Nitrogen-doped Porous Carbon Research Articles

Controllable construction of CoP nanoparticles anchored on a nitrogen-doped porous carbon as an electrocatalyst for highly efficient oxygen reduction in Zn-air batteries

Exploring cost-efficient and highly-efficient noble metal-free catalysts for the oxygen reduction reactions (ORRs) involved in sustainable energy devices remains a great challenge. Transition-metal phosphides supported on heteroatom-doped carbons have shown potential as alternative candidates for precious metals because of their tunable electronic structures and higher catalytic performance. Phosphating was used to construct CoP nanoparticles (NPs) anchored on a nitrogen-doped porous carbon framework (CoP@NC) from Co NPs loaded on NC, using PH3 gas released from NaH2PO2 during heat treatment. The dodecahedral structure of Co NPs was retained in their transformation to CoP NPs. The CoP@NC electrocatalyst shows a remarkable ORR activity with a half-wave potential up to 0.92 V under alkaline conditions, which is attributed to the combined coupling between the well dispersed CoP nanoparticles on the nitrogen-doped carbon and the efficient mass transport in the porous structure. Zinc-air batteries assembled with the CoP@NC electrocatalyst as a cathode have a high open-circuit voltage of 1.51 V and power density of 210.1 mW cm−2. This work provides a novel strategy to develop low-cost catalysts with an excellent ORR performance to promote their practical use in metal-air batteries

Cobalt–nickel bimetallic hybridized nitrogen-doped hierarchical porous carbon as efficient oxygen reduction electrocatalyst

Cobalt–nickel bimetallic hybridized nitrogen-doped hierarchical porous carbon as efficient oxygen reduction electrocatalyst

Mild modification of sponge-like carbon: Ammonia post-treatment for enhanced CO2 adsorption and suitability for supercapacitors

During the synthesis of carbon-based CO2 adsorbents and supercapacitors, the introduction of nitrogen atoms into the carbon matrix has been identified as a means to enhance their performance. Nevertheless, the intricate effects of nitrogen doping on material properties pose a significant challenge in developing efficient methodologies. In this investigation, porous carbons resembling sponges were fabricated utilizing macadamia nut shells as a precursor and a dual salt comprising K2C2O4-KCl as an activating agent. Subsequent modification of the materials through ammonia post-treatment facilitated the production of nitrogen-doped porous carbon. The alterations in surface characteristics and pore morphology after ammonia treatment were meticulously examined to unravel the underlying mechanism of this modification process. The samples under scrutiny showcased remarkable CO2 adsorption capacities, peaking at 6.97 mmol/g at 0 °C and 4.65 mmol/g at 25 °C. Employing mathematical models to probe the influence of pore structure and surface properties on CO2 adsorption efficacy proved to be fruitful. A linear correlation was established to depict CO2 adsorption behavior, underscoring the joint impact of ultramicropore volume and nitrogen content on the adsorption process. Notably, the material exhibited a specific capacitance of 290.4F/g at a current density of 0.5 A/g within a three-electrode configuration, demonstrating commendable rate capability and cyclic stability. The pivotal findings from this inquiry emphasize that ammonia post-treatment represents a gentle modification strategy exerting minimal influence on the pore architecture, thereby efficaciously enhancing both CO2 adsorption and electrochemical performance.

In Situ Self-Assembly of Nitrogen-Doped 3D Flower-like Hierarchical Porous Carbon and Its Application for Supercapacitors.

The hierarchical porous carbon-based materials derived from biomass are beneficial for the enhancement of electrochemical performances in supercapacitors. Herein, we report the fabrication of nitrogen-doped 3D flower-like hierarchical porous carbon (NPC) assembled by nanosheets using a mixture of urea, ZnCl2, and starch via a low-temperature hydrothermal reaction and high-temperature carbonization process. As a consequence, the optimized mass ratio for the mixture is 2:2:2 and the temperature is 700 °C. The NPC structures are capable of electron transport and ion diffusion owing to their high specific surface area (1498.4 m2 g-1) and rich heteroatoms. Thereby, the resultant NPC electrodes display excellent capacitive performance, with a high specific capacitance of 249.7 F g-1 at 1.0 A g-1 and good cycling stability. Remarkably, this implies a superior energy density of 42.98 Wh kg-1 with a power density of 7500 W kg-1 in organic electrolyte for the symmetrical supercapacitor. This result verifies the good performance of as-synthesized carbon materials in capacitive energy storage applications, which is inseparable from the hierarchical porous features of the materials.

