N-doped Carbon Nanosheets Research Articles

Unique Oxygen-Bridged Nickel Atomic Pairs Efficiently Boost Electrochemical Reduction of Carbon Dioxide.

Benefiting from the synergism between adjacent bimetallic atoms, in comparison with single atom catalysts, the dual atom catalysts have displayed great potential in electrocatalytic CO2 reduction reaction (CO2RR). However, the further modulation of the electronic structure of dual atom sites to enhance CO2RR performance still remains a challenge. Herein, an atomically dispersed oxygen-bridged Ni2N6O/NC catalyst with unique Ni-O-Ni sites is successfully synthesized through the microwave pyrolysis of the supported mixture containing the dinuclear nickel phthalocyanine and glucose on N-doped carbon nanosheets. Experiments and density functional theory calculation reveal that the Ni-O-Ni sites can adsorb H+ from the KHCO3 electrolyte to in situ-form the unique Ni-OH-Ni sites without Ni─Ni bonding interaction, which effectively lowers the energy barrier towards the formation of *COOH from CO2. As a result, the Ni2N6OH/NC catalyst exhibits a 99.4% of CO Faradaic efficiency with a 32.4 mA·cm-2 of CO partial current density at -0.7V versus RHE in H-cell, much superior to the Ni2N6/NC with a Ni-Ni bonding interaction prepared by a similar procedure to that for Ni2N6O/NC but replacing microwave pyrolysis by a traditional heating process.

NiCoP nanoparticles distributed on N-doped carbon-nanosheets loading on nickel phosphide as self-supporting electrode for efficient overall water splitting

The investigation of a bifunctional self-supporting catalytic electrode holds significant practical importance for the application of overall water splitting. In this paper, a precursor with a large specific surface is constructed by growing ZIF-67 nanosheets on nickel foam. Subsequently, Ni–Co bimetallic phosphide particles (NiCoP) are obtained through phosphating, which distributed in N-doped carbon material and loaded on nickel phosphide (NiCoP@NC-Ni3P/NF), facilitating the overall water splitting. Due to its large specific surface area, the double electron regulation of Ni and Co, as well as the synergistic interaction between NiCoP and Ni3P, NiCoP@NC-Ni3P/NF exhibits excellent hydrogen/oxygen evolution properties, only requiring 125.6/288.4 mV to achieve 20 mA cm−2. Its performance of overall water splitting only requires an applied voltage of 1.54 V to reach 10 mA cm−2. Moreover, the NiCoP particles embedded in the nitrogen-doped carbon can effectively reduce electrolyte corrosion, ensuring exceptional catalyst stability.

Decrypting Synergy of Alloy & Metal Nanoparticles Within Nitrogen-Doped Carbon Nanosheets for Zn-Air Batteries with Ultralong Cycling Stability.

The exploration of efficient, robust, and low-cost bifunctional electrocatalysts to drive the commercial application of Zn-air batteries (ZABs) is of great significance but still remains a challenge. Herein, a 1D coordination polymer (1D-CP) derived FeNi alloy & Co nanoparticles (NPs) co-implanted N-doped carbon nanosheets (FNC/NCS) is judiciously crafted and employed as a high-performance electrocatalyst for ultralong lifetime ZABs. The key to this strategy is the leveraging of metal-coordinated melamine to direct the pyrolysis of 1D-CP, enabling the in situ formation of well-dispersed FeNi alloy and Co NPs within the carbon matrix. The resulting FNC/NCS exhibits prominent oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity with a small overall oxygen potential difference (ΔE = 0.68V). Density functional theory (DFT) simulation demonstrates that the synergistic effect between FeNi alloy and Co NPs can reduce energy barriers, promote electron transfer, and optimize the formation of crucial intermediates, thereby largely boost ORR/OER activity of FNC/NCS. The FNC/NCS-assembled ZABs possess high specific capacity, large power density, and ultralong cycling life in both aqueous (> 3300h) and solid-state (150h) electrolytes. This work provides a viable strategy for 1D-CP-derived bifunctional electrocatalysts and dissects the synergistic effect between different metal species, affording significant guidance for the development of renewable energy materials.

Structural Regulation of a Multi-Component Co2P2O7-MoN/NC Electrocatalyst for Efficient Oxygen Evolution Reaction.

