Charged Carbon Research Articles

Multilayer pH-responsive hollow mesoporous silica nanoparticles with charge reversal for drug delivery and real-time monitoring by fluorescence

Drug delivery systems (DDSs) with charge reversal could simultaneously achieve long circulation time and enhanced cellular internalization efficiency. Here, hollow mesoporous silica nanoparticles (HMSNs) were used as the basic stuff for encapsulating doxorubicin (DOX), positive-charged chitosan (CS) was grafted on the surface of HMSNs, and negatively charged carboxyl-rich carbon dots (CDs) were coated on the outer layer of CS through non-covalent bonds. The new drug delivery vehicles with 56.6 % drug-loading content were prepared, named as CDs-CS/HMSNs@DOX. Tumor environment with a slightly acidic state could trigger the disruption of the non-covalent bonds, followed by the detachment of CDs, making the negatively charged CDs-CS/HMSNs@DOX change into positively charged CS/HMSNs@DOX. CS swelling reaction also happened in slightly acidic conditions. Both the CS swelling and the detachment of CDs resulted in the exposure of mesopore and drug release. Fluorescence recovery of detached CDs could be used to monitor the release of DOX in real-time. The multilayer pH-responsive nano carries with charge reversal and real-time monitoring demonstrated broad application prospects.

Ionization-modified beetle structure for enhanced demulsification and anti-clogging performances

Superwetting materials are considered to have great potential for oil–water separation in water purification, food processing, petrochemical production, etc. However, weak demulsification performance and clogging are the key challenges in most practical applications. Here, we successfully prepared a charged beetle structure copper foam (SPCS-CF) with a surface composed of superhydrophilic charged carbon nanotubes and superhydrophobic SiO2 bumps, which can apply electrostatic force and wetting driving force to obtain higher demulsification and anti-clogging performances than conventional superhydrophilic materials. These two forces can cause the charged surfactant and the oil to move towards the charged carbon nanotubes and superhydrophobic SiO2 surfaces, respectively, resulting in charge heterogeneity and severe deformation of droplets, thereby enhancing the demulsification performance of SPCS-CF. Therefore, SPCS-CF can separate various oil-in-water emulsions with high separation efficiency (over 99.2 %) and high permeation flux (27,734.0 L m-2 h−1). Furthermore, superhydrophobic SiO2 prevents oil droplets from accumulating in pores and causing clogging by aggregating them on the skeleton. Therefore, this charged beetle structure provides a new perspective for developing advanced materials for demulsification and separation in the petroleum industry and water purification fields.

Biophilic Positive Carbon Dot Exerts Antifungal Activity and Augments Corneal Permeation for Fungal Keratitis.

Fungal keratitis (FK) is an infectious eye disease that poses a significant risk of blindness. However, the effectiveness of conventional antifungal drugs is limited due to the intrinsic ocular barrier that impedes drug absorption. There is an urgent need to develop new therapeutic strategies to effectively combat FK. Herein, we synthesized an ultrasmall positively charged carbon dot using a simple stage-melting method. The carbon dot can penetrate the corneal barrier by opening the tight junctions, allowing them to reach the lesion site and effectively kill the fungi. The results both in vitro and in vivo demonstrated that it exhibited good biocompatibility and antifungal activity, significantly improving the therapeutic effect in a mouse model of FK. Therefore, this biophilic ultrasmall size and positive carbon dot, characterized by its ability to penetrate the corneal barrier and its antifungal properties, may offer valuable insights into the design of effective ocular nanomedicines.