Sustainable electro-Fenton simultaneous reduction of Cr (VI) and degradation of organic pollutants via dual-site porous carbon cathode driving uncoordinated molybdenum sites conversion

Simultaneous removal of heavy metals and organic contaminants remains a substantial challenge in the electro-Fenton (EF) system. Herein, we propose a facile and sustainable “iron-free” EF system capable of simultaneously removing hexavalent chromium (Cr (VI)) and para-chlorophenol (4-CP). The system comprises a nitrogen-doped and carbon-deficient porous carbon (dual-site NPC-D) cathode coupled with a MoS2 nanoarray promoter (MoS2 NA). The NPC-D/MoS2 NA system exhibits exceptional synergistic electrocatalytic activity, with removal rates for Cr (VI) and 4-CP that are 20.3 and 4.4 times faster, respectively, compared to the NPC-D system. Mechanistic studies show that the dual-site structure of NPC-D cathode favors the two-electron oxygen reduction pathway with a selectivity of 81 %. Furthermore, an electric field-driven uncoordinated Mo valence state conversion of MoS2 NA enchances the generation of dynamic singlet oxygen and hydroxyl radicals. Notably, this system shows outstanding recyclability, resilience in real wastewater, and sustainability during a 3 L scale-up operation, while effectively mitigating toxicity. Overall, this study presents an effective approach for treating multiple-component wastewater and highlights the importance of structure-activity correlation in synergistic electrocatalysis.

Study on the adsorption of Ce(III) on phosphonic acid functionalized ZIF-67@SiO2 magnetic porous carbon materials

A ZIF-67 composite SiO2 material (ZIF-67@SiO2) was synthesized using ethyl orthosilicate (TEOS) as a silicon source, followed by one-step carbonization to produce magnetic porous nitrogen-doped carbon material (MNPC@SiO2) using ZIF-67@SiO2 as a carbon precursor. Subsequently, the composite P-MNPC@SiO2 was obtained through functionalization with diethylphosphonoethyltriethoxysilane (DPTS), and its characteristics were analyzed. The adsorption properties of Ce(III) on MNPC@SiO2 and P-MNPC@SiO2 composites were investigated under various conditions through adsorption experiments. Kinetic, isothermal, and thermodynamic models were employed to analyze the adsorption mechanism of P-MNPC@SiO2 on Ce3+ and assess adsorbent stability and regeneration performance. The result shows that P-MNPC@SiO2 exhibited excellent adsorption capacity for Ce3+ and possessed magnetic properties conducive to recycling. Under optimized conditions, P-MNPC@SiO2 reached Ce(III) adsorption saturation within 20 min, with a maximum adsorption capacity of 342.52 mg/g, which was 1.9 times higher than that of the MNPC@SiO2 material. Data fitting shows that surface adsorption controls the rate-limiting step, and Ce(III) forms a monolayer adsorption on the surface of the adsorbent material. Furthermore, P-MNPC@SiO2 exhibits strong stability and regeneration properties.

Nitrogen-doped porous carbon with regulated pore structure and surface wettability as flow electrodes for efficient capacitive deionization

Nitrogen-doped porous carbon with controlled pore structure and wettability was synthesized using spent mushroom substrate (SMS) via physical activation process. The nitrogen-rich feature of precursor enables the carbon material to possess both electrical conductivity and surface wettability, creating an effective conducting network in flow electrodes. These materials have been proven to be highly efficient for deionization due to their ability of maintaining surface wettability and electrical conductivity. Our results show that the SMS-1.5 sample has a high adsorption capacity of 8.38 mg/g, which is 1.8 times greater than the commercial YP-50. The corresponding charge efficiency was up to 90.66 % after being exposed to 1.6 g/L NaCl feed solution for 120 min in flow electrode capacitive deionization device. This study highlights the significance of the inherent nitrogen element in biomass for the synergistic promotion of electrical conductivity and surface wettability, providing a strategy for designing porous carbons with excellent desalination performance.

