Self-sacrificial template synthesis of Fe,N co-doped porous carbon as efficient oxygen reduction electrocatalysts towards Zn-air battery application

Designing highly efficient non-precious based electrocatalysts for oxygen reduction reaction（ORR） is of significance for the rapid development of metal-air batteries.Herein,a hydrothermal-pyrolysis method is employed to fabricate Fe,N co-doped porous carbon materials as effective ORR electrocatalyst through adopting graphitic carbon nitride（g-C₃ N₄） as both the self-sacrificial templates and N sources.The gC₃ N₄ provides a high concentration of unsatur...     

Integrated Ultrafine Co0.85Se in Carbon Nanofibers: An Efficient and Robust Bifunctional Catalyst for Oxygen Electrocatalysis

Transition-metal selenides are emerging as alternative bifunctional catalysts for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR); however, their activity and stability are still less than desirable. Herein, ultrafine Co_0.85Se nanoparticles encapsulated into carbon nanofibers (CNFs), Co_0.85Se@CNFs, is reported as an integrated bifunctional catalyst for OER and ORR. This catalyst exhibits a low OER potential of 1.58 V vs. reversible hydrogen electrode (RHE) (E_{J=10, OER}) to achieve a current density (J) of 10 mA cm⁻² and a high ORR potential of 0.84 V vs. RHE (E_{J=−1, ORR}) to reach −1 mA cm⁻². Thus, the potential between E_{J=10, OER} and E_{J=−1, ORR} is only 0.74 V, indicating considerable bifunctional activity. The excellent bifunctionality can be attributed to high electronic conduction, abundant electrochemically active sites, and the synergistic effect of Co_0.85Se and CNFs. Furthermore, this Co_0.85Se@CNFs catalyst displays good cycling stability for both OER and ORR. This study paves a new way for the rational design of hybrid catalysts composed of transition-metal selenides and carbon materials for efficiently catalyzing OER and ORR.     

Efficient Fe‐Co‐N‐C Electrocatalyst Towards Oxygen Reduction Derived from a Cationic CoII‐based Metal–Organic Framework Modified by Anion‐Exchange with Potassium Ferricyanide

Fe‐Co‐N‐C electrocatalysts have proven superior to their counterparts (e.g. Fe‐N‐C or Co‐N‐C) for the oxygen reduction reaction (ORR). Herein, we report on a unique strategy to prepare Fe‐Co‐N‐C?x (x refers to the pyrolysis temperature) electrocatalysts which involves anion‐exchange of [Fe(CN)₆]^3? into a cationic Co^II‐based metal‐organic framework precursor prior to heat treatment. Fe‐Co‐N‐C‐900 exhibits an optimal ORR catalytic performance in an alkaline electrolyte with an onset potential (E_onset: 0.97 V) and half‐wave potential (E_1/2: 0.86 V) comparable to that of commercial Pt/C (E_onset=1.02 V; E_1/2=0.88 V), which outperforms the corresponding Co‐N‐C‐900 sample (E_onset=0.92 V; E_1/2=0.84 V) derived from the same MOF precursor without anion‐exchange modification. This is the first example of Fe‐Co‐N‐C electrocatalysts fabricated from a cationic Co^II‐based MOF precursor that dopes the Fe element via anion‐exchange, and our current work provides a new entrance towards MOF‐derived transition‐metal (e.g. Fe or Co) and nitrogen‐codoped carbon electrocatalysts with excellent ORR activity.     

Anchoring Fe Species on the Highly Curved Surface of S and N Co-Doped Carbonaceous Nanosprings for Oxygen Electrocatalysis and a Flexible Zinc-Air Battery

Oxygen reduction reaction (ORR) is of critical significance in the advancement of fuel cells and zinc-air batteries. The iron-nitrogen (Fe−N_x) sites exhibited exceptional reactivity towards ORR. However, the task of designing and controlling the local structure of Fe species for high ORR activity and stability remains a challenge. Herein, we have achieved successful immobilization of Fe species onto the highly curved surface of S, N co-doped carbonaceous nanosprings (denoted as FeNS/Fe₃C@CNS). The induction of this twisted configuration within FeNS/Fe₃C@CNS arose from the assembly of chiral templates. For electrocatalytic ORR tests, FeNS/Fe₃C@CNS exhibits a half-wave potential (E_1/2) of 0.91 V in alkaline medium and a E_1/2 of 0.78 V in acidic medium. The Fe single atoms and Fe₃C nanoparticles are coexistent and play as active centers within FeNS/Fe₃C@CNS. The highly curved surface, coupled with S substitution in the coordination layer, served to reduce the energy barrier for ORR, thereby enhancing the intrinsic catalytic activity of the Fe single-atom sites. We also assembled a wearable flexible Zn-air battery using FeNS/Fe₃C@CNS as electrocatalysts. This work provides new insights into the construction of highly curved surfaces within carbon materials, offering high electrocatalytic efficacy and remarkable performance for flexible energy conversion devices.     