MOF‐derived 1D/3D N‐doped porous carbon for spatially confined electrochemical CO2 reduction to adjustable syngas

AbstractElectrochemical reduction of CO2 to syngas (CO and H2) offers an efficient way to mitigate carbon emissions and store intermittent renewable energy in chemicals. Herein, the hierarchical one‐dimensional/three‐dimensional nitrogen‐doped porous carbon (1D/3D NPC) is prepared by carbonizing the composite of Zn‐MOF‐74 crystals in situ grown on a commercial melamine sponge (MS), for electrochemical CO2 reduction reaction (CO2RR). The 1D/3D NPC exhibits a high CO/H2 ratio (5.06) and CO yield (31 mmol g−1 h−1) at −0.55 V, which are 13.7 times and 21.4 times those of 1D porous carbon (derived from Zn‐MOF‐74) and N‐doped carbon (carbonized by MS), respectively. This is attributed to the unique spatial environment of 1D/3D NPC, which increases the adsorption capacity of CO2 and promotes electron transfer from the 3D N‐doped carbon framework to 1D carbon, improving the reaction kinetics of CO2RR. Experimental results and charge density difference plots indicate that the active site of CO2RR is the positively charged carbon atom adjacent to graphitic N on 1D carbon and the active site of HER is the pyridinic N on 1D carbon. The presence of pyridinic N and pyrrolic N reduces the number of electron transfer, decreasing the reaction kinetics and the activity of CO2RR. The CO/H2 ratio is related to the distribution of N species and the specific surface area, which are determined by the degree of spatial confinement effect. The CO/H2 ratios can be regulated by adjusting the carbonization temperature to adjust the degree of spatial confinement effect. Given the low cost of feedstock and easy strategy, 1D/3D NPC catalysts have great potential for industrial application.

System of metastable volume-localized electronic states in positively charged semiconductor single-wall carbon nanotubes

The volume-localized electronic states (SAMOs) with a maximum of their electron wave functions located in the cavity of nanomaterials have been experimentally and theoretically demonstrated in a fullerene. The existence of SAMOs in single-wall carbon nanotubes (SWCNTs) was also predicted theoretically. In the present paper, these volume states in semiconductor SWCNTs were theoretically investigated using numerical quantum modeling based on density functional theory (DFT). It is shown that the well appears in the center of the tube, whose depth increases with increasing positive charge, since the total potential of a positively charged structure can be represented as the sum of the Coulomb potential and the potential of the atoms of the tube wall. In this context, in addition to the well-studied surface-localized states, states localized in the volume of the cylinder also occur. Using the components of the electric transition dipole moment, the lifetime of the volume states was preliminarily estimated in comparison to the lifetime of the ordinary surface states.

Disjoining Pressure Decay Length in Room-Temperature Ionic Liquids: A Molecular Simulation Study.

We present all-atom molecular simulations to investigate the behavior of 1-ethyl-3-methylimidazolium tetrafluoroborate ([EMIM][BF4]) in negatively charged carbon nanopores of different widths (h = 5÷15 nm) and lengths (l = 4÷10 nm). The goal of our study was to determine how the disjoining pressure varies as a function of the pore width at different lengths and to understand the influence of edge effects. Our results show that the edge effect decreases as the pore length increases. Using an exponential function, we can approximate the disjoining pressure at large pore widths and use this approximation to estimate the decay length that can correlate with the electrostatic screening length. The results agreed well with those of previous experimental studies.

Efficient Removal of Acetamiprid Pesticide Using Date Core-Derived Activated Carbon and Korai Clay As A Good Sorbent

We used activated carbon derived from Iraqi date cores to study the efficacious removal of acetamiprid pesticide effluent. This activated carbon was made using chemicals and physical processes involving a 5M hosphoric acid solution. Various factors such as the concentration of acetamiprid pesticide, mixing duration, contact time, the quantity of activated carbon, temperature, and pH of the media were examined to understand how they influence the efficiency of acetamiprid pesticide removal. The results show that maximum adsorption of 0.05 g/L dosage, 150 mg/L dye concentration, and 3-hour contact time adsorption duration were optimal for 97.00- 99.00% removal efficiency. The adsorption equilibrium was performed using Freundlich, Temkin, Harkins-jura, Dupin, Elovitch, and Langmuir. Density function theory (DFT) was used to simulate the pesticide acetamiprid to determine the reaction origin. The results show that the Freundlich model with R2 values equal to 0.738 demonstrated better agreement with the adsorption experimental data. According to thermodynamic analysis, the pesticide is endothermic and spontaneous, indicating increased unpredictability at the adsorbent-adsorbent interface. It also indicates the pHZpc of the negatively charged carbon surface at pH = 2.0. Two models of pseudo-first and pseudo-second order were included in the kinetic analysis. The outcomes indicate that a pseudo-second-order model with R2 > 0.9998 fits the experimental data better.