Realizing efficient and durable non-precious metal-based electrocatalysts for oxygen evolution reaction (OER) still remains a great challenge. Here, a multi-component composite of Co2P2O7-MoN/NC containing pyrophosphate, nitride, and nitrogen-doped carbon is successfully prepared via a facile two-step synthesis method. Combining the structural regulation between the active metal- and non-metal-based species, Co2P2O7-MoN/NC demonstrates superior activity and durability for OER, requiring an overpotential of 278 mV at a current density of 10 mA cm-2, a Tafel slope of 83.3 mV dec-1, and long-term stability over 100 h in an alkaline solution. Post-characterizations reveal that synergistic effect among stable Co2P2O7, partially dissolved MoN, N-doped carbon, and new-formed CoOOH nanosheets enable structural reconstruction, fast charge transfer, and formation of oxygen-containing intermediates, promoting the OER performance significantly. This work provides a promising pathway to tune multi-components to fabricate efficient transition-metal-based electrocatalysts in energy conversion applications.

Co-MOF-derived N-doped carbon nanosheet arrays on biomass carbon fiber membrane for highly sensitive detection of luteolin

Rapid and accurate determination of luteolin (LU) content is important for drug dosage control, treatment and prevention of disease. Traditional chromatographic and spectroscopic methods are gradually replaced by more sensitive and rapid electrochemical detection. 3D carbonized eggshell fiber membrane (3D CEFM) with good electrical conductivity and mechanical stability is prepared at high temperatures. To enhance the sensing performance of LU, nitrogen-doped carbon nanosheet arrays/3D CEFM (Co-NC NSAs/3D CEFM) derived from ZIF-67 nanosheet arrays (ZIF-67 NSAs) are prepared on the surface of 3D CEFM. Due to the synergistic effect, the Co-NC NSAs (thickness ∼ 1 μm, height ∼ 3 μm) provides a shorter electron transport path, while the 3D CEFM (pore size ∼5 μm) offers good electrical conductivity and a large solution contact area. Co-NC NSAs/3D CEFM electrode has a sensitivity of 1.31 μA·μM−1·cm−2 in the 0–60 μM LU and a limit of detection (LOD) of 0.04 μM (S/N = 3). Meanwhile, the electrode demonstrated recoveries of 98.0 % to 103.5 % in real samples, with a relative standard deviation (RSD) of 1.2 to 2.3 %. These results indicate that the electrode has significant potential for practical applications.

Rh, Co, and N-doped titanium mesh-based carbon nanosheet arrays for enhanced nitrite reduction reaction and ammonia generation

The electrocatalytic transformation of nitrite pollutants into valuable ammonia is crucial for the nitrogen cycle. However, the complex multi-reaction process necessitates the development of highly efficient and selective electrocatalysts. This study focuses on the creation of Rh-doped Co@NC anchored on a titanium mesh as an electrocatalyst to enhance the electrocatalytic nitrite reduction reaction (eNO2RR) for NH3 synthesis. By doping a trace amount of Rh within zeolitic imidazolate framework-67 nanosheets and subsequently pyrolyzing the material, uniformly distributed Rh and Co nanoparticles are anchored onto N-functionalized porous carbon nanosheet arrays. Consequently, the three-dimensional electrode enhances mass and electron transfer while providing abundant surface-exposed active sites for NH3 generation through eNO2RR. The Rh0.6 wt%–Co@NC/TM electrocatalyst, with a minimal Rh loading of 0.6 wt%, exhibits the highest Faradaic efficiency of 98.8 ± 0.7 % at −0.3 V, along with an NH3 yield of 1777.1 ± 7.0 μmol h−1 cm−2 at −0.7 V. Additionally, the electrocatalyst demonstrates exceptional durability over 20 consecutive cycles and remarkable environmental adaptability. Extensive experimental studies reveal that the superior performance of Rh0.6 wt%–Co@NC/TM arises from the synergistic catalysis between Co and Rh, which enhances NO2– adsorption and the production of active hydrogen for eNO2RR to NH3 synthesis. This research highlights that Rh incorporation facilitates the kinetics of eNO2RR and offers valuable insights for the development of efficient electrocatalysts towards NH3 synthesis.