Cellulose nanofiber enabled high-mass loading N-doped porous carbon electrode for zinc-ion supercapacitors

Zinc-ion hybrid supercapacitors (ZHSCs) are among the most promising electrochemical energy storage technologies because of their high energy density, environmental sustainability, low price, and inherent security. High-load, high-capacity cathodes are critical for the practical application of ZHSCs. However, it is challenging to achieve optimal performance of high-loading electrodes due to slow reaction kinetics, retarded ion transport, and structural instability. Herein, a salt-template technique was used to fabricate nitrogen-doped porous carbon (NPC) with large surface area, abundant mesopores, and electroactive nitrogen dopants. When combined with a fibrous network scaffold of carbon nanotubes and cellulose nanofibers (CNT/CNF), the optimized NPC delivered an outstanding specific capacitance of 133.4 mAh g−1 and a remarkable capacity retention of 95.4% after 10,000 cycles. More impressively, we achieved a cathode with high mass-loading of 10 mg cm−2 without significantly sacrificing the electrochemical performance (area capacity of 2.05 mAh cm−2 and good cycling stability with capacity retention of 86.2% after 3000 cycles). The excellent performance can be attributed to the continuous electron/ion conduction pathways of CNT/CNF scaffold and redox-active surface generated by the favorable heteroatom-doped porous carbon. In sum, this work offers a platform for making high mass-loading carbon electrodes for practical ZHSCs.

Enhanced activity and durability of Pt nanoclusters catalyst by using nitrogen-doped carbon layer coated carbon nanotubes as anchors and nanowires for ORR

Platinum-based catalysts remain the top choice for oxygen reduction reaction (ORR) in fuel cells. However, their activity and durability in the acidic medium are still under improvement. In this work, the Pt nanoclusters anchored the nitrogen-doped carbon nanotubes (Pt-NCNTs) have been synthesized by using a series process of pyrrole coating on the CNTs and subsequent pyrolysis to the chemical immersion reduction of Pt ions. The inner CNTs of Pt-NCNTs function as the nanowires offering a high-speed pathway for electron transport, and the Pt nanoclusters increases the active sites. The theoretical calculation demonstrates that the local structural defects and the uneven charge distribution induced by nitrogen-containing functional groups and porous structure are favorable to capture Pt ions for the nucleation of Pt nanoclusters. Compared with the commercial 40 wt% Pt/C (0.94 and 0.80 V), the Pt-NCNTs-1000 with Pt loading amount of 33.0 wt% owns the more positive onset potential and half-wave potential of 0.97 and 0.81 V in the sulfuric acid medium. Meanwhile, the strong attachment of Pt nanoclusters on the nitrogen-doped porous carbon layer results in a stable interface to effectively prevent the metallic species from migration and agglomeration during the electrode reactions. Therefore, the ORR current of Pt-NCNTs-1000 retained 84.3% of the initial value after 50000 s operation superior to the commercial Pt/C (64.6%).

Sulfur dioxide-resistant platinum-based intermetallic nanocatalysts encaged by porous nitrogen-doped carbon for oxygen reduction reaction

SO2, one of the considerable air pollutants, exhibits a stronger binding affinity with Pt when compared to O2, thereby inducing irreversible degradation of the Oxygen Reduction Reaction (ORR) catalyzed by Pt-based catalysts. Despite this detrimental phenomenon, scarce investigations have delved into the realm of contaminant-tolerant catalysts, and so far, no effective SO2-tolerant catalysts have been proposed. To meet this challenge, we designed and synthesized a core–shell structure catalyst equipped with a dual protection mechanism. This was achieved through the in-situ polymerization of aniline monomers, concomitantly reducing Pt2+. The resulting shell effectively hinders the transmission of SO2 to the active sites of Pt, while permitting the unimpeded transmission of O2. Simultaneously, the intermetallic core inhibits the adsorption of SO2. Therefore, this catalyst exhibits exemplary ORR activity coupled with exceptional resistance to SO2 resistance. In particular, the PtFe@FeNC/C-10 catalyst, optimized in terms of the quantity of added aniline, demonstrates a mass activity 1.84 times greater and a specific activity 4.03 times higher than that of commercial Pt/C catalysts. Following exposure to SO2-induced poisoning, the E1/2 value of the PtFe@FeNC/C-10 catalyst undergoes a decrease of only 51.7 mV, lower than that observed for the commercial Pt/C catalyst (92.0 mV). Moreover, the results of an accelerated durability test affirm the superior stability of PtFe@FeNC/C-10 in comparison to commercial Pt/C. This stability advantage is attributed to the protective carbon shell, which effectively prevents the detachment and agglomeration of Pt nanoparticles.

