Graphitic Carbon Nitride Research Articles

Potassium and Boron Co-Doping of g-C3N4 Tuned CO2 Reduction Mechanism for Enhanced Photocatalytic Performance: A First-Principles Investigation

Graphitic phase carbon nitride (g-C3N4, abbreviated as CN) can be used as a photocatalyst to reduce the concentration of atmospheric carbon dioxide. However, there is still potential for improvement in the small band gap and carrier migration properties of intrinsic materials. K-B co-doped CN (KBCN) was investigated as a promising photocatalyst for carbon dioxide reduction via the Density Functional Theory (DFT) method. The electronic and optical properties of CN and KBCN indicate that doping K and B can improve the catalytic performance of CN by promoting charge migration and separation. In terms of the Gibbs free energy change, the CO2 reduction reaction catalysed by KBCN results in CH3OH, and its optimal pathway is CO2 → *CO2 → *COOH → CO → *OCH → HCHO → *OCH3 → CH3OH. Compared with CN, the doping elements K and B shift the rate-determining step from CO2 → *CO2 to *CO2 → *COOH. The K and B elements co-doping tuned the charge distribution between the catalyst and the adsorbate and reduced the Gibbs free energy of the rate-determining step from 1.571 to 0.861 eV, suggesting that the CO2 reduction activity of KBCN is superior to that of CN. Our work provides useful insights for the design of metallic–nonmetallic co-doped CN for photocatalytic CO2 reduction (CO2PR) reactions.

Conductive Islands Assisted Resistive Switching in Biomimetic Artificial Synapse for Associative Learning and Image Recognition

AbstractSolution‐processed memristor devices hold significant potential for advancing synaptic applications, offering scalable, cost‐effective, and efficient solutions for next‐generation neuromorphic systems. These devices replicate the behavior of biological synapses with their gradual and continuous changes in resistance, making them promising for neuromorphic computing and artificial neural networks. However, understanding the temporal characteristics and cumulative effect of successive pulses on the devices is essential for emulating the dynamics of biological synapses. This study proposes a hybrid materials‐based conductive islands‐assisted resistive switching (CIARS) in a solution‐processed active layer consisting of thermally exfoliated graphitic carbon nitride (g‐C3N4 abbreviated as CN) nanosheets embedded with silver nanoparticles (Ag NPs). The fabricated devices demonstrate repeatable and bipolar memory features with a lower operating voltage (≤0.5 V), emulating the frequency and amplitude‐dependent synaptic plasticities. The threshold switching occurs due to the formation of conduction filaments (CFs) of silver ion (Ag+), whereas the analog behavior results from the voltage pulse‐dependent modulation of Schottky barrier height combined with metallic CFs formation. The experimental findings demonstrate the efficacy of the CIARS mechanism within the material platform, highlighting its potential for applications in associative learning, Morse code detection, and image recognition.

Visible‐Light‐Induced Rapid Elimination of Antibiotic Resistance Contaminations Using Graphitic Carbon Nitride Tailored with Carrier Confinement Domains

AbstractSolar water disinfection facilitated by photocatalyst has been considered a viable point‐of‐use (POU) method for mitigating antibiotic resistance contaminations at the household or community levels. Here, density functional theory calculations are used to guide the fabrication of a carrier confinement domains (CCD)‐decorated graphitic carbon nitride (CN) photocatalyst. The CCD integration effectively disrupts the electron distribution symmetry of CN, amplifies its local electron density, and facilitates the formation of long‐range ordered structure, thereby enhancing charge separation efficiency. Importantly, the CCD directs the migration of photogenerated carriers to specific regions upon light illumination, effectively minimizing their spatial proximity. As a result, the overall reactive oxygen species level of the photocatalytic system is markedly elevated, with a twelvefold increase in H2O2 concentration, alongside a nearly two‐order‐of‐magnitude rise in •O2− and •OH steady‐state concentrations. Remarkably, a record‐high disinfection efficiency is attained, successfully inactivating 7 log of antibiotic‐resistant bacteria within 30 min. Additionally, the photocatalyst can be integrated into a continuous‐flow fixed‐bed reactor, facilitating clean water production for up to 60 h at a rate of 121 L m−2 day−1, highlighting its significant potential for POU applications.

