Electrochemical Oxygen Research Articles

Taxonomy of Antioxidants to Deactivate Reactive Superoxide for Rejuvenating Batteries.

In lithium batteries employing oxygen electrochemistry as their cathodic process, superoxide radical is recognized as a reactive nucleophile that decomposes electrolytes and therefore deteriorate battery durability. Herein, we categorized the antioxidants employed for deactivating reactive superoxide in batteries into three groups after their working mechanisms were clearly understood and classified. Radical scavengers, as the first group, are sacrificed to provide moieties to neutralize the radical activity of superoxide. The reversible superoxide dismutase mimics (SODm's), distinguished from radical scavengers by their catalytic turnover, were divided into two families in terms of the anti-aging mechanism: electron-mediating SODm (e-SODm) and chemo-catalytic SODm (c-SODm). The redox-active e-SODm family, as the second group, mediates an electron from a superoxide radical to another superoxide, driving oxidation to dioxygen and reduction to peroxide, respectively. The c-SODm family, as the third group, chemically catalyzes superoxide disproportionation reaction, lowering the activation energy of the dismutation between the same radicals.

Balancing Activity and Selectivity in Two-electron Oxygen Reduction through First Coordination Shell Engineering in Cobalt Single Atom Catalysts.

The electrochemical two-electron oxygen reduction reaction (2e- ORR) offers a potentially cost-effective and eco-friendly route for the production of hydrogen peroxide (H2O2). However, the competing 4e- ORR that converts oxygen to water limits the selectivity towards hydrogen peroxide. Accordingly, achieving highly selective H2O2 production under low voltage conditions remains challenging. Herein, guided by first-principles density functional theory (DFT) calculations, we show that modulation the first coordination sphere in Co single atom catalysts (Co-N-C catalysts with Co-NxO4-x sites), specifically the replacement of Co-N bonds with Co-O bonds, can weaken the *OOH adsorption strength to boost the selectivity towards H2O2 (albeit with a slight decrease in ORR activity). Further, by synthesizing a series of N-doped carbon-supported catalysts with Co-NxO4-x active sites, we were able to validate the DFT findings and explore the trade-off between catalytic activity and selectivity for 2e- ORR. A catalyst with trans-Co-N2O2 sites exhibited excellent catalytic activity and H2O2 selectivity, affording a H2O2 production rate of 12.86 [[EQUATION]]and an half-cell energy-efficiency of 0.07 [[EQUATION]] during a 100-h H2O2 production test in a flow-cell.

Bias‐Free Photoelectrochemical Water Oxidation Coupled with Electrochemical Oxygen Reduction Reaction via Fe‐Based Electrodes with Long‐Term Operation

AbstractPhotoelectrochemistry (PEC) is a green and sustainable approach in the synthesis of H2O2, depending on the semiconductor to initiate two‐electron water oxidation into hydrogen peroxide (H2O2). However, the photoanodes generally have sluggish charge transfer and a limited number of active sites, which limit the yield and faradaic efficiency (FE) for the production of H2O2. Herein, Ti‐doped Fe2O3 photoanode with the modification of ZnO passivation layer (ZnO/Ti‐Fe2O3) for PEC H2O2 production is developed. The optimized photoanode has shown a high FE and selectivity for two‐electron water oxidation, achieving a yield approaching 0.56 µmol min−1 cm−2 at 1.23 VRHE and an average FE over 80% in the potential range from 1.0 to 1.6 VRHE. Impressively, an unassisted PEC system is designed to generate H2O2 at the ZnO/Ti‐Fe2O3 photoanode while performing an oxygen reduction reaction (ORR) at the Fe(Co)‐NC cathode. The integrated system enables the average PEC H2O2 production rate of 0.275 µmol min−1 cm−2 without applying any additional bias. Moreover, an unassisted PEC cell obtains a long‐term stability of 100 h. This work demonstrates new possibilities in designing efficient and stable PEC assemblies using low‐cost earth‐abundant materials for light‐driven catalysis.