Ultra-stable electrocatalysts for overall urea degradation by NiFeCoZn–S modified N-doped carbon

Urea degradation is a viable method to produce hydrogen in a sustainable way, while having an important place in environmental protection and energy security. In this work, ultrathin N-doped carbon (NC) nanosheets, modified by ultrafine multiple transition metal sulfide (NiFeCoZn–S) nanoparticles, are synthesized to serve as electrocatalysts for overall urea degradation. This unique structure allows NiFeCoZn–S/NC to have a relatively large ECSA and active sites, stemming from the small dimensions of the NiFeCoZn–S particles and the hierarchical nanoarchitecture of the NC. Thus, NiFeCoZn–S/NC has a significant urea oxidation reaction (UOR) activity of 1.31 V at 10 mA cm−2 in an electrolyte consisting of 1.0 M KOH and 0.33 M urea. Furthermore, when the catalyst was used in an electrolytic cell for urea degradation, a potential of 1.49 V was achieved up to 10 mA cm−2. Additionally, the catalyst exhibits only a 6.1 % performance decay after 660 h of operation at 10 mA cm−2. Its exceptional stability outshines that of existing urea catalysts, rendering it an attractive prospect for future applications.

Insight into the mechanism of 5-hydroxymethylfurfural electroreduction to 2,5-bis(hydroxymethyl)furan over Cu anchored N-doped carbon nanosheets

Insight into the mechanism of 5-hydroxymethylfurfural electroreduction to 2,5-bis(hydroxymethyl)furan over Cu anchored N-doped carbon nanosheets

Ultrathin Two-Dimensional Ordered Porous Carbon Host with Atomically Dispersed Electrocatalytic Sites toward High Volumetric Energy Lithium-Sulfur Battery

Despite multimodal approaches to increase the gravimetric capacity of lithium-sulfur (Li-S) batteries over the years, strategies on achieving high volumetric capacity (Qv) at close to practical cell operating conditions with high areal sulfur loading and low electrolyte-to-sulfur (E/S) ratio are still lacking. Here, we report that a synergistic effect of a carbonaceous framework with precisely-controlled porous structure/dimension and highly-active, surface-mediated electrocatalysis by a ruthenium (Ru) single-atom electrocatalyst (SAC) composed of N2RuCl2 achieves high Qv in Li-S batteries. Two-dimensional (2D) and hierarchically ordered porous structures of polymer interfacial self-assembly derived N-doped carbon nanosheets (NCNS) realize a highly-packed sulfur cathode with outstanding Li+ ion diffusivity and electrode stability, which have been considered as main impediments to achieving high Qv in a dense sulfur cathode. Moreover, homogeneous incorporation of N2RuCl2 SAC which has novel Ru coordination environment with two N and Cl atoms on the surface of NCNS remarkably accelerated the reaction kinetics of Li-S electrochemistry and achieved high Qv even at high sulfur loading (5.0 mg cm−2), extremely low E/S ratio (4.5 μL mg−1), and low electrode porosity (50 %).

Constructing ZnSe/CoSe2/N-doped carbon composite with multiple heterointerfaces using a solvent-assisted strategy to enhance lithium storage

Interface engineering, as an effective strategy for preparing high power density and long-life battery anodes, can promote the electrochemical performance of materials. Herein, metal organic frameworks (MOFs) derived N-doped carbon nanosheets loaded nanoscale ZnSe/CoSe2 particle composite with multiple heterointerfaces is fabricated by solvent assisted strategy. Wherein the content of water in the solvent is a key factor in establishing a homogeneous heterojunction containing cubic phase CoSe2 (c-CoSe2) and orthorhombic phase CoSe2 (o-CoSe2). The built-in electric field generated by the energy band gap difference between ZnSe and CoSe2 or c-CoSe2 and o-CoSe2, and a strong interaction between ZnSe/CoSe2 particles and N-doped carbon nanosheets, can reduce the migration barrier of Li+ at the interface, accelerate charge transfer, and promote the lithium storage kinetic process. In addition, nanoscale ZnSe/CoSe2 particles coupled with N-doped carbon nanosheets can also generate more active sites, reduce volume expansion, and maintain the structural integrity of the anode material. Based on the above structural advantages, the prepared ZnSe/CoSe2-3# exhibits a high reversible capacity (1188 mAh g−1 after 280 cycles at 0.5 A g−1), and excellent long-term cycling stability (788 mAh g−1 at 1 A g−1 over 600 cycles).