A Phthalocyanine‐Based Layered Two‐Dimensional Conjugated Metal–Organic Framework as a Highly Efficient Electrocatalyst for the Oxygen Reduction Reaction

Layered two‐dimensional (2D) conjugated metal–organic frameworks (MOFs) represent a family of rising electrocatalysts for the oxygen reduction reaction (ORR), due to the controllable architectures, excellent electrical conductivity, and highly exposed well‐defined molecular active sites. Herein, we report a copper phthalocyanine based 2D conjugated MOF with square‐planar cobalt bis(dihydroxy) complexes (Co‐O₄) as linkages (PcCu‐O₈‐Co) and layer‐stacked structures prepared via solvothermal synthesis. PcCu‐O₈‐Co 2D MOF mixed with carbon nanotubes exhibits excellent electrocatalytic ORR activity (E_1/2=0.83 V vs. RHE, n=3.93, and j_L=5.3 mA cm^?2) in alkaline media, which is the record value among the reported intrinsic MOF electrocatalysts. Supported by in situ Raman spectro‐electrochemistry and theoretical modeling as well as contrast catalytic tests, we identified the cobalt nodes as ORR active sites. Furthermore, when employed as a cathode electrocatalyst for zinc–air batteries, PcCu‐O₈‐Co delivers a maximum power density of 94 mW cm^?2, outperforming the state‐of‐the‐art Pt/C electrocatalysts (78.3 mW cm^?2).     

吡啶掺杂碳载钴酞菁催化氧还原的电化学性能及在燃料电池中的应用

以碳黑(Vulcan XC-72R)为载体, 吡啶(Py)和钴酞菁(CoPc)为催化剂前驱体, 经溶剂分散法制备了Py掺杂碳负载纳米钴酞菁复合催化剂(Py-CoPc/C). 通过扫描电镜-能谱分析(SEM-EDS)、X射线光电子能谱(XPS)分析和X射线衍射(XRD)分析技术对催化剂的组成和微观结构进行了表征, 并运用线性扫描循环伏安法(LSV)和旋转圆盘电极(RDE)技术考察了不同Py掺杂含量对碳载钴酞菁(CoPc/C)催化氧还原反应(ORR)活性的影响及稳定性. 结果显示: Py掺杂可以明显改善CoPc/C 对ORR的电催化性能, 其中掺杂20%Py下所制备的20%Py-20%CoPc/C 催化剂对ORR表现出最佳的催化活性, 以其制备的气体扩散电极在O₂气氛饱和的0.1 mol·L^-1 KOH 电解质溶液中, 0.2 V (相对于标准氢电极)即可产生明显的氧还原电流, 半波电位为-0.03 V. 相比于40%Py/C 和未掺杂的40%CoPc/C, 20%Py-20%CoPc/C催化剂的半波电位分别正移了160 和15 mV. 进一步运用RDE理论研究表明, 在Py-CoPc/C 电极上ORR的电子转移总数为2.38, 高于CoPc/C电极上的电子转移总数1.96, 从而使ORR的选择性明显提高. SEM-EDS和XRD分析表明Py掺杂提高了CoPc/C催化剂的分散性和N含量, 更利于O₂的吸附. XPS分析表明: 吡啶结构的N与石墨结构的N均存在于Py-CoPc/C 催化剂中,与催化剂表面的Co离子配位可能是促使ORR活性提高的原因. 最后以20%Py-20%CoPc/C制备了膜电极组装(MEA)电极, 应用于H₂/O₂ 燃料电池单电池发电, 室温下获得最大发电功率密度为21 mW·cm^-2, 相对于CoPc/C提高至2.4倍.     