Research on Graphitic Carbon Nitride (g-C3N4) prepared by template-based method and its photocatalytic properties

Abstract. The Graphitic Carbon Nitride (g-C3N4), a non-metallic polymer photocatalytic material, has a wide range of raw materials and a simple preparation process. Due to its unique electronic structure and excellent photocatalytic performance, g-C3N4 has attracted wide attention in the field of environmental purification and energy conversion in recent years. However, g-C3N4 faces a lot of challenges, including a wide band gap, many interlayer defects, and poor interlayer electron transport. Nevertheless, its unique semiconductor structure and chemical stability still provide the possibility to explore the effect of its piezoelectric properties on photocatalysis, which paves the way for a novel approach to environmentally friendly hydrogen production. Therefore, the paper delves into the application of different template methods in the preparation of g-C3N4 by reviewing the related literature, and analyzes the role of different template materials in the preparation. In addition, in this paper, the photocatalytic properties of g-C3N4 are explored, which are mainly reflected in the photocatalytic water separation performance and photocatalytic degradation of organic dyes. It is found that the g-C3N4 shows great potential in the fields of photocatalytic water decomposition for hydrogen production and degradation of organic pollutants due to its unique band gap, nontoxicity, low cost and wide range of sources. Future research should continue to explore more kinds of template materials and their preparation processes, with the aim of realizing further enhancement of the performance of g-C3N4 photocatalysts and promoting their practical applications in the fields of environment and energy.

Efficient uranium removal by amidoxime functionalized graphitic carbon nitride and its potential mechanism

Efficient uranium removal by amidoxime functionalized graphitic carbon nitride and its potential mechanism

A Z-scheme g-C3N4/TiO2 heterojunction for enhanced performance in protecting magnesium and nickel couple from galvanic corrosion

Large interfacial contact is crucial for designing novel heterostructure materials to achieve good photoelectrochemical performance. Herein, we prepared a composite photoanode consisting of titanium dioxide (TiO2) nanotubes and graphitic carbon nitride (g-C3N4) nanosheets for enhancing the photocathodic protection (PCP) capability of the nickel-coated Mg alloy (Mg/Ni). The composite g-C3N4/TiO2 (CN/TiO2) photoanode was achieved by depositing g-C3N4 on the TiO2 nanotubes grown titanium foil via a one-step thermal polymerization of melamine and thiourea mixture. A series of characterizations, including transmission electron microscope, X-ray photoelectron spectroscopy, and electron paramagnetic resonance spectra, manifested the successful deposition of g-C3N4 at the inner wall of the TiO2 nanotubes to achieve sufficient interfacial contact and the formation of a Z-scheme heterojunction to promote the charge carriers’ transfer and separation. Compared with the pure TiO2 photoanode, the heterojunction exhibited enhanced photoelectrochemical and photocathodic protection performances, which was confirmed by the electrochemical measurements. The heterojunction achieved a duration of 6.5 h to protect the Mg-Ni couple from galvanic corrosion, representing a tenfold enhancement compared with the uncoupled Mg/Ni electrode. These findings demonstrate the great potential of constructing a unique Z-scheme heterojunction with a sizeable interfacial contact area to enhance the PCP capability of metals.

A Well‐Coupled Supramolecular System Accelerates Photophosphorylation

AbstractSupramolecular assembly allows multiple chemical/bio‐components integrated as one system for cascade biochemical reactions. Herein the graphitic carbon nitrides (g‐C3N4) as photocatalyst trapped in a dipeptide hydrogel covering adenosine triphosphate (ATP) synthase accelerates the photophosphorylation through ATP synthesis. Self‐assembled N‐fluorenylmethoxycarbonyl diphenylalanine (Fmoc‐FF) as nanofibrils to allow g‐C3N4 nanosheets are embedded as a complex Fmoc‐FF/g‐C3N4 hydrogel. Fmoc‐FF gel exhibits good electronic coupling with g‐C3N4, which enables a photo‐induced proton generation. The transmembrane proton gradient can be established by ATP synthase‐lipid reconstituted on the surface of the Fmoc‐FF/g‐C3N4 hydrogel to enhance the ATP synthesis. It indicates that the Fmoc‐FF/g‐C3N4/ATP synthase‐lipid film can possess a longer‐term ATP production capability and allow repeated immersion for sustained ATP production. Such a hydrogel‐supported ATP synthesis platform is achieved by a procedure at a larger scale.

