Theoretical study of PdNi and PdCu clusters embedded on graphene modified by monovacancy and nitrogen doping.

The stability and reactivity of Pd4Ni4 and Pd4Cu4 clusters embedded on graphene modified by monovacancy and nitrogen doping were investigated using auxiliary density functional theory (ADFT) calculations. The most stable structure of the Pd4Ni4 cluster is found in high spin multiplicity, whereas the lowest stable energy structure of the Pd4Cu4 cluster is a close shell system. The interaction energies between the bimetallic clusters and the defective graphene systems are significantly higher than those reported in the literature for the Pd-based clusters deposited on pristine graphene. It is observed that the composites studied present a HOMO-LUMO gap less than 1 eV, which suggests that they may present a good chemical reactivity. Therefore, from the results obtained in this work it can be inferred that the single vacancy graphene and pyridinic N-doped graphene are potentially good support materials for Pd-based clusters.

Evolution of High-Index Facets Pt Nanocrystals Induced by N-Defective Sites in the Integrated Electrode for Enhanced Methanol Oxidation.

Highly efficient and durable Pt electrocatalysts are the key to boost the performance of fuel cells. The high-index facets (HIF) Pt nanocrystals are regarded as excellent catalytic activity and stability catalysts. However, nucleation, growth and evolution of high-index facets Pt nanocrystals induced by defective sites is still a challenge. In this work, tetrahexahedron (THH) and hexactahedron (HOH) Pt nanocrystals are synthesized, which are loaded on the nitrogen-doped reduced graphene oxide (N-rGO) support of the integrated electrodes by the square wave pulse method. Experimental investigations and density functional theory (DFT) calculations are conducted to analyze the growth and evolution mechanism of HIF Pt nanocrystals on the graphene-derived carbon supports. It shows that the H adsorption on the N-rGO/CFP support can induce evolution of Pt nanocrystals. Moreover, the N-defective sites on the surface of N-rGO can lead to a slower growth of Pt nanocrystals than that on the surface of reduced graphene oxide (rGO). Pt/N-rGO/CFP (20 min) shows the highest specific activity in methanol oxidation, which is 1.5 times higher than that of commercial Pt/C. This research paves the way on the design and synthesis of HIF Pt nanocrystal using graphene-derived carbon materials as substrates in the future.

Nickel Single Atom Density-Dependent CO2 Efficient Electroreduction.

The transition metal-nitrogen-carbon (M─N─C) with MNx sites has shown great potential in CO2 electroreduction (CO2RR) for producing high value-added C1 products. However, a comprehensive and profound understanding of the intrinsic relationship between the density of metal single atoms and the CO2RR performance is still lacking. Herein, a series of Ni single-atom catalysts is deliberately designed and prepared, anchored on layered N-doped graphene-like carbon (x Ni1@NG-900, where x represents the Ni loading, 900 refers to the temperature). By modulating the precursor, the density of Ni single atoms (DNi) can be finely tuned from 0.01 to 1.19 atoms nm-2. The CO2RR results demonstrate that the CO faradaic efficiency (FECO) predominantly increases from 13.4% to 96.2% as the DNi increased from 0 to 0.068 atoms nm-2. Then the FECO showed a slow increase from 96.2% to 98.2% at -0.82 V versus reversible hydrogen electrode (RHE) when DNi increased from 0.068 to 1.19 atoms nm-2. The theoretical calculations are in good agreement with experimental results, indicating a trade-off relationship between DNi and CO2RR performance. These findings reveal the crucial role of the density of Ni single atoms in determining the CO2RR performance of M─N─C catalysts.

A multifunctional N-GO/PtCo nanocomposite bridged carbon fiber interface for the electrochemical aptasensing of CA15-3 oncomarker.

The development of integrated analytical devices is crucial for advancing next-generation point-of-care platforms. Herein, we describe a facile synthesis of a strongly catalytic and durable Nitrogen-doped graphene oxide decorated platinum cobalt (NGO-PtCo) nanocomposite that is conjugated with target-specific DNA aptamer (i-e. MUC1) and grown on carbon fiber. Benefitting from the combined features of the high electrochemical surface area of N-doped GO, high capacitance and stabilization by Co, and high kinetic performance by Pt, a robust, multifunctional, and flexible nanotransducer surface was created. The designed platform was applied for the specific detection of a blood-based oncomarker, CA15-3. The electrochemical characterization proved that nanosurface provides a highly conductive and proficient immobilization support with a strong bio-affinity towards MUC1 aptamer. The specific interaction between CA15-3 and the aptamer alters the surface properties of the aptasensor and the electroactive signal probe generated a remarkable increase in signal intensity. The sensor exhibited a wide dynamic range of 5.0 × 10-2 -200 U mL-1, a low limit of detection (LOD) of 4.1 × 10-2 U mL-1, and good reproducibility. The analysis of spiked serum samples revealed outstanding recoveries of up to 100.03 %, by the proposed aptasensor. The aptasensor design opens new revelations in the reliable detection of tumor biomarkers for timely cancer diagnosis.