The Future of 2D Materials Production: Graphene and Borophene on larger scale

The production of graphene and borophene, two distinct materials with remarkable properties, is investigated through the manipulation of charged ions in a plasma environment. Plasma, characterized by ionized atoms or molecules, offers a unique setting where diverse chemical reactions can take place. This research focuses on utilizing this environment to create longer-chain graphene and carbon nanotubes by manipulating charged carbon ions. When positively and negatively charged carbon ions coexist within the plasma, they have the potential to interact and form bonds. This interaction results in the growth of extended carbon structures, particularly graphene. By carefully controlling plasma conditions such as temperature, pressure, and composition, scientists can guide the formation of longer-chain graphene and carbon nanotubes from these charged carbon ions. Similarly, the production of borophene, a material composed of boron atoms, also takes place in a plasma state. By introducing positively and negatively charged boron ions into the plasma, these ions interact and potentially form bonds, leading to the growth of extended borophene structures. This innovative approach unlocks the potential for tailored materials with enhanced property.

Graphene nanowalls formation investigated by Electron Energy Loss Spectroscopy

The properties of layered materials are significantly dependent on their lattice orientations. Thus, the growth of graphene nanowalls (GNWs) on Cu through PECVD has been increasingly studied, yet the underlying mechanisms remain unclear. In this study, we examined the GNWs/Cu interface and investigated the evolution of their microstructure using advanced Scanning transmission electron microscopy and Electron Energy Loss Spectroscopy (STEM-EELS). GNWs interface and initial root layers of comprise graphitic carbon with horizontal basal graphene (BG) planes that conform well to the catalyst surface. In the vertical section, the walls show a mix of graphitic and turbostratic carbon, while the latter becomes more noticeable close to the top edges of the GMWs film. Importantly, we identified growth process began with catalysis at Cu interface forming BG, followed by defect induction and bending at ‘coalescence points’ of neighboring BG, which act as nucleation sites for vertical growth. We reported that although classical thermal CVD mechanism initially dominates, growth of graphene later deviates a few nanometers from the interface to form GNWs. Nascent walls are no longer subjected to the catalytic action of Cu, and their development is dominated by the stitching of charged carbon species originating in the plasma with basal plane edges.

Hepatotoxicity evaluations of different surface charged carbon quantum dots in vivo and in vitro

Recently, carbon quantum dots (CQDs) have become popular because of their simple synthesis and potential applications. Although CQDs have high biocompatibility, their biotoxicity must be verified to reduce the possible risks associated with large-scale application. In this study, the hepatotoxicity of three CQD types, namely diammonium citrate (AC)-based (CQDs-AC), spermidine trihydrochloride (Spd)-based (CQDs-Spd), and AC- and Spd-based CQDs (CQDs-AC/Spd), were evaluated in vivo and in vitro. It was observed in vivo that CQDs-Spd and CQDs-AC/Spd, but not CQDs-AC, caused histopathological damage, including liver steatosis and mild mixed inflammatory cell infiltration; however, reduced liver function was only observed in CQD-Spd–treated mice. The in vitro results revealed that only CQDs-Spd significantly decreased the number of viable HepG2 cells (NADH depletion) and induced oxidative stress (heme oxygenase-1 activation) after 24 h of exposure, which promoted inflammatory factor secretion (NF-κB activation). Additionally, decreasing zonula occludens-2 and α1-antitrypsin protein expression in HepG2 cells suggested that CQD-Spd exposure increases the risk of liver diseases. Our results revealed that CQDs-Spd had greater hepatotoxic potential than CQDs-AC and CQDs-AC/Spd, which might be attributable to their high positive surface charge. Overall, the risk of CQD-induced hepatotoxic risk must be considered when applying positively charged CQDs.