Enhanced electrochemical oxygen reduction reaction on “C–O–Si” bonds in Si-doped graphene-like carbon

The use of heteroatom-doped carbon materials as non-precious metal catalysts for oxygen reduction reactions has attracted much attention from researchers. This paper presents the synthesis of two-dimensional Si-doped graphene-like materials (Si-GLC) featuring “C–O–Si” bonds through an in-situ doping method. Since the electronegativity of the Si (1.90) is much smaller than that of C (2.55) and O (3.44), the formation of the “C–O–Si” bond causes Si to lose a large number of electrons and become positively charged. This increases the adsorption of electronegative oxygen, thereby improving the activity of oxygen reduction reactions. The adsorption energy of oxygen molecules on Si-GLC was calculated to be −3.57 eV using density functional theory, much lower than on GLC (−2.18 eV). This suggests that Si doping enhances the adsorption of oxygen molecules by graphene-like materials, which is crucial for improving the performance of oxygen reduction reaction. Si-GLC displayed a half-wave potential of 0.80 V (vs. RHE) and a diffusion-limited current density of 5.81 mA cm−2 in 0.1 M KOH solution, demonstrating excellent catalytic activity for oxygen reduction reaction. It also exhibits good stability and tolerance to methanol crossover effect. In-situ doping creates “C–O–Si” bonds, modulating charge density and providing a strategy for high-performance oxygen reduction catalysts.

Hydrogen Peroxide Electrosynthesis via Selective Oxygen Reduction Reactions Through Interfacial Reaction Microenvironment Engineering.

The electrochemical two-electron oxygen reduction reaction (2e- ORR) offers a compelling alternative for decentralized and on-site H2O2 production compared to the conventional anthraquinone process. To advance this electrosynthesis system, there is growing interest in optimizing the interfacial reaction microenvironment to boost electrocatalytic performance. This review consolidates recent advancements in reaction microenvironment engineering for the selective electrocatalytic conversion of O2 to H2O2. Starting with fundamental insights into interfacial electrocatalytic mechanisms, an overview of various strategies for constructing the favorable local reaction environment, including adjusting electrode wettability, enhancing mesoscale mass transfer, elevating local pH, incorporating electrolyte additives, and employing pulsed electrocatalysis techniques is provided. Alongside these regulation strategies, the corresponding analyses and technical remarks are also presented. Finally, a summary and outlook on critical challenges, suggesting future research directions to inspire microenvironment engineering and accelerate the practical application of H2O2 electrosynthesis is delivered.

Facile One-Pot Synthesis of Silicon Carbide-Carbon Supported Gold Nanoparticles (Au/SiC-C) as a Durable Electrocatalyst for Electrochemical Oxygen Reduction Reaction

Facile One-Pot Synthesis of Silicon Carbide-Carbon Supported Gold Nanoparticles (Au/SiC-C) as a Durable Electrocatalyst for Electrochemical Oxygen Reduction Reaction

Metal oxide plating for maximizing the performance of ruthenium(IV) oxide-catalyzed electrochemical oxygen evolution reaction.

Hydrogen production by proton exchange membrane water electrolysis requires an anode with low overpotential for oxygen evolution reaction (OER) and robustness in acidic solution. While exploring new electrode materials to improve the performance and durability, optimizing the morphology of typical materials using new methods is a big challenge in materials science. RuO2 is one of the most active and stable electrocatalysts, but further improvement in its performance and cost reduction must be achieved for practical use. Herein, we present a novel technology, named "metal oxide plating", which can provide maximum performances with minimum amount. A uniform single-crystal RuO2 film with thickness of ∼2.5 nm was synthesized by a solvothermal-post heating method at an amount (x) of only 18 μg cm-2 (ST-RuO2(18)//TiO2 NWA). OER stably proceeds on ST-RuO2(18)//TiO2 NWA with ∼100% efficiency to provide a mass-specific activity (MSA) of 341 A gcat-1 at 1.50 V (vs. RHE), exceeding the values for most of the state-of-the-art RuO2 electrodes.

Shedding Light on the Active Species in a Cobalt-Based Covalent Organic Framework for the Electrochemical Oxygen Evolution Reaction.