Detection of Tyrosinase Activity and Inhibitor Validation Based on N-GQDs Fluorescence Sensor.

Tyrosinase inhibitors have the ability to resist melanin formation and can be used for clinical and cosmetic, so it is becoming extremely crucial to search a rapid and effective method for detecting t the activity of tyrosinase. In this study, a sensing probe based on Nitrogen-doped graphene quantum dots (N-GQDs) were prepared with carbamide and citric acid. Tyrosinase can oxidize dopamine to dopamine quinone, which can quench the fluorescence of N-GQDs based on the principle of fluorescence resonance energy transfer (FRET) process, and then the detection of tyrosinase activity can be achieved. The result demonstrated that the fluorescence intensity of N-GQDs was a linear correlation with the activity of tyrosinase. Wide detection linear ranges between 0.05 and 5 U/mL and high selectivity. The detection range of tyrosinase was 0.05 to 5 U/mL and LOD of 0.005 U/mL. According to the above, the fluorescence method established in this work could be successfully used for the trace analysis of tyrosinase and it was verified that KA is an inhibitor of tyrosinase.

The development of sensitive graphene-based surface acoustic wave sensors for NO2 detection at room temperature.

Bilayer graphene (Bl-Gr) and sulphur-doped graphene (S-Gr) have been integrated with LiTaO3 surface acustic wave (SAW) sensors to enhance the performance of NO2 detection at room temperature. The sensitivity of the Bl-Gr SAW sensors toward NO2, measured at room temperature, was 0.29º/ppm, with a limit of detection of 0.068 ppm. The S-Gr SAW sensors showed 0.19º/ppm sensitivity and a limit of detection of 0.140 ppm. The origin of these high sensitivities was attributed to the mass loading and elastic effects of the graphene-based sensing materials, with surface changes caused by the absorption of the NO2 molecules on the sensing films. Although there are no significant differences regarding the sensitivity and detection limit of the two types of sensors, the measurements in the presence of interferent gases and various humidity conditions outlined much better selectivity and sensing performances towards NO2 gas for the Bl-Gr SAW sensors.

Aminophenylboronic acid-modified nitrogen-doped graphene quantum dots and their applications in lysine sensing based on interplaying fluorescent mechanisms.

Using nitrogen-doped graphene quantum dots (N-GQDs) and 3-aminophenylboronic acid (APBA), a novel fluorescence nanosensor was developed. This nanosensor exhibits high selectivity and sensitivity for lysine detection. Its sensing mechanism involves the suppression of electron transfer from APBA to the N-GQDs unit, thereby inhibiting photoinduced electron transfer and initiating internal charge transfer. At an optimal pH of 7, the protonated α-amine and ε-amine groups of lysine interact with the amide and boronic acid moieties, respectively. This interaction results in a redshift of fluorescence, substantially enhancing the response signal. A linear response was observed within a concentration range 0.40-3.01 µM, with the detection limit being 0.005 µM. A similar linear range was also achieved for the determination of lysine in human serum. Density functional theory calculations correlating molecular orbits and geometries support UV-vis and fluorescence findings. Additionally, the nanosensor was successfully applied to detect lysine in living cells and real samples, including milk and honey. For practical application, we construct a lysine-specific sensing platform using a commercial chip (TCS34725) that collects red, blue, and green signals, thereby facilitating the convenient use of the nanosensor. Overall, this study offers new perspectives on the development and application of fluorescent nanosensors for detecting individual amino acids.

A novel electrochemical immunosensor for sensitive detection of depression marker Apo-A4 based on bipyridine-functionalized covalent organic frameworks.