Polymer-Assisted Electrophoretic Synthesis of N-Doped Graphene-Polypyrrole Demonstrating Oxygen Reduction with Excellent Methanol Crossover Impact and Durability

The design and synthesis of metal-free catalysts with superior electrocatalytic activity, high durability, low cost, and under mild conditions is extremely desirable but remains challenging. To address this problem, a polymer-assisted electrochemical exfoliation technique of graphite in the presence of an aqueous acidic medium is reported. This simple, cost-effective, and mass-scale production approach could open the possibility for the synthesis of high-quality nitrogen-doped graphene–polypyrrole (NG-PPy). The NG-PPy catalyst displays an improved half wave potential (E_1/2=0.77 V) in alkaline medium compared with G-PPy (E_1/2=0.66 V). Most importantly, this catalyst demonstrates excellent stability with high methanol tolerance, and it outperforms the commercial Pt/C catalyst and other previously reported metal-free catalysts. The content of graphitic nitrogen atoms is the key factor for the enhancement of electrocatalytic activity towards oxygen reduction reactions (ORR). Interestingly, the NG-PPy catalyst can be used as a cathode material in a zinc–air battery, which demonstrates a higher peak power density (59 mW cm⁻²) than G-PPy (36.6 mW cm⁻²), highlighting the importance of the low-cost material synthesis approach towards the development of metal-free efficient ORR catalysts for fuel cell and metal–air battery applications. Remarkably, the polymer-assisted electrophoretic exfoliation of graphite with a high yield (≈88 wt %) of few-layer graphene flakes could pave the way towards the mass production of high-quality graphene for a variety of applications.     

S-Block Potassium Single-atom Electrocatalyst with K−N4 Configuration Derived from K+/Polydopamine for Efficient Oxygen Reduction

Currently, single-atom catalysts (SACs) research mainly focuses on transition metal atoms as active centers. Due to their delocalized s/p-bands, the s-block main group metal elements are typically regarded as catalytically inert. Herein, an s-block potassium SAC (K−N−C) with K-N₄ configuration is reported for the first time, which exhibits excellent oxygen reduction reaction (ORR) activity and stability under alkaline conditions. Specifically, the half-wave potential (E_1/2) is up to 0.908 V, and negligible changes in E_1/2 are observed after 10,000 cycles. In addition, the K−N−C offers an exceptional power density of 158.1 mW cm⁻² and remarkable durability up to 420 h in a Zn-air battery. Density functional theory (DFT) simulations show that K−N−C has bifunctional active K and C sites, can optimize the free energy of ORR reaction intermediates, and adjust the rate-determining steps. The crystal orbital Hamilton population (COHP) results showed that the s orbitals of K played a major role in the adsorption of intermediates, which was different from the d orbitals in transition metals. This work significantly guides the rational design and catalytic mechanism research of s-block SACs with high ORR activity.     

Efficient Oxygen Reduction Reaction (ORR) Catalysts Based on Single Iron Atoms Dispersed on a Hierarchically Structured Porous Carbon Framework

Single Fe atoms dispersed on hierarchically structured porous carbon (SA‐Fe‐HPC) frameworks are prepared by pyrolysis of unsubstituted phthalocyanine/iron phthalocyanine complexes confined within micropores of the porous carbon support. The single‐atom Fe catalysts have a well‐defined atomic dispersion of Fe atoms coordinated by N ligands on the 3D hierarchically porous carbon support. These SA‐Fe‐HPC catalysts are comparable to the commercial Pt/C electrode even in acidic electrolytes for oxygen reduction reaction (ORR) in terms of the ORR activity (E_1/2=0.81 V), but have better long‐term electrochemical stability (7 mV negative shift after 3000 potential cycles) and fuel selectivity. In alkaline media, the SA‐Fe‐HPC catalysts outperform the commercial Pt/C electrode in ORR activity (E_1/2=0.89 V), fuel selectivity, and long‐term stability (1 mV negative shift after 3000 potential cycles). Thus, these nSA‐Fe‐HPCs are promising non‐platinum‐group metal ORR catalysts for fuel‐cell technologies.     