Reconciling electrolyte donicity and polarity for lithium carbon fluoride batteries

For nonaqueous electrolytes designed for carbon fluoride batteries, a higher donicity is beneficial for stabilizing positively charged carbon atoms, while a moderate polarity is favorable for detaching negatively charged fluorine atoms.

Rapid targeting and imaging of mitochondria via carbon dots using an amino acid-based amphiphile as a carrier.

Green-fluorescent biocompatible carbon dots with a quantum yield of 40% were successfully synthesized through a solvothermal process and then they are comprehensively characterized. The carbon dots showed a negatively charged surface owing to the presence of carboxylic groups. This negative surface charge hinders the effective targeting and imaging of mitochondria. To address this limitation, a new approach is developed in this study. An amphiphile containing phenylalanine, with a positively charged polar head consisting of triphenylphosphine and a hydrophobic aliphatic tail, was designed, synthesized, purified, and characterized. This amphiphile formed spherical micelle-type nanostructures in an aqueous medium in the aggregated state. Although these nanoprobes lack inherent fluorescence, they exhibited the capability to image mitochondria when their spherical micelle-type nanostructures were decorated with negatively charged fluorescent nanocarbon dots in both cancerous (KB cells) and non-cancerous (CHO cells) cell lines. Notably, carbon dots without the amphiphile failed to penetrate the cell membrane as they exhibited significantly low emission inside the cell. This study extensively explored the cell entry mechanism of the hybrid nanoprobes. The photophysical changes and the interaction between the negatively charged carbon dots and the positively charged nanospheres of the amphiphile were also analyzed in this study.

A Nanoinhibitor Targeting cGAS-STING Pathway to Reverse the Homeostatic Imbalance of Inflammation in Psoriasis.

Psoriasis is a chronic skin inflammation characterized by dysregulated crosstalk between immune cells and keratinocytes. Here we show that the cyclic GMP-AMP synthase (cGAS)-stimulator of interferon genes (STING) pathway is a key regulator of psoriatic inflammation in a mouse model. Platinum-doped positively charged carbon dots (Pt-CDs) were designed to inhibit the cGAS-STING pathway. By inhibiting the cGAS-STING pathway with Pt-CDs, the secretion of proinflammatory cytokines in macrophages was reduced, and the proinflammatory cytokines-induced breakdown of immunological tolerance and overexpression of chemokines in keratinocytes was restored, which reversed the homeostatic imbalance through breaking these cytokines-mediated intercellular positive feedback loop. Topical Pt-CDs treatment exhibited therapeutic effects in imiquimod-induced psoriasis mice without noticeable toxicity. The reversal of elevated expression of STING, phosphorylated STING, and downstream genes within psoriatic lesions indicates that Pt-CDs effectively inhibit the cGAS-STING pathway. This work suggests a promising strategy for psoriasis treatment by targeting the cGAS-STING pathway with Pt-CDs nanoinhibitor to restore skin homeostatic balance.

Formation of vesicles between negatively charged carbon quantum dots and cationic surfactant cetylpyridinium chloride (CPC) due to oxidative photo induced electron transfer