A novel electrochemical immunosensor for detecting potential depression biomarker Apolipoprotein A4 (Apo-A4) was developed using a multi-signal amplification approach. Firstly, the sensor utilized a modified electrode material, NG-PEI-COF, combining bipyridine-functionalized covalent organic framework (COF) and polyethyleneimine-functionalized nitrogen-doped graphene (NG-PEI), providing high surface area and excellent electron transfer capability for the first-stage amplification in electrical signal conduction. Subsequently, gold nanoparticles (AuNPs) were further electrodeposited onto the electrode, providing good biocompatibility and abundant binding sites for immobilizing the target antigen, thus achieving the second-stage amplification in target recognition and binding. To address the lack of redox properties of the antigen, a tracer probe was formed by loading AuNPs, anti-Apo-A4, and toluidine blue (TB) successively onto COF, leading to the third-stage amplification in signal conversion. The constructed electrochemical immunosensor TB/Ab/AuNPs/COF-Apo-A4/AuNPs/NG-PEI-COF/GCE exhibited excellent detection performance against Apo-A4 with a linear range of 0.01 to 300 ng mL-1 and had a low detection limit of 2.16 pg mL-1 (S/N = 3). In addition, the biosensor had good reproducibility (RSD = 2.31%), stability, and significant anti-interference performance toward other depression biomarkers. The sensor has been successfully used for the quantitative detection of Apo-A4 in serum, providing potential applications for detecting Apo-A4 in the clinic and serving as a reference for constructing sensing methods based on COF.

Fluorescence/electrochemical dual-mode strategy for Golgi protein 73 detection based on molybdenum disulfide/ferrocene/palladium nanoparticles and nitrogen-doped graphene quantum dots.

Golgi protein 73 (GP73) is a new serum marker associated with early diagnosis and postoperative assessment of hepatocellular carcinoma (HCC). Herein, an electrochemical/fluorescence dual-signal biosensor was designed for determination of GP73 based on molybdenum disulfide/ferrocene/palladium nanoparticles (MoS2-Fc-PdNPs) and nitrogen-doped graphene quantum dots (NGQDs). GP73 aptamer (Apt) was labeled with NGQDs to form the NGQDs-Apt fluorescence probe. MoS2-Fc-PdNPs served not only as the fluorescence quencher but also as electrochemical enhancer. The sensing platform (NGQDs-Apt/MoS2-Fc-PdNPs) was formed based on the fluorescence resonance energy transfer (FRET) mechanism. In the presence of GP73, the specific binding of NGQDs-Apt to GP73 interrupted FRET, restoring the fluorescence of NGQDs-Apt at λex/em = 348/438 nm and enhancing the oxidation current of Fc in MoS2-Fc-PdNPs at 0.04 V through differential pulse voltammetry (DPV). Under the optimal conditions, the DPV current change and fluorescence recovery have a good linear relationship with GP73 concentration from 1.00 to 10.0 ng/mL. The calibration equation for the fluorescence mode was Y1 = (0.0213 ± 0.00127)X + (0.0641 ± 0.00448) and LOD was 0.812 ng/mL (S/N = 3). The calibration equation of the electrochemical mode was Y2 = (3.41 ± 0.111)X + (1.62 ± 0.731), and LOD of 0.0425 ng/mL (S/N = 3). The RSDs of fluorescence mode and electrochemical mode after serum detection were 1.62 to 5.21% and 0.180 to 6.62%, respectively. By combining the electrochemical and fluorescence assay, more comprehensive and valuable information for GP73 was provided. Such dual-mode detection platform shows excellent reproducibility, stability, and selectivity and has great application potential.

Investigation of Laser-Induced Graphene (LIG) on a Flexible Substrate and Its Functionalization by Metal Doping for Gas-Sensing Applications.

Graphene materials synthesized using direct laser writing (laser-induced graphene; LIG) make favorable sensor materials because of their large surface area, ease of fabrication, and cost-effectiveness. In particular, LIG decorated with metal nanoparticles (NPs) has been used in various sensors, including chemical sensors and electronic and electrochemical biosensors. However, the effect of metal decoration on LIG sensors remains controversial; hypotheses based on computational simulations do not always match the experimental results, and even the experimental results reported by different researchers have not been consistent. In the present study, we explored the effects of metal decorations on LIG gas sensors, with NO2 and NH3 gases as the representative oxidizing and reducing agents, respectively. To eliminate the unwanted side effects arising from metal salt residues, metal NPs were directly deposited via vacuum evaporation. Although the gas sensitivities of the sensors deteriorate upon metal decoration irrespective of the metal work function, in the case of NO2 gas, they improve upon metal decoration in the case of NH3 exposure. A careful investigation of the chemical structure and morphology of the metal NPs in the LIG sensors shows that the spontaneous oxidation of metal NPs with a low work function changes the behavior of the LIG gas sensors and that the sensors' behaviors under NO2 and NH3 gases follow different principles.