Zeolitic Imidazolate Frameworks Derived Co9S8/Nitrogen-Doped Hollow Porous Carbon Spheres as Efficient Bifunctional Electrocatalysts for Rechargeable Zinc–Air Batteries

The development of nonprecious metal-based electrocatalysts with remarkable catalytic activity and long-cycling lifespan toward oxygen reduction reaction (ORR) and evolution reaction (OER) is especially important for rechargeable zinc–air batteries (ZABs). Herein, monodispersed Co₉S₈ nanoparticles embedded in nitrogen-doped hierarchically porous hollow carbon spheres (Co₉S₈ NPs/NHCS) are synthesized through a template-assisted strategy followed by a co-assembly, thermal annealing, and sulfurization process. Benefiting from larger specific surface area, hierarchically porous hollow structure, and carbon nanotubes self-growth, the obtained Co₉S₈ NPs/NHCS-0.5 electrocatalyst exhibits decent performance for ORR (E_1/2=0.85 V) and OER (E₁₀=1.55 V). A rechargeable ZAB assembled using the Co₉S₈ NPs/NHCS-0.5 as air cathode delivers a maximum power density of 116 mW cm⁻², high open circuit voltage of 1.47 V, and good durability (no obvious voltage decay after 1200 cycles (200 hours)). Such a hierarchically porous hollow structure of Co₉S₈ NPs/NHCS-0.5 provides a confined space shell and an interconnected hollow core to achieve outstanding bifunctional catalytic activity and cycling stability, which surpass the benchmark Pt/C-RuO₂.     

Metal-Free B,N co-Doped Hierarchical Porous Carbon Electrocatalyst with an Excellent O2 Reduction Performance

Fuel cells have attracted increasing attention due to their low cost, high energy density, low environmental pollution, and abundant raw materials. Oxygen reduction reaction (ORR) is a core technology of fuel cells, and the development of new electrocatalysts with high ORR performance is highly desirable. Herein, we synthesize a series of B, N co-doped hierarchical porous carbons using a soft template method with the integration of self-assembly, calcination and etching. The obtained materials exhibit hierarchical porous structures, controllable pore distribution, partial graphite structures, and B, N co-doping. They can function as the cost-effective and metal-free electrocatalysts, facilitating the diffusion of electrolyte ions and the improvement of ORR performance. Especially, the B, N co-doped porous carbon with the B-to-N molar ratio of 5 (BNC-5) displays a high ORR activity with a half-wave potential (E_1/2) of 0.73 V, an onset potential (E_onset) of 0.94 V, and a high limiting current density (J_L) of 5.98 mA cm⁻², superior to the N-doped C (NC) and BNC-1 (the B-to-N molar ratio=1), BNC-3 (the B-to-N molar ratio=3) and BNC-7 (the B-to-N molar ratio=7) under the identical conditions. Moreover, the BNC-5 exhibits good cycling stability after 5000 cyclic voltammetry (CV) cycles and excellent tolerance toward even 3 M methanol. This research provides a new approach for the facile synthesis of dual element-doped carbon electrocatalysts with high ORR performance.     

Defect-enriched heterointerfaces N–MoO2–Mo2C supported Pd nanocomposite as a novel multifunctional electrocatalyst for oxygen reduction reaction and overall water splitting

Developing highly efficient, cost-saving, and durable multifunctional electrocatalysts for oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and hydrogen evolution reaction (HER) continues to be a significant challenge in the energy field. In this work, we decide to prepare an unusual multifunctional electrocatalyst, such as icosahedral palladium nanocrystals (PdNCs) encapsulating on N–MoO₂–Mo₂C half-hollow nanotube (HHNT) heterointerface, using an in-situ chemical reaction and following sonic probe irradiation method. All the experiments demonstrate that special defect-enriched heterointerfaces N–MoO₂–Mo₂C supported Pd nanocomposite can greatly improve the ORR activity (E_onset = 1.01 V and E_1/2 = 0.90 V) with good stability, outstanding HER (η₁₀ = 65 mV) and OER (η₁₀ = 180 mV) performances than those of commercial precious electrocatalysts (Platinum on carbon [Pt/C] and ruthenium oxide [RuO₂]). The overall water splitting electrolyzer fabricates by Pd/N–MoO₂–Mo₂C as both anode and cathode electrodes to achieve a current density of 10 Ma/cm² at a cell voltage of 1.56 V, which surpasses the most recent reported electrocatalysts.     