Nitrogen-doped magnetic porous carbon nanospheres derived from dual templates-induced mesoporous polydopamine coated Fe3O4 for efficient extraction and sensitive determination of volatile nitrosamines by gas chromatography-mass spectroscopy

N-nitrosamines (NAs) are highly carcinogenic compounds commonly found in food, beverages, and consumer products. Due to their wide polarity range, it is challenging to find a suitable carbon adsorbent that can simultaneously adsorb and enrich both polar and nonpolar NAs with good recovery. In this study, nitrogen-doped magnetic mesoporous carbon nanospheres (M-MCN) were prepared and employed as an adsorbent for magnetic solid-phase extraction (MSPE) to extract and concentrate four NAs. The introduction of nitrogen functional groups enhanced the hydrophilicity of the carbon material, allowing M-MCN to achieve a balance between hydrophilicity and hydrophobicity, resulting in good recovery for both polar and nonpolar NAs. A method combining MSPE with gas chromatography-mass spectrometry (GC-MS) was developed for the determination of NAs in processed meat and alcoholic beverages. The method exhibited a good linear range (1–100 ng g−1, r2 > 0.9967) and trace-level detection (0.53–6.6 ng g−1). The recovery rates for the four NAs ranged between 85.7 and 110.7 %, with intra-day precision expressed as relative standard deviation (RSD) between 4.1 and 10.7 %, and inter-day precision between 4.8 and 12.9 %. The results demonstrated not only good accuracy and precision but also provided a new adsorbent for the enrichment of trace-level NAs in processed meat and alcoholic beverage samples.

Synergistic Engineering of CoO/MnO Heterostructures Integrated with Nitrogen-Doped Carbon Nanofibers for Lithium-Ion Batteries.

The integration of heterostructures within electrode materials is pivotal for enhancing electron and Li-ion diffusion kinetics. In this study, we synthesized CoO/MnO heterostructures to enhance the electrochemical performance of MnO using a straightforward electrostatic spinning technique followed by a meticulously controlled carbonization process, which results in embedding heterostructured CoO/MnO nanoparticles within porous nitrogen-doped carbon nanofibers (CoO/MnO/NC). As confirmed by density functional theory calculations and experimental results, CoO/MnO heterostructures play a significant role in promoting Li+ ion and charge transfer, improving electronic conductivity, and reducing the adsorption energy. The accelerated electron and Li-ion diffusion kinetics, coupled with the porous nitrogen-doped carbon nanofiber structure, contribute to the exceptional electrochemical performance of the CoO/MnO/NC electrode. Specifically, the as-prepared CoO/MnO/NC exhibits a high reversible specific capacity of 936 mA h g-1 at 0.1 A g-1 after 200 cycles and an excellent high-rate capacity of 560 mA h g-1 at 5 A g-1, positioning it as a competitive anode material for lithium-ion batteries. This study underscores the critical role of electronic and Li-ion regulation facilitated by heterostructures, offering a promising pathway for designing transition metal oxide-based anode materials with high performances for lithium-ion batteries.

Nitrogen-Doped Cellulose-Based Porous Carbon for Electrocatalytic CO2 Reduction to CO

Nitrogen-Doped Cellulose-Based Porous Carbon for Electrocatalytic CO2 Reduction to CO

3D-interconnected N-doped porous carbon with hierarchical pore structure as a high-efficiency catalyst for H2S oxidation at room temperature

Nitrogen-doped porous carbons (NPCs) have been regarded as an efficient metal-free catalyst for H2S oxidation. However, critical factors affecting their desulfurization ability are still unclear, making it difficult to accurately adjust their desulfurization performance to meet industrial requirements. Herein, a novel 3D-interconnected NPC with hierarchical pore structure was synthesized by one-step “leavening” strategy using rice husk and (NH4)2C2O4 as a carbon source and foaming agent, respectively, for H2S oxidation at room temperature. Pyrolysis temperature is the major factor for physicochemical properties of NPCs, and breakthrough sulfur capacity of the optimal NPC reaches up to 1036.68 mg/g, which can remain stable during three desulfurization-regeneration cycles. Comparative experiment shows that H2S capacity of NPC is 1.8 and 4.0 times those of PC and NC, respectively, revealing the excellent desulfurization performance of NPC. The structure-effect relationships between H2S and NPC reveal that both textural and chemical properties of NPC, especially specific surface area, structural defect, and pyrrolic N, play dominant roles in H2S removal. It is very necessary to balance the relationship between textural performances and pyrrolic N to synthesize optimal NPC catalyst. This work provides a valuable reference for rational design of high-efficiency carbon-based catalysts for persistent desulfurization at room temperature.