Enhancing photovoltaic performance of dye-sensitized solar cells through TiO2/g-C3N4 nanocomposite photoanodes for improved charge carrier management

This study explores the enhancement of dye-sensitized solar cells (DSSCs) through the modification of porous TiO2 photoanodes by incorporating two-dimensional graphitic carbon nitride (g-C3N4) synthesized from urea. The combination of wide-bandgap TiO2 with narrow-bandgap g-C₃N₄ extends the optical response range of the TiO2 heterostructure composites from ultraviolet to visible light. The introduction of g-C3N4 with TiO2 to form a heterojunction significantly boosts the photovoltaic performance of the device by minimizing charge recombination at the photoanode-electrolyte interface. Upon optimizing the g-C3N4 loading, a peak power conversion efficiency (PCE) of 10.79 % is achieved, representing an impressive 42 % improvement over the pristine TiO2-based device. This enhancement is primarily attributed to the efficient separation of photogenerated charge carriers, facilitated by the type II band alignment between g-C3N4 and TiO2. This alignment, enabled by favorable conduction and valence band offsets, accelerates the separation of photogenerated carriers and prolongs electron lifetime.

NiPd Nanoparticles on Nanoporous Carbon Embedded in Graphitic Carbon Nitride for Transfer Hydrogenation and Suzuki–Miyaura Coupling Reactions

NiPd Nanoparticles on Nanoporous Carbon Embedded in Graphitic Carbon Nitride for Transfer Hydrogenation and Suzuki–Miyaura Coupling Reactions

Development of engineered Zn-MOF/g-C3N4 based photoelectrochemical system for real-time sensors and removal of naproxen in wastewater

Naproxen-contaminated water may lead to the accumulation of the drug in aquatic organisms and can pose high risks to an aquatic environment and human beings. Therefore, this work aimed to develop photoelectrochemical sensing and degradation of naproxen (NPX) using zinc-metal organic framework /graphitic carbon nitride thin film-based fluorine-doped tin oxide (Zn-MOF/g-C3N4/FTO) as anode material for the sensing and degradation of naproxen (NPX). The surface morphology, structure, surface property, surface area, optical property, photocurrent, and charge transfer kinetics abilities were studied using different techniques. The nanocomposites showed a superior photocurrent response (0.815 mA cm-2) compared to the original g-C3N4 (0.328 mA cm-2). The photo-anode made of Zn-MOF@g-C3N4/FTO displayed the highest photocurrent value, indicating that the alignment of the two semiconductor bands prevented the quick recombination of electron-hole pairs. Owing to these attractive features, the Zn-MOF/g-C3N4/FTO electrode was applied for photoelectrochemical detection of NPX using chronoamperometry. Interestingly, the nanocomposites-based FTO ascribed a lower detection limit (2.3 ng l-1) with a wide linear range concentration of NPX (0.5 to 200 µg l-1). Additionally, the analytical assessment of repeatability and reproducibility demonstrated robust performance, with commendable relative standard deviations (RSD%) of 2.54 % and 2.40 %, respectively. On the other hand, a remarkable degradation efficiency of 97.52 % was attained when employing a bias potential of 0.1 V during a 2 h photoelectrocatalytic oxidation of NPX. The degradation process was primarily driven by the active participation of holes and hydroxyl radicals in ring opening and subsequent cleavage of by-products. The notable effectiveness of this degradation can be attributed to the combined and synergistic effects of both electrochemical and photocatalytic degradation techniques. The current state demonstrates its effectiveness in the photoelectrochemical sensing and removal of NPX using MOF/g-C3N4 nanocomposites-based electrode materials in wastewater.

Oxygen-Doped Porous Ultrathin Graphitic Carbon Nitride Nanosheets for Photocatalytic Hydrogen Evolution and Rhodamine B Degradation.

Graphite phase carbon nitride (g-C3N4) is a highly promising metal-free photocatalyst, but its low activity, due to limited quantum efficiency and small specific surface area, restricts its practical application. While exfoliating bulk crystals into porous thin-layer nanosheets and incorporating dopants have been shown to improve photocatalytic efficiency, these methods are typically complex, time-consuming, and costly processes. In this study, we developed a simple approach to synthesize oxygen-doped porous g-C3N4 (OCN) nanosheets. The resulting OCN exhibited significantly enhanced light absorption and visible-light photocatalytic activity compared to bulk g-C3N4 (BCN) and g-C3N4 (CN). The OCN achieved an impressive hydrogen evolution reaction (HER) rate of 8.02 mmol g-1 h-1, eight times greater than BCN, and demonstrated a high Rhodamine B (RhB) degradation rate of 97.3 % owing to the generation of abundant singlet oxygen. These improvements in photocatalytic performance are attributed to the narrow band gap and enhanced electron transfer properties, suggesting a promising route for the efficient design of g-C3N4-based photocatalysts.