Density Functional Theory-Based Approaches to Improving Hydrogen Storage in Graphene-Based Materials.

Various technologies have been developed for the safe and efficient storage of hydrogen. Hydrogen storage in its solid form is an attractive option to overcome challenges such as storage and cost. Specifically, hydrogen storage in carbon-based structures is a good solution. To date, numerous theoretical studies have explored hydrogen storage in different carbon structures. Consequently, in this review, density functional theory (DFT) studies on hydrogen storage in graphene-based structures are examined in detail. Different modifications of graphene structures to improve their hydrogen storage properties are comprehensively reviewed. To date, various modified graphene structures, such as decorated graphene, doped graphene, graphene with vacancies, graphene with vacancies-doping, as well as decorated-doped graphene, have been explored to modify the reactivity of pristine graphene. Most of these modified graphene structures are good candidates for hydrogen storage. The DFT-based theoretical studies analyzed in this review should motivate experimental groups to experimentally validate the theoretical predictions as many modified graphene systems are shown to be good candidates for hydrogen storage.

Exploring the Potential of Nitrogen-Doped Graphene in ZnSe-TiO2 Composite Materials for Supercapacitor Electrode.

The current study explores the prospective of a nitrogen-doped graphene (NG) incorporated into ZnSe-TiO2 composites via hydrothermal method for supercapacitor electrodes. Structural, morphological, and electronic characterizations are conducted using XRD, SEM, Raman, and UV analyses. The electrochemical study is performed and galvanostatic charge-discharge (GCD) and cyclic voltammetry (CV) are evaluated for the supercapacitor electrode material. Results demonstrate improved performance in the ZnSe-NG-TiO2 composite, indicating its potential for advanced supercapacitors with enhanced efficiency, stability, and power density. Specific capacity calculations and galvanic charge-discharge experiments confirmed the promising electrochemical activity of ZnSe-NG-TiO2, which has a specific capacity of 222 C/g. The negative link among specific capacity and current density demonstrated the composite's potential for high energy density and high-power density electrochemical devices. Overall, the study shows that composite materials derived from multiple families can synergistically improve electrode characteristics for advanced energy storage applications.

High-Performing Atomic Electrocatalyst for Chlorine Evolution Reaction.

Electrocatalysts facilitating chlorine evolution reaction (ClER) play a vital role in chlor-alkali industries. Owing to a huge amount of chlorine consumed worldwide, inexpensive high-performing catalysts for Cl2 production are highly demanded. Here, a superb ClER catalyst fabricated through uniform dispersion of Pt single atoms (SAs) in C2 N2 moieties of N-doped graphene (denoted as Pt-1) is presented, which demonstrates near 100% exclusive ClER selectivity, long-term durability, extraordinary Cl2 production rate (3500 mmol h-1 gPt -1 ), and >140 000-fold increased mass activity over industrial electrodes in acidic medium. Excitingly, at the typical chlor-alkali industries' operating temperature (80 °C), Pt-1 supported on carbon paper electrode requires a near thermoneutral ultralow overpotential of 5 mV at 1 mA cm-2 current density to initiate the ClER, consistent with the predicted density functional theory (DFT) calculations. Altogether these results show the promising electrocatalyst of Pt-1 toward ClER.

Improved Photo-Excited Carriers Transportation of WS2 -O-Doped-Graphene Heterostructures for Solar Steam Generation.

Two-dimensional (2D) transition metal dichalcogenides and graphene have revealed promising applications in optoelectronic and energy storage and conversion. However, there are rare reports of modifying the light-to-heat transformation via preparing their heterostructures for solar steam generation. In this work, commercial WS2 and sucrose are utilized as precursors to produce 2D WS2 -O-doped-graphene heterostructures (WS2 -O-graphene) for solar water evaporation. The WS2 -O-graphene evaporators demonstrate excellent average water evaporation rate (2.11 kg m-2  h-1 ) and energy efficiency (82.2%), which are 1.3- and 1.2-fold higher than WS2 and O-doped graphene-based evaporators, respectively. Furthermore, for the real seawater with different pH values (pH 1 and 12) and rhodamine B pollutants, the WS2 -O-graphene evaporators show great average evaporation rates (≈2.08 and 2.09 kg m-2  h-1 , respectively) for producing freshwater with an extremely low-grade of dye residual and nearly neutral pH values. More interestingly, due to the self-storage water ability of WS2 -O-graphene evaporators, water evaporation can be implemented without the presence of bulk water. As a result, the evaporation rate reaches 3.23 kg m-2  h-1 , which is ≈1.5 times higher than the regular solar water evaporation system. This work provides a new approach for preparing 2D transition metal dichalcogenides and graphene heterostructures for efficient solar water evaporation.