Synergistic Al-Al Dual-Atomic Site for Efficient Artificial Nitrogen Fixation.

Synthesis of ammonia by electrochemical nitrogen reduction reaction (NRR) is a promising alternative to the Haber-Bosch process. However, it is commonly obstructed by the high activation energy. Here, we report the design and synthesis of an Al-Al bonded dual atomic catalyst stabilized within an amorphous nitrogen-doped porous carbon matrix (Al2NC) with high NRR performance. The dual atomic Al2-sites act synergistically to catalyze the complex multiple steps of NRR through adsorption and activation, enhancing the proton-coupled electron transfer. This Al2NC catalyst exhibits a high Faradaic efficiency of 16.56±0.3 % with a yield rate of 29.22±1.2 μg h-1 mgcat -1. The dual atomic Al2NC catalyst shows long-term repeatable, and stable NRR performance. This work presents an insight into the identification of synergistic dual atomic catalytic site and mechanistic pathway for the electrochemical conversion of N2 to NH3.

A hierarchical porous structure and nitrogen-doping jointly enhance the lithium-ion storage capacity of biomass-derived carbon materials

Biomass-derived carbon materials are considered potential lithium-ion anode materials because they are sustainable, renewable, economical, and environmentally friendly and have tunable microstructures. However, biomass-derived carbon materials have low specific capacity and show capacity degradation during long-term electrochemical cycling, which prevents their application in high-performance lithium-ion batteries. Hence, in this paper, nitrogen-doped hierarchical porous carbon (NHPC) is synthesized from a biomass waste material, corncob, through one-step activation and carbonization procedures. N-doping in the NHPC modifies the electron distribution on the surface of carbon, resulting in the generation of additional lithium-ion storage sites and enhancing electrode wettability to increase the conductivity. Additionally, the doping procedure results in a hierarchical porous structure with an increased specific surface area and pore volume, which facilitates ion transport and provides remarkable cycling stability. The electrochemical performance of NHPC is improved by the jointly beneficial combination of N-doping and the hierarchical porous structure. The optimized NHPC electrode provides a reversible specific capacity of 700 mAh g−1 after 100 cycles at 100 mA g−1. This study provides a simple and efficient method for improving the electrochemical properties of biomass-derived carbon materials through elemental doping and modulation of microscopic morphology and structure.

Nitrogen-doped porous carbon derived from cross-cutting bamboo for high-performance supercapacitors by one-pot ball milling method

In this work, Nitrogen-doped cross-cut KOH-activated porous carbon (NCKC) was obtained through a simple and effective fabrication process. Cross-cut bamboo, KOH, and urea are mixed through a one-pot ball milling strategy. The obtained sample (NCKC) has a high specific capacitance in the three-electrode test (367 F·g−1 at 0.2 A· g−1), and maintains a satisfactory specific capacitance of 183 F·g−1 at a high current of 50 A·g−1. Moreover, an aqueous supercapacitor based on NCKC with 1 M Na2SO4 as the electrolyte can provide an outstanding specific energy of 31.1 W h kg−1 with a specific power of 200 W·kg−1, without any noticeable reduction in capacity even after 40,000 cycles. This is attributed to the fact that NCKC has an abundant hierarchical pore structure. The cross-cutting process can shorten natural pores origin from bamboo native structures, and facilitate hydrophilicity in the resulting porous carbon. The results reveal that the synergistic effect of cross-cutting process, ball milling, and N-doping in carbon enhanced the electrochemical performance of carbon remarkably. The results show such one-pot ball milling method simplifies the preparation process and is of great interest for the innovation and application of high-performance electrode materials.