While considerable efforts have been devoted to developing functionalized covalent organic frameworks (COFs) as oxygen evolution electrocatalysts in recent years, studies related to the investigation of the true catalytically active species for the oxygen evolution reaction (OER) remain lacking in the field. In this work, the active species of a cobalt-functionalized COF (TpBpy-Co) is studied as electrochemical OER catalyst through a series of electrochemical measurements and post-electrolysis characterizations. These results suggest that cobalt oxide-based nanoparticles are formed in TpBpy-Co from Co(II) ions coordinated to the COF backbone when exposing TpBpy-Co to alkaline media, and these newly formed nanoparticles serve as the primary active species for oxygen evolution. The study thus emphasizes that caution is warranted when assessing the catalytic activity of COF electrocatalysts, as the pristine COF may act as the pre-catalyst, with the active species forming only under catalyst operating conditions. Specifically, strong coordination between COFs and metal centers under electrochemical operation conditions is crucial to avoid unintended transformation of COF electrocatalysts. This work thus contributes to the rational development of earth-abundant COF OER catalysts for the production of green hydrogen from renewable resources.

Indium oxide thick-films decorated with PdO and PtO2 particles for oxygen detection in humid environments

Abstract Thick film indium oxide chemiresistive sensors decorated with PdO and PtO2 particles were investigated for oxygen detection under humid conditions (tested ranging from 20%- 80% RH) across a temperature range of 50 °C to 400 °C. The PtO2-decorated In2O3 sensors demonstrated a significantly higher response to oxygen, showing a 500% increase at 200 °C compared to the PdO-decorated sensors (response values of 41 and 8, respectively). Tests in dry air were conducted to assess the effect of humidity on sensor performance, revealing a maximum response of 74 for PtO2-In2O3 at 400 °C, more than three times higher than the response of 22 for PdO-In2O3. Selectivity tests confirmed that the sensors responded more strongly to oxygen than to interfering gases. The integration of an active carbon cloth (ACC) filter effectively reduced interferences from isobutylene and ethylene, enhancing sensor’s selectivity. A comparison of both sensors demonstrated that PtO2-decorated In2O3 has greater potential as an alternative to existing Pb-based electrochemical oxygen sensors, particularly in humid environments.

Engineering Delocalized Polarizations in Metal Oxide Electrodes with Conducting Polymers for Efficient and Durable Water-Splitting.

Oxygen evolution reaction is a pivotal anodic reaction for electrolysis, however, it remains the obstacle from its sluggish reaction kinetics originating from multiple electron transfer pathways at electrochemical interfaces. Especially, it remains a challenge to achieve stable operation at elevated current densities as electrodes suffer oxidative environment in corrosive conditions. Herein, we report that the conducting polymer polypyrrole electrodeposited Pr0.7Sr0.3CoO3 perovskite oxides for durable oxygen evolution electrodes. We found that the conducting polymer electrodeposited oxides exhibited a highly durable electrochemical oxygen evolution performance maintaining >99% of initial activities during the accelerated durability test. Meanwhile, bare metal oxides presented significant performance drops (<6% of initial activities) over the consecutive 20,000 accelerated durability test. High-resolution transmission electron microscope images identified the maintenance of high crystallinity of the heterostructure, suggesting that the electrodeposited pPy clusters can effectively delocalize highly polarized electrodes preventing material corrosion. The overall water electrolysis experiments further demonstrated that the heterostructure showed excellent stability at the high current density of 100 mA cm-2 over 700 hours. This marks the first report of the delocalized polarization benefiting from conducting polymers for durable oxygen evolution for perovskite oxides, suggesting great potential for scalable water electrolysis.

Greatly Enhanced Oxygen Reduction Reaction in Anion Exchange Membrane Fuel Cell and Zn-Air Battery via Hole Inner Edge Reconstruction of 2D Pd Nanomesh.

Platinum group metals (PGM) have yet to be the most active catalysts in various sustainable energy reactions. Their high cost, however, has made maximizing the activity and minimizing the dosage become an urgent priority for the practical applications of emerging technologies. Herein, a novel 2DPd nanomesh structure possessing hole inner reconstructed edges (HIER) with exposed high energy facets and overstretched lattice parameters is fabricated through a facile room-temperature reduction method at gram-scale yields. The HIER enhances the catalytic performance of Pd in electrochemical oxygen reduction reaction (ORR), achieving superior mass activity (MA) of 2.672 A mgPd -1, which is 27.8 fold and 23.6 fold higher, respectively, than those of the commercial Pt/C (0.096 A mgPt -1) and Pd/C (0.113 A mgPd -1) at 0.9 VRHE. Most significantly, in H2-air anion exchange membrane fuel cell (AEMFC) and Zn-air battery (ZAB) applications, this unique Pd catalyst delivers a much-outperformed peak power density of 0.86 and 0.22W cm-2, respectively, compared with 0.54 and 0.13W cm-2 of the commercial Pt/C catalyst, indicating a novel pathway in electrocatalyst designs through HIER engineering.