Functionalized N-doped carbon nanosheets derived from metal−organic framework as oil-based lubricant additives for improved tribological performance

Herein, the functionalized N-doped carbon nanosheet (N@PCNs) was successfully achieved through pyrolysis of metal−organic framework (MOF) and then surface modification with anti-wear agent. Firstly, the N@PCNs was obtained via carbonization of copper pyridine coordination polymer-based MOFs. Then tannic acid (TA) cross-linked by polyethylenimine (PEI) via Michael addition was grafted on the N@PCNs surfaces. Finally, the anti-wear agent 2,5-dimercaptothiadiazole dimer (DTD) was grafted onto N@PCNs via Michael addition reaction with TA to obtain DTD-N@PCNs. The average COF of 500SN decreases to 0.110 from 0.195, accompanied by 69.3% reduction in wear volume with 1.00 wt% DTD-N@PCNs addition. The lubrication performance is ascribed to the formation of a stable protective film through DTD-N@PCNs facilitating tribochemical reactions, preventing direct contact of the ball-disc pairs.

A Vacuum Vapor Deposition Strategy to Fe Single-Atom Catalysts with Densely Active Sites for High-Performance Zn-Air Battery.

Iron single-atom catalysts (SACs) have garnered increasing attention as highly efficient catalysts for the oxygen reduction reaction (ORR), yet their performance in practical devices remains suboptimal due to the low density of accessible active sites. Anchoring iron single atoms on 2D support is a promising way to increase the accessible active sites but remains difficult attributing to the high aggregation tendency of iron atoms on the 2D support. Herein, a vacuum vapor deposition strategy is presented to fabricate an iron SAC supported on ultrathin N-doped carbon nanosheets with densely active sites (FeSAs-UNCNS). Experimental analyses confirm that the FeSAs-UNCNS achieves densely accessible active sites (1.11×1020sitesg-1) in the configuration of Fe─N4O. Consequently, the half-wave potential of FeSAs-UNCNS in 0.1m KOH reaches a remarkable value of 0.951V versus RHE. Moreover, when employed as the cathode of various kinds of Zn-air batteries, FeSAs-UNCNS exhibits boosting performances by achieving a maximum power density of 306mWcm-2 and long cycle life (>180h) at room temperature, surpassing both Pt/C and reported SACs. Further investigations reveal that FeSAs-UNCNS facilitates the mass and charge transfer during catalysis and the atomic configuration favors the desorption of *OH kinetically.

Self-assembly formation of Co quantum dot loaded N-doped porous carbon cathode for quinoline degradation in the electro-Fenton system

Quinoline is high toxicity and difficult biodegradation in oil washing wastewater. Therefore, efficient removal of quinoline contaminant from water bodies poses a major challenge. Hence, Co quantum dot loaded N-doped porous carbon (CoNC) nanosheets grown in situ on carbon cloth were fabricated as cathode for the degradation of quinoline in electro-Fenton system. Under optimal conditions (c(Fe2+) = 0.5 mM, U = -0.3 V, pH = 3), quinoline was completely degraded within 15 min with superior apparent rate constant of 0.385 min−1, which was 19.6 times higher than that of the ZIF-L precursor, due to the abundance of Co QDs active sites and hydrophilicity and electrical conductivity of N-doped porous carbon. In addition, three reaction pathways for quinoline were deduced by combining Density Functional Theory (DFT) calculation and Liquid Chromatography-Mass Spectrometry (LC-MS). More importantly, in situ FTIR and free energy calculations were analyzed to reveal that pathway Ⅰ as spontaneous reaction was the main reaction pathway. Finally, the toxicity of the intermediates was assessed with ECOSAR software and E. coli experiments, and the overall toxicity decreased during the degradation reactions. This work provides novel perspectives on environmental protection by designing in-situ grown cathodes through self-assembly method, thereby effectively purifying pollutants from wastewater.

Cobalt@Ruthenium Core@Shell nanoparticles embedded within nitrogen-doped carbon nanosheets as reversible oxygen electrocatalysts