Surface Coordination Chemistry of Graphitic Carbon Nitride from Ag Molecular Probes.

Graphitic carbon nitride (g-C3N4) has gained significant attention for its catalytic properties,especiallyin the development of Single Atom Catalysts (SACs).However,the surface chemistry underlying the formation of these isolated metal sites remains poorly understood.In thisstudyweemploy Surface OrganoMetallic Chemistry (SOMC) together with advanced microscopic and spectroscopic techniquesfor an in-depth analysis of functionalizedg-C3N4materials, where tailored organosilver probe molecules are used to monitor surface processes and characterize resulting surface species. Amulti-technique approach-including high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM), X-ray absorption spectroscopy (XAS), and multinuclear solid-state Nuclear Magnetic Resonance spectroscopy (ssNMR),coupled with density functional theory (DFT) calculations- identifies three primary surface speciesin Ag-functionalized g-C3N4:bis-NHC-Ag+, dispersed Ag+sites, andphysisorbed molecular precursor.These findings highlight a dynamic grafting process and provide insights into the surface coordination chemistryof functionalizedg-C3N4materials.

Polarized electric field-mediated graphitic carbon nitride-based S-scheme heterostructure for efficient photocatalytic removal of bisphenol A

Tuning interface charge transfer is considered as a feasible way to promote electron migration and separation in heterojunction system, but the role of in-plane electron behavior in single phase has received little attention. Here, a carboxyl functionalized graphitic carbon nitride (CCN) coupled PbBiO2Br (PBOB) S-scheme heterostructure is elaborately designed for investigation. Compared with pristine CN/PBOB, although the existence of carboxyl group weakens the built-in electric field strength of CCN/PBOB (ΔΦ = 0.44 eV), the formed polarized electric field (µ = 3.18 Debye) is conducive to the pre-separation of photogenerated electrons and holes in CCN, thereby improving interface charge transfer. In addition, the introduced carboxyl group can also serve as an O2 adsorption site to enhance its activation, and generate reactive oxygen species (ROS) through a two-step single-electron O2 reduction route. Thus, the optimized CCN/PBOB exhibits excellent photocatalytic ROS generation ability, which can remove 88.7 % of bisphenol A and significantly reduce the acute toxicity of the formed intermediates. This work provides a new perspective for the development of advanced heterojunction photocatalyst by regulating in-plane/interface charge dynamics, and helps to fully understand the pollutant detoxification/degradation process initiated by molecular oxygen activation.

Self-Assembly Synthesis of Oxygen and Sulfur Co-Doped Porous Graphitic Carbon Nitride Nanosheets for Boosting CO2 Photoreduction.

Graphitic carbon nitride (CN) has garnered considerable attention in the field of visible-light CO2 photoreduction, but its efficiency remains limited by the intrinsic π-conjugated skeleton. Here, O and S were co-doped CN (O, S/CN) by a facile "hydrolysis + calcination" approach to modulate the physicochemical and electronic structure. Distinctive from S doped CN (SCN), O, S/CN owned porous layer structure with several nanosheets and less SO4 2- groups on the surface. The amount of heteroatom-doping was achieved by changing the hydrothermal temperature. The optimum O, S/CN-80 achieved moderate CO production rate of 1.29 μmol g-1 h-1, which was 3.79 times as much as SCN (0.34 μmol g-1 h-1). The O and most S atoms were substitutionally doped and the effect of S doped state on the improved efficiency of CO generation in O, S/CN was also explored based on the theoretical calculations. This work provides an inspiration to develop efficient dual-doped CN photocatalysts for photocatalytic CO2 reduction.

Visual aptasensor based on PtNPs/g-C3N4 and DNase I for the field detection of acetamiprid.