Novel Mg- and Ga-doped ZnO/Li-Doped Graphene Oxide Transparent Electrode/Electron-Transporting Layer Combinations for High-Performance Thin-Film Solar Cells.

Herein, a novel combination of Mg- and Ga-co-doped ZnO (MGZO)/Li-doped graphene oxide (LGO) transparent electrode (TE)/electron-transporting layer (ETL) has been applied for the first time in Cu2 ZnSn(S,Se)4 (CZTSSe) thin-film solar cells (TFSCs). MGZO has a wide optical spectrum with high transmittance compared to that with conventional Al-doped ZnO (AZO), enabling additional photon harvesting, and has a low electrical resistance that increases electron collection rate. These excellent optoelectronic properties significantly improved the short-circuit current density and fill factor of the TFSCs. Additionally, the solution-processable alternative LGO ETL prevented plasma-induced damage to chemical bath deposited cadmium sulfide (CdS) buffer, thereby enabling the maintenance of high-quality junctions using a thin CdS buffer layer (≈30 nm). Interfacial engineering with LGO improved the Voc of the CZTSSe TFSCs from 466 to 502 mV. Furthermore, the tunable work function obtained through Li doping generated a more favorable band offset in CdS/LGO/MGZO interfaces, thereby, improving the electron collection. The MGZO/LGO TE/ETL combination achieved a power conversion efficiency of 10.67%, which is considerably higher than that of conventional AZO/intrinsic ZnO (8.33%).

Boosting Li-O2 Battery Performance via Coupling of P-N Site-Rich N, P Co-Doped Graphene-Like Carbon Nanosheets with Nano-CePO4.

Development of efficient and robust cathode catalysts is critical for the commercialization of Li-O2 batteries (LOBs). Herein, a well-designed CePO4 @N-P-CNSs cathode catalyst for LOBs via coupling P-N site-rich N, P co-doped graphene-like carbon nanosheets (N-P-CNSs) with nano-CePO4 via a novel "in situ derivation" coupling strategy by in situ transforming the P atoms of P-C sites in N-P-CNSs to CePO4 is reported. The CePO4 @N-P-CNSs exhibit superior bifunctional ORR/OER activity relative to commercial Pt/C-RuO2 with an overall overpotential of 0.64 V (vs RHE). Moreover, the LOB with CePO4 @N-P-CNSs as the cathode catalyst delivers a low charge overpotential of 0.67 V (vs Li/Li+ ), high discharge capacity of 29774 mAh g-1 at 100 mA g-1 and long cycling stability of 415 cycles, respectively. The remarkably enhanced LOB performance is attributable to the in situ derived CePO4 nanoparticles and the P-N sites in N-P-CNSs, which facilitate increased bifunctional ORR/OER activity, promote the rapid and effective decomposition of Li2 O2 and inhibit the formation of Li2 CO3 . This work may provide new inspiration for designing efficient, durable, and cost-effective cathode catalysts for LOBs.

Oxidative Cleavage of ß-O-4 Linkage in Lignin via Co Nanoparticles Embedded in 3DNG as Catalyst.

The cleavage of ß-O-4 linkage in lignin is one of the key steps for oxidative conversion of lignin to low-molecular-weight aromatics. Herein, Co nanoparticles embedded in three-dimensional network of nitrogen-doped graphene (Co/NG@3DNG-X) were prepared through an immersion-pyrolysis procedure, in which X denotes the pyrolysis temperature. The detailed characterization of Co/NG@3DNG-X shows that the Co nanoparticles are coated with a few layers of nitrogen-doped graphene (NG) sheets that are further embedded in 3DNG matrix. The catalytic activities of the Co/NG@3DNG-X for the oxidative cleavage of ß-O-4 linkage in lignin model compounds with O2 as oxidant are explored. It is demonstrated that catalytic activities of as-prepared Co/NG@3DNG-X can be tuned by varying the pyrolysis condition, and the Co/NG@3DNG-900 shows the highest catalytic activity, which is attributed to the enriched Co-Nx species, the strong surface basicity, the high specific surface and the mesoporous motif of 3DNG network. More pronouncedly, the Co/NG@3DNG-900 can also effectively catalyze the oxidative cleavage of organosolv lignin, generating certain monomeric aromatics. Additionally, the intrinsic magnetic property of Co nanoparticles makes the Co/NG@3DNG-X be easily recovered from the reaction mixture, and the as-coated thin NG layer can protect Co nanoparticle from oxidation condition, which putting together afford the Co/NG@3DNG-X with good reusability and stability.