Rational design and engineering of cost-effective, high-performance reversible oxygen electrocatalysts for both the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is imperative in advancing the progress of rechargeable metal-air batteries (r-MABs). Herein, nanocomposites based on Co@Ru core@shell nanoparticles embedded within N-doped carbon nanosheets (Co@Ru/CS) are prepared via facile galvanic exchange reactions of RuCl3 with Co/NC and used as an effective oxygen electrocatalyst for rechargeable zinc-air battery (r-ZAB). Electrochemical studies demonstrate a remarkable bifunctional catalytic performance of Co@Ru/CS towards both ORR and OER, featuring a low potential gap (ΔE) of only 0.69 V between the OER potential (E10,OER) at 10 mA cm−2 and half-wave potential (E1/2,ORR) of ORR, which is much lower than that of commercial Pt/C + RuO2 catalysts (0.76 V). Combined studies of experimental characterizations and density functional theory calculations show that the ORR activity arises primarily from the N-doped carbon and CoNx moieties in the composites, whereas RuO2/CoOOH produced at high electrode potentials is responsible for the OER activity. Co@Ru/CS based r-ZAB exhibits an open circuit voltage of 1.447 V, specific capacity of 781 mAh gZn−1, and maximum power density of 115 mW cm−2 at 0.83 V, a performance better than that with commercial Pt/C + RuO2 (1.412 V, 760.56 mAh gZn−1, and 91 mW cm−2). Results from this research underline the substantial impact of structural engineering on optimizing the electrocatalytic activity of nanocomposites for r-MABs.

Shuttle-free zinc–iodine batteries enabled by a cobalt single atom anchored on N-doped porous carbon host with ultra-high specific surface area

Aqueous zinc‑iodine batteries are favorable solutions for grid-level energy storage owing to their cost-effective components and intrinsic safety. Nevertheless, the sluggish conversion kinetics and polyiodide shuttle effect have significantly hindered their practical applications. Herein, a Co single atom anchored on N-doped porous carbon nanosheets (Co-SAs@NPC) was produced through an efficient molten-salt engaged pyrolysis process and further utilized as the iodine host for aqueous zinc-iodine batteries. The large specific surface area (1741 m2 g−1) combined with abundant heteroatom-containing functional groups can afford a tight physical and chemical confinement towards iodine species. Meanwhile, the presence of Co single atoms exhibits high electrocatalytic activity towards I2 reduction reactions. According to the experimental results and DFT theoretical calculations, the resulting Co-SAs@NPC can simultaneously offer generous electrochemical active sites and electrocatalytic activity, which displays a high adsorption ability towards iodide species and boost the reversible redox reactions between iodine and iodides. Consequently, the as-assembled zinc-iodine batteries with Co-SAs@NPC/I2 cathodes can deliver a high specific capacity (295 mA h g−1 at 0.3 A g−1), good rate performance (199 mAh g−1 at 20 A g−1), and long cyclic stability over 10,000 cycles. Additionally, the absence of polyiodide shuttle was analyzed by a series of ex-situ spectrum analyses.

Bagasse derived N-doped graphitic carbon encapsulated cobalt nanoparticles as an efficient bifunctional catalyst for water splitting reactions

The utilization of non-precious metal-based electrodes to unlock cost-effective and scalable processes for the production of clean energy is highly desirable. Herein, we reported a straightforward hydrothermal carbonization method for the synthesize of nitrogen-doped graphitic carbons integrated with cobalt (Co@NGC-600, Co@NGC-700, and Co@NGC-800) from sugarcane bagasse and their electrocatalytic applications in oxygen and hydrogen evolution reactions. The graphitic nature of the Co integrated N-doped carbon materials was confirmed by Raman and XPS analysis. FESEM and HRTEM analysis confirms the dispersion of Co on N-doped carbon nanosheets. The Co@NGC-800 catalyst shows low overpotential and Tafel slope, requiring only 304 mV (84.1 mV dec−1) for oxygen electrode and 234 mV (118 mV dec−1) for HER at a current density of 10 mA cm−2. Moreover, Co@NGC-800 materials showed better activity than Co@NGC-700, Co Co@NGC-600, and Co@NC. The active Co@NGC-800 bifunctional electrocatalysts pair contributes to the fabrication of a water electrolyser with a 10 mA/cm2 current density at 1.68 V. The Co@NGC-800 // Co@NGC-800 electrocatalyst exhibits good stability over a period of 24 h with negligible potential aberration during the process of water splitting. The electrocatalytic performance of the prepared catalyst in a 1.0 M KOH solution exhibits admirable bifunctional activity and remarkable stability. In fact, it outperforms cobalt-based and carbon-supported electrocatalysts, including highly valued commercial catalysts like IrO2 and Pt@C. The solar cell configuration, utilizing the energetic bifunctional Co@NGC-800 electrocatalyst, can continuously generate hydrogen and oxygen. The overall water-splitting process of Co@NGC-800 catalyst delivered at a cell voltage of 1.68 V, enabling sustained and efficient oxygen and hydrogen evolution at a large scale.