A visual aptasensor based on the combination of graphitic carbon nitride loaded with platinum nanoparticles (PtNPs/g-C3N4) and deoxyribonuclease I (DNase I) was developed for detecting acetamiprid. The prepared PtNPs/g-C3N4 exhibited excellent peroxidase (POD)-like activity, demonstrating the capacity to oxidize the colourless o-phenylenediamine (OPD) to produce the coloured product diaminophenazine (DAP) in the presence of hydrogen peroxide (H2O2). The DNA aptamer of acetamiprid can adsorb onto the surface of PtNPs/g-C3N4, thereby inhibiting its POD activity. The binding of acetamiprid to its aptamer results in the aptamer desorbing from the surface of PtNPs/g-C3N4 and subsequent digestion by DNase I. Ascribed to the synergistic effect of these factors, the aptasensor can achieve the rapid on-site detection of acetamiprid based on the acetamiprid-induced the colour change of the solution just with the smartphone. Furthermore, due to the remarkable fluorescence signal of DAP at 570nm, the aptasensor under fluorescence mode enables highly sensitive and quantitative detection of acetamiprid with a linear range of 1 ng/mL to 4µg/mL and a detection limit as low as 0.31 ng/mL.Theaptasensor has successfully realized the detection of acetamiprid in river water and cucumber samples, offering a novel perspective for the rapid assessment of environmental pollution and food safety risks associated with acetamiprid residues.

Z-Scheme Enabled 1D/2D Nanocomposite of ZnO Nanorods and Functionalized g-C3 N4 Nanosheets for Sustainable Degradation of Terephthalic Acid.

The urgent need to mitigate water pollution and achieve Sustainable Development Goal 14 (SDG 14)-Life below water, necessitates developing efficient and eco-friendly wastewater treatment technologies. This research addresses this challenge by photocatalytic degradation of terephthalic acid, a precursor for PET bottles using environment-friendly and biocompatible photocatalysts. The 1D/2D nanocomposite comprising zinc oxide (ZnO) nanorods and functionalized graphitic carbon nitride (Zn-TG) nanosheets were synthesized and thoroughly characterized. The nanocomposite effectively mitigated the individual drawbacks of Zn-TG agglomeration and the wide band gap of ZnO as confirmed through zeta potential and Tauc's plot studies, respectively. The synthesized nanocomposite achieved ~100 % degradation within 60 minutes, exhibiting superior kinetics (~2.5 times) compared to pristine samples. The enhanced degradation efficiency was elucidated by efficient charge carrier transfer (~5 times faster) and separation (~2 times improved) as confirmed through electrochemical impedance spectroscopy and time-resolved photoluminescence studies. The proposed Z-scheme pathway provides mechanistic insights. This proposed mechanism is supported by extensive electron paramagnetic resonance (EPR) and scavenger studies. The liquid chromatography-mass spectrometry (LC-MS) analysis confirms the formation of less toxic byproducts for ensuring that the wastewater treatment process is efficient and environmentally friendly. This research helps in developing a highly effective and sustainable wastewater treatment technology.

Catalytic hydrogenation of CO2 by composite nickel species supported on KCl-doped graphitic carbon nitride under normal temperature and atmospheric pressure

CO2 can be used as a cheap C1 feedstock to produce value-added chemical products and fuels. In this work, it was proposed for the first time that potassium chloride-doped graphitic carbon nitride-supported composite nickel species (CNS/KCl-g-C3N4) was prepared to catalyze CO2 hydrogenation with potassium borohydride (KBH4) as a hydrogen donor to produce formate at normal temperature and atmospheric pressure. The catalytic activity of CNS/KCl-g-C3N4 reached the best when the nickel loading was optimized as 15 wt%. By using CNS/KCl-g-C3N4, the hydrogen production volume and rate of KBH4 hydrolysis were reduced by 49 % and 32 %, respectively, while the formate concentration was increased by 43 %. It was speculated that the catalytic hydrogenation of CO2 was enhanced due to the chemical adsorption of CO2 on the catalyst surface by interacting with the K-N bonds and -NH2 groups, and the formation of BH4-n(OH)n- (n=0–3) with higher activity from BH4- on the Ni0 sites.

Theoretical Study of the Magnetic Mechanism of a Pca21 C4N3 Monolayer and the Regulation of Its Magnetism by Gas Adsorption

