enhanced stability due to strong Pt-P interaction. To our knowledge, this is the first report identifying the MOR performance on PtP2 intermetallic nanocrystals, highlighting their potential as highly active and stable nanocatalysts for DMFCs.

Superior Catalytic Performance and Methanol Tolerance of Co@Mesoporous Graphene Nanocomposites toward Oxygen Reduction Reaction

AbstractThe global energy crisis and growing concerns about environmental pollution have spurred researchers to explore eco‐friendly methods of generating clean energy. Previous studies have often relied on noble metal catalysts to facilitate oxygen reduction reactions (ORR) in energy production reactions. However, their high cost has limited their widespread adoption, making the development of highly active and affordable ORR catalysts a significant challenge. In this study, a vacuum heat treatment technique was employed to fabricate a cobalt‐loaded mesoporous graphene (Co−Gs) nanocomposite. The inclusion of cobalt in graphene enhances the reaction, while the presence of mesoporous graphene provides a larger surface area to accommodate the active sites of Co. This synergistic effect promotes the improvement of catalytic performance. Additionally, the stability and methanol tolerance of Co−Gs nanocomposites is also superior than that of Pt−C. The excellent catalytic performance of the Co−Gs nanocomposite is attributed to a four‐electron pathway within the nanocomposite, as demonstrated by electrocatalytic kinetics investigations. Additionally, the interface interaction between the Co nanoparticles and Gs enhances the efficiency of electron transfer, effectively improving the catalytic performance. These findings highlight the potential of Co‐loaded graphene nanocomposites as highly efficient and cost‐effective electrocatalysts for clean energy application.