Tailoring the work function of graphene via defects, nitrogen-doping and hydrogenation: A first principles study.

The effect of defects, nitrogen doping, and hydrogen saturation on the work function of graphene is investigated via first principle calculations. Whilst Stone-Wales defects have little effect, single and double vacancy defects increase the work function by decreasing charge density in theπ-electron system. Substitutional nitrogen doping in defect-free graphene significantly decreases the work function, because the nitrogen atoms donate electrons to theπ-electron system. In the presence of defects, these competing effects mean that higher nitrogen content is required to achieve similar reduction in work function as for crystalline graphene. Doping with pyridinic nitrogen atoms at vacancies slightly increases the work function, since pyridinic nitrogen does not contribute electrons to theπ-electron system. Meanwhile, hydrogen saturation of the pyridinic nitrogen atoms significantly reduces the work function, due to a shift from pyridinic to graphitic-type behavior. These findings clearly explain some of the experimental work functions obtained for carbon and nitrogen-doped carbon materials in the literature, and has implications in applications such as photocatalysis, photovoltaics, electrochemistry, and electron field emission.

Nitrogen-doped graphene for tetracycline removal via enhancing adsorption and non-radical persulfate activation.

Nitrogen-doped graphene (NG) was synthesized via direct thermal annealing treatment. The obtained NG showed outstanding removal ability for tetracycline (TC) ascribed to enhanced adsorption and persulfate activation. The maximum TC adsorption capacity calculated from the Langmuir model of NG was 227.3 mg/g, which was 1.66 times larger than nitrogen-free graphene. The coexistence of NG and persulfate (PS) exhibited complete degradation of TC within 120 min attributed to the successful modification of nitrogen. Further analysis demonstrated that non-radical electron transfer was the dominant degradation pathway, which was different from the widely acknowledgeable radical mechanism. An electron donor-mediator-acceptor system was introduced, in which TC, NG, and PS performed as electron donor, mediator, and acceptor, respectively. The potential intermediates in the TC degradation process were detected and toxicity assessment was also performed. In addition, more than 75.8% of total organic carbon was removed, and excellent reusability was manifested in multiple adsorption and degradation experiments.

Investigating the electrochemical advanced oxidation mechanism of N-doped graphene aerogel: Molecular dynamics simulation combined with DFT method.

Nitrogen-doped graphene as a perfectly-efficient and environmentally compatible electrocatalyst won widespread attention in electrochemical advanced oxidation processes (EAOP). However, the relationship between surface structure regulation and activity of catalysts is still lacking in systematic scientific guidance. Herein, nitrogen-doped graphene aerogel (NGA) was conveniently prepared through hydrothermal treatment, and then utilized to fabricate the gas diffusion electrode (GDE) as the cathode for tetracycline (TC) removal. High free radical yield (81.2 µM) and fast reaction rate (0.1469 min-1) were found in NGA system. The molecular dynamics simulation (MD) results showed that the interaction energy of NGA was greater than the raw graphene aerogel (GA). The adsorption activation of H2O2 and the degradation of TC occurred in the first adsorption layer of catalysts, and both processes turned more orderly after nitrogen doping. Moreover, the van der Waals interaction was stronger than the electrostatic interaction. Density function theory (DFT) revealed that the adsorption energy of H2O2 at graphitic N, pyridinic N, and pyrrolic N sites was -0.03 eV, -0.39 eV, and -0.30 eV, respectively. Pyridinic N sites were inferred as the main functional regions of in-situ activation •OH, there were more likely to occur ectopic reaction in pyrrolic N, and graphitic N were responsible for improving H2O2 production. By revealing the microstructure and activation characteristics of NGA, an experiment-simulation complementary strategy is provided in the EAOP to discover or to optimize new catalysts.