Reactivity and Stability of Reduced Ir-Weight TiO2-Supported Oxygen Evolution Catalysts for Proton Exchange Membrane (PEM) Water Electrolyzer Anodes.

Reducing the iridium demand in Proton Exchange Membrane Water Electrolyzers (PEM WE) is a critical priority for the green hydrogen industry. This study reports the discovery of a TiO2-supported Ir@IrO(OH)x core-shell nanoparticle catalyst with reduced Ir content, which exhibits superior catalytic performance for the electrochemical oxygen evolution reaction (OER) compared to a commercial reference. The TiO2-supported Ir@IrO(OH)x core-shell nanoparticle configuration significantly enhances the OER Ir mass activity from 8 to approximately 150 A gIr-1 at 1.53 VRHE while reducing the iridium packing density from 1.6 to below 0.77 gIr cm-3. These advancements allow for viable anode layer thicknesses with lower Ir loading, reducing iridium utilization at 70% LHV from 0.42 to 0.075 gIr kW-1 compared to commercial IrO2/TiO2. The identification of the Ir@IrO(OH)x/TiO2 OER catalyst resulted from extensive HAADF-EDX microscopic analysis, operando XAS, and online ICP-MS analysis of 30-80 wt % Ir/TiO2 materials. These analyses established correlations among Ir weight loading, electrode electrical conductivity, electrochemical stability, and Ir mass-based OER activity. The activated Ir@IrO(OH)x/TiO2 catalyst-support system demonstrated an exceptionally stable morphology of supported core-shell particles, suggesting strong catalyst-support interactions (CSIs) between nanoparticles and crystalline oxide facets. Operando XAS analysis revealed the reversible evolution of significantly contracted Ir-O bond motifs with enhanced covalent character, conducive to the formation of catalytically active electrophilic OI- ligand species. These findings indicate that atomic Ir surface dissolution generates Ir lattice vacancies, facilitating the emergence of electrophilic OI- species under OER conditions, while CSIs promote the reversible contraction of Ir-O distances, reforming electrophilic OI- and enhancing both catalytic activity and stability.

Machine Learning-Aided Discovery of Low-Pt High Entropy Intermetallic Compounds for Electrochemical Oxygen Reduction Reaction.

Advancing the design of cathode catalysts to significantly maximize platinum utilization and augment the longevity has emerged as a formidable challenge in the field of fuel cells. Herein, we rationally design a high entropy intermetallic compound (HEIC, Pt(FeCoNiCu)3) for catalyzing oxygen reduction reaction (ORR) by an efficient machine learning stategy, where crystal graph convolutional neural networks are employed to expedite the multicomponent design. Based on a dataset generated from first-principles calculations, the model can achieve a high prediction accuracy with mean absolute errors of 0.003 for surface strain and 0.011 eV atom-1 for formation energy. In addition, we identify two chemical features (atomic size difference and mixing enthalpy) as new descriptors to explore advanced ORR catalysts. The carbon supported Pt(FeCoNiCu)3 catalyst with small particle size is successfully synthesized by a freeze-drying-annealing technology, and exhibits ultrahigh mass activity (4.09 A mgPt -1) and specific activity (7.92 mA cm-2). Meanwhile, The catalyst also shows significantly enhanced electrochemical stability which can be ascribed to the sluggish diffussion effect in the HEIC structure. Beyond offering a promising low-Pt electrocatalysts for fuel cell cathode, this work offers a new paradigm to rationally design advanced catalysts for energy storage and conversion devices.

Stabilization of High‐Valent Molecular Cobalt Sites through Oxidized Phosphorus in Reduced Graphene Oxide for Enhanced Oxygen Evolution Catalysis

AbstractHeterogeneous molecular cobalt (Co) sites represent one type of classical catalytic sites for electrochemical oxygen evolution reaction (OER) in alkaline solutions. There are dynamic equilibriums between Co2+, Co3+ and Co4+ states coupling with OH−/H+ interaction before and during the OER event. Since the emergence of Co2+ sites is detrimental to the OER cycle, the stabilization of high‐valent Co sites to shift away from the equilibrium becomes critical and is proposed as a new strategy to enhance OER. Herein, phosphorus (P) atoms were doped into reduced graphene oxide to link molecular Co2+ acetylacetonate toward synthesizing a novel heterogeneous molecular catalyst. By increasing the oxidation states of P heteroatoms, the linked Co sites were spontaneously oxidized from 2+ to 3+ states in a KOH solution through OH− ions coupling at an open circuit condition. With excluding the Co2+ sites, the as‐derived Co sites with 3+ initial states exhibited intrinsically high OER activity, validating the effectiveness of the strategy of stabilizing high valence Co sites.