FeNi alloy embedded in three-dimensional nitrogen-doped porous carbon as bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries

Iron‑nickel (FeNi) alloy is one of the efficient bifunctional oxygen electrocatalysts for zinc-air batteries (ZABs). However, FeNi alloy nanoparticles prepared by traditional synthesis strategies are easy to agglomerate and have non-uniform sizes, which is not conducive to the improvement of catalytic activity and stability. Here, we have successfully encapsulated two different kinds of nitrogen-rich metal phthalocyanines (MPcs) in situ doping in zeolitic imidazolate framework (ZIF-8) homogeneously by the “double solvents” method. The ligand nitrogen and macrocyclic structure of MPcs encapsulated in ZIF-8 not only helps metal dispersion and enhances the metal-ligand‑nitrogen (M-Nx) structure, but also enhances the graphitisation of three-dimensional (3D) porous carbon after pyrolysis. Thus, a FeNi alloy uniformly embedded in 3D nitrogen-doped porous carbon materials (FeNi@NC) was constructed in the subsequent pyrolysis process and used as an efficient bifunctional oxygen reduction/evolution (ORR/OER) electrocatalyst for rechargeable ZABs. Impressively, the FeNi@NC catalyst carries high half-wave potential (0.850 V) in ORR and the low overpotential (291 mV) in OER, significantly better than Pt/C (0.830 V) and RuO2 (307 mV), respectively. In addition, the rechargeable ZAB assembled with FeNi@NC air cathode has a specific capacity of 649 mW cm−2 and shows no significant degradation after 240 h of charging and discharging cycles. This study provides a new design idea for the manufacture of carbon-supported non-noble metal alloy catalysts with bifunctional oxygen catalytic activity, and verifies the feasibility of regulating the composition of non-noble metals to construct a rechargeable ZABs with excellent performance.

Iron Active Center Coordination Reconstruction in Iron Carbide Modified on Porous Carbon for Superior Overall Water Splitting.

In this work, a novel liquid nitrogen quenching strategy is engineered to fulfill iron active center coordination reconstruction within iron carbide (Fe3C) modified on biomass-derived nitrogen-doped porous carbon (NC) for initiating rapid hydrogen and oxygen evolution, where the chrysanthemum tea (elm seeds, corn leaves, and shaddock peel, etc.) is treated as biomass carbon source within Fe3C and NC. Moreover, the original thermodynamic stability is changed through the corresponding force generated by liquid nitrogen quenching and the phase transformation is induced with rich carbon vacancies with the increasing instantaneous temperature drop amplitude. Noteworthy, the optimizing intermediate absorption/desorption is achieved by new phases, Fe coordination, and carbon vacancies. The Fe3C/NC-550 (550 refers to quenching temperature) demonstrates outstanding overpotential for hydrogen evolution reaction (26.3mV at -10 mAcm-2) and oxygen evolution reaction (281.4 mV at 10mAcm-2), favorable overall water splitting activity (1.57 V at 10 mAcm-2). Density functional theory (DFT) calculations further confirm that liquid nitrogen quenching treatment can enhance the intrinsic electrocatalytic activity efficiently by optimizing the adsorption free energy of reaction intermediates. Overall, the above results authenticate that liquid nitrogen quenching strategy open up new possibilities for obtaining highly active electrocatalysts for the new generation of green energy conversion systems.

Nitrogen-Doped Porous Carbon Derived from Covalent Triazine Framework for Catalytic Oxidation of Benzyl Alcohol.

The catalytic oxidation of alcohols is an important transformation in the chemical industry. Carbon materials with a large surface area and N doping show great promise as metal-free catalysts for the reaction. In this study, a rich N-containing covalent triazine framework polymerized by cyanuric chloride and p-phenylenediamine was used to synthesize N-doped porous carbon with the assistance of a pore-forming agent-NaCl. First, the mass ratio of the polymer/NaCl was optimized to 1:9. Then, the influence of the pyrolysis temperatures (700-1000 °C) on the materials was studied in detail. It was found that the carbon materials were gradually exfoliated by molten salt at high temperatures. XRD and Raman characterizations showed them with a certain graphitization. The optimal doped carbon CNN-1-9-900 achieved the highest surface area of 199.03 m2g-1 with the largest pore volume of 0.29 cm3g-1. Furthermore, it had a high N content of 9.9 at% with the highest relative proportion of pyridinic/graphitic N. Due to the synergistic effect between the surface area and pyridinic/graphitic N, CNN-1-9-900 showed the best performance for benzyl alcohol oxidation with TBHP at moderate conditions, and the process also worked for its derivatives.