Decorating Single-Atomic Mn Sites with FeMn Clusters to Boost Oxygen Reduction Reaction

The regulation of electron distribution of single-atomic metal sites by atomic clusters is an effective strategy to boost their intrinsic activity of oxygen reduction reaction (ORR). Herein we report the construction of single-atomic Mn sites decorated with atomic clusters by an innovative combination of post-adsorption and secondary pyrolysis. The X-ray absorption spectroscopy confirms the formation of Mn sites via Mn-N₄ coordination bonding to FeMn atomic clusters (FeMn_ac/Mn-N₄C), which has been demonstrated theoretically to be conducive to the adsorption of molecular O₂ and the break of O−O bond during the ORR process. Benefiting from the structural features above, the FeMn_ac/Mn-N₄C catalyst exhibits excellent ORR activity with half-wave potential of 0.79 V in 0.5 M H₂SO₄ and 0.90 V in 0.1 M KOH as well as preeminent Zn-air battery performance. Such synthetic strategy may open up a route to construct highly active catalysts with tunable atomic structures for diverse applications.     

Singlet Oxygen Induced Site-Specific Etching Boosts Nitrogen-Carbon Sites for High-Efficiency Oxygen Reduction

Targeted construction of carbon defects near the N dopants is an intriguing but challenging way to boost the electrocatalytic activity of N-doped carbon toward oxygen reduction reaction (ORR). Here, we report a novel site-specific etching strategy that features targeted anchoring of singlet oxygen (¹O₂) on the N-adjacent atoms to directionally construct topological carbon defects neighboring the N dopants in N-doped carbon (¹O₂−N/C). This ¹O₂−N/C exhibits the highest ORR half-wave potential of 0.915 V_RHE among all the reported metal-free carbon catalysts. Pyridinic-N bonded with a carbon pentagon of the neighboring topological carbon defects is identified as the primary active configuration, rendering enhanced adsorption of O₂, optimized adsorption energy of the ORR intermediates, and a significantly decreased total energy barrier for ORR. This ¹O₂-induced site-specific etching strategy is also applicable to different precursors, showing a tremendous potential for targeted construction of high-efficiency active sites in carbon-based materials.     

Imine Gels Based on Ferrocene and Porphyrin and Their Electrocatalytic Property

A series of porphyrin‐based imine gels have been synthesized via dynamic covalent gelation between 5,10,15,20‐tetra(4‐aminophenyl)‐21H,23H‐porphyrin (H₂TAPP) derivatives and various aldehyde compounds. The porphyrin‐ferrocene imine gels based on MTAPP (M=H₂, Ni²⁺, Co²⁺, Pd²⁺ and Zn²⁺) and ferrocene‐1,1′‐dicarbaldehyde (NA) display efficient HER, OER and ORR activities in alkaline media. Among the gels, CoTAPP‐NA shows an HER current density of 10 mA cm^?2 at low overpotential of 470 mV and small Tafel slope of 110 mV decade^?1 in alkaline media. CoTAPP‐NA also exhibits OER catalytic activity with low overpotential (416 mV for 10 mA cm^?2). CoTAPP‐NA shows ability in overall water splitting in alkaline media. In addition, CoTAPP‐NA exhibits onset potential (E_p) of 0.95 V and half‐wave potential (E_1/2) of 0.84 V in 1.0 mol L^?1 KOH solution for oxygen reduction. Moreover, the gel catalyst shows good stability.     

Construction of Co4 Atomic Clusters to Enable Fe−N4 Motifs with Highly Active and Durable Oxygen Reduction Performance

Fe−N−C catalysts with single-atom Fe−N₄ configurations are highly needed owing to the high activity for oxygen reduction reaction (ORR). However, the limited intrinsic activity and dissatisfactory durability have significantly restrained the practical application of proton-exchange membrane fuel cells (PEMFCs). Here, we demonstrate that constructing adjacent metal atomic clusters (ACs) is effective in boosting the ORR performance and stability of Fe−N₄ catalysts. The integration of Fe−N₄ configurations with highly uniform Co₄ ACs on the N-doped carbon substrate (Co₄@/Fe₁@NC) is realized through a “pre-constrained” strategy using Co₄ molecular clusters and Fe(acac)₃ implanted carbon precursors. The as-developed Co₄@/Fe₁@NC catalyst exhibits excellent ORR activity with a half-wave potential (E_1/2) of 0.835 V vs. RHE in acidic media and a high peak power density of 840 mW cm⁻² in a H₂−O₂ fuel cell test. First-principles calculations further clarify the ORR catalytic mechanism on the identified Fe−N₄ that modified with Co₄ ACs. This work provides a viable strategy for precisely establishing atomically dispersed polymetallic centers catalysts for efficient energy-related catalysis.     