For metal-free low-dimensional ferromagnetic materials, a hopeful candidate for next-generation spintronic devices, investigating their magnetic mechanisms and exploring effective ways to regulate their magnetic properties are crucial for advancing their applications. Our work systematically investigated the origin of magnetism of a graphitic carbon nitride (Pca21 C4N3) monolayer based on the analysis on the partial electronic density of states. The magnetic moment of the Pca21 C4N3 originates from the spin-split of the 2pz orbit from special carbon (C) atoms and 2p orbit from N atoms around the Fermi energy, which was caused by the lone pair electrons in nitrogen (N) atoms. Notably, the magnetic moment of the Pca21 C4N3 monolayer could be effectively adjusted by adsorbing nitric oxide (NO) or oxygen (O2) gas molecules. The single magnetic electron from the adsorbed NO pairs with the unpaired electron in the N atom from the substrate, forming a Nsub-Nad bond, which reduces the system’s magnetic moment from 4.00 μB to 2.99 μB. Moreover, the NO adsorption decreases the both spin-down and spin-up bandgaps, causing an increase in photoelectrical response efficiency. As for the case of O2 physisorption, it greatly enhances the magnetic moment of the Pca21 C4N3 monolayer from 4.00 μB to 6.00 μB through ferromagnetic coupling. This method of gas adsorption for tuning magnetic moments is reversible, simple, and cost-effective. Our findings reveal the magnetic mechanism of Pca21 C4N3 and its tunable magnetic performance realized by chemisorbing or physisorbing magnetic gas molecules, providing crucial theoretical foundations for the development and utilization of low-dimensional magnetic materials.

Facile synthesis of CQD/g-C3N4 as a highly effective metal-free photocatalyst for the degradation of carmoisine and indigo carmine dye

The development of extensive dye pollution in the water ecosystem seriously endangers the health of the living organism. For effectively eradicating dyecontaminants from water bodies, photocatalysis is consideredan effective, energy-consumption, inexpensive disinfection technique. As an alternative to conventional metal-based catalysts, heterogeneous metal-free photocatalysts are more sustainable and kinder to the environment. Here, we reported the simplehydrothermalchemical production of Carbon Quantum dots (CQD)-doped graphitic carbon nitride(GCN). Analytical instruments such as XRD, SEM, FE-SEM, HR-TEM, EDX, FT-IR, thesurface area of BET analysis, photoluminescence, and UV–vis spectroscopy, zeta potentialwere used to characterize the as-prepared CQD doped GCN (CDCN). The degradation studies reveal that the CDCN catalyst displays the highest rate of degradation performance than pure GCN. Within 60 min, it shows 96 % degradation toward indigo Carmine (IC) and 93 % decomposition towards carmoisine dye (CM). Significant e−/h+ separation, an increased surface area, and a high redox potential capacity to induce charge bears may all contribute to the CDCN catalyst’s enhanced photocatalytic degradation efficiency. The efficiency of the photocatalytic process was optimized by studying and altering many variables. These include Dye concentration, catalyst concentration, and variation of the pH solution were some of these. The nanocomposite exhibited excellent stability after three successive runs of the photocatalytic procedure. According to the kinetics analysis results indicate that the photocatalytic decomposition of Indigo Carmine (IC) and carmoisine (CM) dye follows pseudo-first-order kinetics. For better photodegradation performance, a potential photocatalytic method employing several pairs of electron-hole acceptor scavengershas been put forth. Based on the positionsof the band gap and the result of the characterization, a feasible mechanismpathway for charge carriers was also presented.

Novel N-doped carbon nanotubes impregnated Mn spheres with polydopamine coating as an efficient polysulfide immobilizer for Li-S batteries

Lithium-sulfur (Li-S) batteries are one of the most promising energy storage and conversion devices due to the high theoretical capacity and cost-effectiveness of sulfur. However, they still suffer from sluggish redox kinetics and the shuttle effect caused by complex polysulfides. In this work, graphitic carbon nitride (g-C3N4) is utilized as a template and further hydrothermally treated with an Mn source and glucose. The pyrolysis of g-C3N4 gives rise to N-doped carbon nanotubes, producing abundant sites for physical confinement and chemical adsorption of polysulfides, while glucose carbonization brings forth amorphous carbon and Mn source produces metal spheres. Afterward, polydopamine (PDA) induces N-doped carbon coating and promotes interface connection as well as electron immigration. This synergistic design possesses a high surface area of micropores and mesopores to aggregate sulfur and accelerate redox kinetics. As a result, the N-doped carbon nanotube with Mn spheres and PDA coating@sulfur (CN/Mn-PDA@S) exhibits a high reversible capacity of 813.5 mAh g−1 at 1 C with a decay rate of 0.064% per cycle and remarkable capacity retention at 2 C with rate performance up to 4 C. Therefore, the novel design of N-doped carbon nanotubes with Mn spheres and PDA coating serves as an efficient polysulfide immobilizer for Li-S batteries.