The tuning of photo physical properties of highly emissive carbon quantum dots which was synthesized from citric acid in DMF medium through solvothermal method is investigated inside micelles formed by different types of surfactants like cationic surfactant cetylpyridinium chloride (CPC), cetrimonium bromide (CTAB), anionic surfactant sodium dodecyl sulfate (SDS) and neutral surfactant polyethylene glycol tert-octyl phenyl ether (TX100), polyoxoethylene lauryl ether (BRIJ-35). Interestingly, only CPC interacts with greater extent and formed co-assembly with negatively-charged carbon quantum dots (CQDs) whereas other surfactants like CTAB, SDS, TX100 and BRIJ-35 do not alter the fluorescence intensity extensively. This results in the formation of a non fluorescent vesicle. No phase separation was observed over the large concentration barrier of the CPC surfactant. However, no such vesicle formation takes place for another cationic surfactant CTAB excluding the role of only electrostatic interaction. The synthesized vesicle is characterized by various techniques including HRTEM, DLS. For the aqueous solution of CQDs having concentration of 0.5 mg/ml, addition of CPC leads to formation of different sized vesicles of size 40 nm to 100 nm. The driving force behind this formation of non-fluorescent vesicles is oxidative photo induced electron transfer which is revealed by the highest occupied molecular orbital (HOMO) –lowest unoccupied molecular orbital (LUMO) interaction between the donor (CQDs) and the acceptor (CPC). We trust such type vesicle can be a suitable alternative for drug carriers, biomarkers and other various applications also.

4-6 carbophene: A two-dimensional carbon material with Dirac cone and superior activity for electrochemical oxygen reduction reactions

The positive exploration of efficient and cost-effective electrocatalysts for the oxygen reduction reaction (ORR) is crucial for the sustainable development of energy conversion and storage technologies. Recently, a new type of two-dimensional (2D) carbon crystals, called 4-6 carbophene, has been successfully synthesized. It consists of a four-carbon ring and a six-carbon ring. In this work, we have discovered that 4-6 carbophene is a two-dimensional Dirac cone material through density-functional theory (DFT) calculations. Therefore, we further investigated the oxygen reduction reaction on 4-6 carbophene to understand its catalytic properties. The results demonstrate that on 4-6 carbophene, the ORR prefers a direct four-electron pathway. Under acidic conditions, the ORR overpotential of 4-6 carbophene is as low as 0.59 V, which is comparable to some metal benchmark catalysts, demonstrating that 4-6 carbophene is a metal-free ORR candidate catalyst. In addition, the richly charged carbon atoms on 4-6 carbophene exhibit remarkable charge transfer when binding to the adsorbed intermediates. This results in a strong binding strength. Thus, 4-6 carbophene has favorable ORR catalytic activity. This work not only provides promising low-cost catalysts in pure carbon materials for ORR, promoting the development of metal-free ORR catalysts, but also enhances the understanding of Dirac cone two-dimensional materials for applications in catalysis.

Chitosan-PEI passivated carbon dots for plasmid DNA and miRNA-153 delivery in cancer cells

These days carbon dots have been developed for multiple biomedical applications. In the current study, the transfection potential of synthesized carbon dots from single biopolymers such as chitosan, PEI-2kDa, and PEI-25kDa (CS-CDs, PEI2-CDs, and PEI25-CDs) and by combining two biopolymers (CP2-CDs and CP25-CDs) through a bottom-up approach have been investigated. The characterization studies revealed successful synthesis of fluorescent, positively charged carbon dots <20 nm in size. Synthesized carbon dots formed a stable complex with plasmid DNA (EGFP-N1) and miRNA-153 that protected DNA/miRNA from serum-induced degradation. In-vitro cytotoxicity analysis revealed minimal cytotoxicity in cancer cell lines (A549 and MDA-MB-231). In-vitro transfection of EGFP-N1 plasmid DNA with PEI2-CDs, PEI25-CDs and CP25-CDs demonstrated that these CDs could strongly transfect A549 and MDA-MB-231 cells. The highest EGFP-N1 plasmid transfection efficiency was observed with PEI2-CDs at a weight ratio of 32:1. PEI25-CDs polyplex showed maximum transfection at a weight ratio of 8:1 in A549 at a weight ratio of 16:1 in MDA-MB-231 cells. CP25-CDs exhibited the highest transfection at a weight ratio of 16:1 in both cell lines. The in-vitro transfection of target miRNA, i.e., miR-153 in A549 and MDA-MB-231 cells with PEI2-CDs, PEI25-CDs, and CP25-CDs suggested successful transfer of miR-153 into cells which induced significant cell death in both cell lines. Importantly, CS-CDs and CP2-CDs could be tolerated by cells up to 200 μg/mL concentration, while PEI2-CDs, PEI25-CDs, and CP25-CDs showed non-cytotoxic behavior at low concentrations (25 μg/mL). Together, these results suggest that a combination of carbon dots synthesized from chitosan and PEI (CP25-CDs) could be a novel vector for transfection nucleic acids that can be utilized in cancer therapy.