Highly efficient iron–nitrogen electrocatalyst derived from covalent organic polymer for oxygen reduction

Developing non-precious metal catalyst with high activity, good stability and low cost for electrocatalytic oxygen reduction reaction(ORR) is critical for the wide application of energy conversion system. Here, we developed a cost–effective synthetic strategy via silica assistance to obtain a novel Fe_3C/Fe–N_x–C(named as COPBP-PB-Fe-900-SiO_2) catalyst with effective active sites of Fe–N_xand Fe_3C from the rational design two-dimensional covalent organic polymer(COPBP-PB). The nitrogen-rich COP effectively promotes the formation of active Fe–N_x sites. Additionally, the silica not only can effectively suppress the formation of large Fe-based particles in the catalysts, but also increases the degree of carbonization of the catalyst.The as-prepared COPBP-PB-Fe-900-SiO_2 catalyst exhibits high electrocatalytic activity for ORR with a halfwave potential of 0.85 V vs. reversible hydrogen electrode(RHE), showing comparable activity as compared with the commercial Pt/C catalysts in alkaline media. Moreover, this catalyst also shows a high stability with a nearly constant onset potential and half-wave potential after 10,000 cycles. The present work is highly meaningful for developing ORR electrocatalysts toward wide applications.     

Co3+-Rich Na1.95CoP2O7 Phosphates as Efficient Bifunctional Catalysts for Oxygen Evolution and Reduction Reactions in Alkaline Solution

Implementing sustainable energy conversion and storage technologies is highly reliant on crucial oxygen electrocatalysis, such as the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). However, the pursuit of low cost, energetic efficient and robust bifunctional catalysts for OER and ORR remains a great challenge. Herein, the novel Na-ion-deficient Na_2−xCoP₂O₇ catalysts are proposed to efficiently electrocatalyze OER and ORR in alkaline solution. The engineering of Na-ion deficiency can tune the electronic structure of Co, and thus tailor the intrinsically electrocatalytic performance. Among the sodium cobalt phosphate catalysts, the Na_1.95CoP₂O₇ (NCPO5) catalyst exhibits the lowest ΔE (E_J10,OER−E_J−1,ORR) of only 0.86 V, which favorably outperforms most of the reported non-noble metal catalysts. Moreover, the Na-ion deficiency can stabilize the phase structure and morphology of NCPO5 during the OER and ORR processes. This study highlights the Na-ion deficient Na_2−xCoP₂O₇ as a promising class of low-cost, highly active and robust bifunctional catalysts for OER and ORR.     

Iron Carbide Nanoparticles Encapsulated in Mesoporous Fe‐N‐Doped Carbon Nanofibers for Efficient Electrocatalysis

Exploring low‐cost and high‐performance nonprecious metal catalysts (NPMCs) for oxygen reduction reaction (ORR) in fuel cells and metal–air batteries is crucial for the commercialization of these energy conversion and storage devices. Here we report a novel NPMC consisting of Fe₃C nanoparticles encapsulated in mesoporous Fe‐N‐doped carbon nanofibers, which is synthesized by a cost‐effective method using carbonaceous nanofibers, pyrrole, and FeCl₃ as precursors. The electrocatalyst exhibits outstanding ORR activity (onset potential of ?0.02 V and half‐wave potential of ?0.140 V) closely comparable to the state‐of‐the‐art Pt/C catalyst in alkaline media, and good ORR activity in acidic media, which is among the highest reported activities of NPMCs.     

Spectroscopic Identification of Active Sites of Oxygen-Doped Carbon for Selective Oxygen Reduction to Hydrogen Peroxide

The electrochemical synthesis of hydrogen peroxide (H₂O₂) via a two-electron (2 e⁻) oxygen reduction reaction (ORR) process provides a promising alternative to replace the energy-intensive anthraquinone process. Herein, we develop a facile template-protected strategy to synthesize a highly active quinone-rich porous carbon catalyst for H₂O₂ electrochemical production. The optimized PCC₉₀₀ material exhibits remarkable activity and selectivity, of which the onset potential reaches 0.83 V vs. reversible hydrogen electrode in 0.1 M KOH and the H₂O₂ selectivity is over 95 % in a wide potential range. Comprehensive synchrotron-based near-edge X-ray absorption fine structure (NEXAFS) spectroscopy combined with electrocatalytic characterizations reveals the positive correlation between quinone content and 2 e⁻ ORR performance. The effectiveness of chair-form quinone groups as the most efficient active sites is highlighted by the molecule-mimic strategy and theoretical analysis.