Electronic Synergistic Effects on the Stability and Oxygen Evolution Reaction Efficiency of the Mesoporous LiMn2-xMxO4 (M = Mn, Fe, Co, Ni, and Cu) Electrodes.

Stable porous manganese oxide-based electrodes are essential for clean energy generation and storage because of their high natural abundance and health safety. This investigation focuses on mesoporous LiMn2-xMxO4 (where M is Fe, Co, Ni, and Cu and x is 0, 0.1, 0.3, 0.5, and 0.67) electrodes and thin/thick films. The mesoporous electrodes and films are fabricated by coating clear and homogeneous ethanol solutions of the salts (LiNO3, [Mn(OH2)4](NO3)2, and [M(OH2)x](NO3)2) and surfactants (P123 and CTAB) and calcining at elevated temperature (denoted as F-LiMn2-xMxO4, G-LiMn2-xMxO4, and meso-LiMn2-xMxO4, respectively). The electrochemical properties, stability, and oxygen evolution reaction (OER) performance of the F/G-LiMn2-xMxO4 electrodes are investigated in alkaline media using a three electrode setup. The F-LiMn1.33M0.67O4 electrodes (where M is Mn, Fe, Co, and Ni) exhibit low Tafel slopes of 60, 43, 44, and 32 mV/dec, respectively. While all the Mn-rich and F-LiMn2-xFexO4 electrodes degrade via Mn(VI) disproportionation reaction, the 33% Co electrode shows high stability during the OER. The nickel-based electrodes are stable with as little as 15% Ni and display excellent OER performance over 25% Ni, albeit undergoing a transformation that accumulates Ni(OH)2 species on the electrode surface. Copper in the F-LiMn2-xCuxO4 electrodes is homogeneous at low Cu percentages but forms a CuO phase above 15% Cu, undergoes degradation, and displays a weak OER performance. In short, Co and Ni stabilize the F-LiMn1.33Co0.67O4 and F-LiMn1.7Ni0.3O4 electrodes, which display excellent OER performance.

Fluorine-Doped Graphene Oxide-Modified Graphite Felt Cathode for Hydrogen Peroxide Generation

Electrochemical oxygen reduction via the two-electron pathway (2e-ORR) is an emerging method for producing H2O2. It is cleaner, safer, and more convenient compared to the anthraquinone process. Graphite felt is one of the cathode candidates for large-scale cells due to its excellent mechanical properties. However, commercial graphite felt often fails to achieve the desired hydrogen-peroxide yield because of its low catalytic selectivity for the 2e-ORR pathway. Fluorine-doped carbon materials are expected to enhance 2e-ORR selectivity. This is because the electronic structure of carbon atoms adjacent to fluorine atoms may facilitate the production of hydrogen peroxide while hindering its further reduction. In this study, fluorine-doped graphene oxide (FGO) was prepared by the hydrothermal method. Subsequently, graphite felt modified with FGO was fabricated and used as the cathode for H2O2 production. The results indicated that in alkaline media, the graphite felt modified with FGO achieved a catalytic selectivity of 93% and a generation rate of 8.91 mg cm⁻2 h⁻¹. In comparison, commercial graphite felt had a catalytic selectivity of 75% and a generation rate of 2.10 mg cm⁻2 h⁻¹. Moreover, graphite felt modified by FGO also exhibited excellent electrocatalytic performance for H2O2 generation in neutral media. This research provides a fundamental study to promote the application of graphite felt in the environmentally friendly electrocatalytic production of hydrogen peroxide in industries.