Ru embedded into N-Doped Porous Carbon Nanosheets as a Robust Catalyst for Efficient Hydrogenation of Levulinic Acid to γ-Valerolactone

Ru embedded into N-Doped Porous Carbon Nanosheets as a Robust Catalyst for Efficient Hydrogenation of Levulinic Acid to γ-Valerolactone

2D ZIF-8 derived N-doped porous carbon nanosheets for high-performance Li-Se batteries

Lithium-selenium (Li-Se) batteries have attracted increasing attention because of excellent carbonate electrolyte compatibility, comparable theoretical volumetric specific capacity and high electrical conductivity. However, there are still unavoidable issues such as large volume expansion, rapid capacity decay and slow electrochemical reaction kinetics for practical applications. In this work, we report 2D ZIF-8 derived N-doped porous carbon nanosheets (NPC-NS) as Se host for high-performance Li-Se batteries. The unique 2D structure of Se@NPC-NS facilitates Li+ diffusion and charge transfer, thus the Se@NPC-NS cathode exhibits fast electrochemical reaction kinetics. In addition, the N doping enhances electronic conductivity and porous structure mitigates the volume expansion. As a result, the Se@NPC-NS cathode delivers a high reversible capacity of 585 mAh/g with a capacity retention of 99.1 % at 0.5C (1C = 675 mA g−1) after 225 cycles. Especially after 500 cycles at a high current density of 10C, the Se@NPC-NS cathode still displays a reversible specific capacity of 307 mAh/g with only 0.03 % capacity decay per cycle. This work would shed some light on the 2D carbon host as Se-based cathode for high-rate and long-life performance Li-Se batteries.

Highly Active CoNi-CoN3 Composite Sites Synergistically Accelerate Oxygen Electrode Reactions in Rechargeable Zinc-Air Batteries.

Reaching rapid reaction kinetics of oxygen reduction (ORR) and oxygen evolution reactions (OER) is critical for realizing efficient rechargeable zinc-air batteries (ZABs). Herein, a novel CoNi-CoN3 composite site containing CoNi alloyed nanoparticles and CoN3 moieties is first constructed in N-doped carbon nanosheet matrix (CoNi-CoN3/C). Benefiting from the high electroactivity of CoNi-CoN3 composite sites and large surface area, CoNi-CoN3/C shows a superior half-wave potential (0.88V versus RHE) for ORR and a small overpotential (360mV) for OER at 10mAcm-2. Theoretical calculations have demonstrated that the introduction of CoNi alloys has modulated the electronic distributions near the CoN3 moiety, inducing the d-band center of CoNi-CoN3 composite site to shift down, thus stabilizing the valence state of Co active sites and balancing the adsorption of OER/ORR intermediates. Accordingly, the reaction energy trends exhibit optimized overpotentials for OER/ORR, leading to superior battery performances. For aqueous and flexible quasi-solid-state rechargeable ZABs with CoNi-CoN3/C as catalyst, a large power density (250mWcm-2) and high specific capacity (804mAhg-1) are achieved. The in-depth understanding of the electroactivity enhancement mechanism of interactive metal nanoparticles and metal coordinated with nitrogen (MNx) moieties is crucial for designing novel high-performance metal/nitrogen-doped carbon (M─N─C) catalysts.

Insights into the efficient water treatment over N-doped carbon nanosheets with layered minerals as template: The role of interfacial electron tunneling and transfer

Peroxymonosulfate (PMS) oxidation reactions have been extensively studied recently. Due to the high material cost and low catalytic capability, PMS oxidation technology cannot be effectively applied in an industrial water treatment process. In this work, we developed a modification strategy based on enhancing the neglected electron tunneling effect to optimize the intrinsic electron transport process of the catalyst. The 2D nitrogen-doped carbon-based nanosheets with small interlayer spacing were prepared by self-polymerization of dopamine hydrochloride inserted into the natural layered bentonite template. Systematic characterizations confirmed that the smaller layer spacing in the 2D nitride-doped carbon-based nanosheets reduces the depletion layer width. The weak electronic shielding effect derived by the small layer spacing on the material subsurface enhanced the bulk electron tunneling effect. More bulk electrons could be migrated to the catalyst surface to activate PMS molecules. The PMS activation system showed ultrafast oxidation capability to degrade organic pollutants and strong ability to resist interference from environmental matrixes due to the optimized electron transfer process. Furthermore, the developed membrane reactor exhibited strong catalytic stability during the continuous degradation of P-Chlorophenol (CP).