Nitrogen and boron coordinating atoms adjust single-atom catalyst anchored on divacancy defect graphene for highly efficient electrochemical oxygen reduction

In this study, spin-polarized density functional theory (DFT) calculations were utilized to explore the oxygen reduction reaction (ORR) on a transition metal anchored to divacancy graphene (TM@dv-graphene). Our findings demonstrate that divacancy graphene serves as an effective substrate for stabilizing single transition metals, thereby facilitating the ORR. We elucidate the mechanisms of ORR by examining the adsorption of O2, OOH, OH, 2OH, and O intermediates, and identifying two competing ORR pathways: the O* and 2OH* mechanisms. Most TM@dv-graphene catalysts predominantly favor the O* mechanism, with Rh and Ir being notable exceptions that preferentially follow the 2OH* mechanism. Moreover, catalysts co-coordinated with B and N atoms significantly enhance the adsorption of key intermediates, thereby improving ORR activity Specifically, the Co-N4, Co-N2B2, Pd-N2B2, and Pt-N2B2 catalysts demonstrate promising ORR activity with lower overpotentials of 0.47, 0.46, 0.58, and 0.46 V, respectively. This work establishes a foundational framework for comprehending the electrochemical mechanisms of ORR, thus facilitating the design of highly efficient single-atom electrocatalysts.

Unveiling the Activity Origin of Electrochemical Oxygen Evolution on Heteroatom‐Decorated Carbon Matrix

AbstractChemical modification via functional dopants in carbon materials holds great promise for elevating catalytic activity and stability. To gain comprehensive insights into the pivotal mechanisms and establish structure‐performance relationships, especially concerning the roles of dopants, remains a pressing need. Herein, we employ computational simulations to unravel the catalytic function of heteroatoms in the acidic oxygen evolution reaction (OER), focusing on a physical model of high‐electronegative F and N co‐doped carbon matrix. Theoretical and experimental findings elucidate that the enhanced activity originates from the F and pyridinic‐N (Py−N) species that achieve carbon activation. This activated carbon significantly lowers the conversion energy barrier from O* to OOH*, shifts the potential‐limiting step from OOH* formation to O* generation, and ultimately optimizes the energy barrier of the potential‐limiting step. This wok elucidates that the critical role of heteroatoms in catalyzing the reaction and unlocks the potential of carbon materials for acidic OER.

Surface‐Engineered Pt‐Ni(111) Nanocatalysts for Boosting Their ORR Performance via Thermal Treatment

AbstractThe electrochemical oxygen reduction reaction (ORR) is critical for fuel cell application, and modifying surface structures of electrocatalysts has proven effective in improving their catalytic performances. In this study, we investigated surface‐engineered Pt−Ni nano‐octahedra subjected to annealing in various atmospheres. All octahedral nanocrystals retained their Pt−Ni {111} facets at an elevated temperature following the annealing treatments. Air annealing led to the formation of nickel‐rich shells on the Pt−Ni surface. In contrast, hydrogen (H₂) as a reducing gas facilitated the reduction of surface Ni species, incorporating them into the Pt−Ni bulk alloy, which resulted in superior mass activity and specific activity for ORR‐approximately 2.4 and 2.3 times as high as those from the unmodified counterpart, respectively. After 20,000 potential cycles, the H₂/Ar‐annealed Pt−Ni nano‐octahedra maintained a mass activity of 3.92 A/ , surpassing the initial mass activity of the unannealed counterparts (2.95 A/ ). These findings demonstrate a viable approach for tailoring catalyst surfaces to enhance performance in various energy storage and conversion applications.

Unveiling the Activity Origin of Electrochemical Oxygen Evolution on Heteroatom-Decorated Carbon Matrix.

Chemical modification via functional dopants in carbon materials holds great promise for elevating catalytic activity and stability. To gain comprehensive insights into the pivotal mechanisms and establish structure-performance relationships, especially concerning the roles of dopants, remains a pressing need. Herein, we employ computational simulations to unravel the catalytic function of heteroatoms in the acidic oxygen evolution reaction (OER), focusing on a physical model of high-electronegative F and N co-doped carbon matrix. Theoretical and experimental findings elucidate that the enhanced activity originates from the F and pyridinic-N (Py-N) species that achieve carbon activation. This activated carbon significantly lowers the conversion energy barrier from O* to OOH*, shifts the potential-limiting step from OOH* formation to O* generation, and ultimately optimizes the energy barrier of the potential-limiting step. This wok elucidates that the critical role of heteroatoms in catalyzing the reaction and unlocks the potential of carbon materials for acidic OER.