Self-cleaning and photodegradle PVDF separation membranes modified with self-assembled TiO2-g-CS/CNTs particle

This work obtained separation membranes with UV-cleaning performance by adding TiO2-g-CS/CNTs photocatalyst to the PVDF. The positively charged chitosan (CS) and negatively charged carboxylic carbon nanotube (CNTs-COOH) can be self-assembled into the bilayer structure on the surface of TiO2 particles through electrostatic attraction. The presence of many hydrophilic groups in CS and CNTs-COOH significantly improves the hydrophilicity of TiO2-g-CS/CNTs-PVDF membrane, and helps TiO2 to be uniformly dispersed on the upper surface. TiO2-g-CS/CNTs promote the change of pore structure and expand the flux of the modified membrane to 4.5 times that of pure PVDF. Zeta potential demonstrates that the TiO2-g-CS particles successfully attracted CNTs in the PVDF matrix, and the membrane surface was still positively charged. Thus, the combined effect of the positively charged TiO2-g-CS and the highly adsorbed CNTs enhanced the retention of the contaminants. More importantly, there is a charge transfer between the grafted CS and TiO2 interface to obtain a broader light absorption band. The excitation carriers provided by CNTs significantly contribute to the photocatalytic performance after transfer between TiO2 and CS; thus, TiO2-g-CS/CNTs-PVDF produces higher photocatalytic activity for dye molecules (degradation rate > 97 %).

Agglomeration Drives the Reversed Fractionation of Aqueous Carbonate and Bicarbonate at the Air-Water Interface.

In the course of our investigations of the adsorption of ions to the air-water interface, we previously reported the surprising result that doubly charged carbonate anions exhibit a stronger surface affinity than singly charged bicarbonate anions. In contrast to monovalent, weakly hydrated anions, which generally show enhanced concentrations in the interfacial region, multivalent (and strongly hydrated) anions are expected to show a much weaker surface propensity. In the present work, we use resonantly enhanced deep-UV second-harmonic generation spectroscopy to measure the Gibbs free energy of adsorption of both carbonate (CO32-) and bicarbonate (HCO3-) anions to the air-water interface. Contrasting the predictions of classical electrostatic theory and in support of our previous findings from X-ray photoelectron spectroscopy, we find that carbonate anions do indeed exhibit much stronger surface affinity than do the bicarbonate anions. Extensive computer simulations reveal that strong ion pairing of CO32- with the Na+ countercation in the interfacial region results in the formation of near-neutral agglomerate clusters, consistent with a theory of interfacial ion adsorption based on hydration free energy and capillary waves. Simulated X-ray photoelectron spectra predict a 1 eV shift in the carbonate spectra compared to that of bicarbonate, further confirming our experiments. These findings not only advance our fundamental understanding of ion adsorption chemistry but also impact important practical processes such as ocean acidification, sea-spray aerosol chemistry, and mammalian respiration physiology.

Unleashing the power of capacitive deionization: Advancing ion removal with biomass-derived porous carbonaceous electrodes

Capacitive deionization (CDI) is a promising electrochemical technique for the removal and recycling of ions from micro-polluted wastewater but is still hindered by the co-ion expulsion effect and anode oxidation. In this study, these issues are addressed through optimization of both materials and electrochemical systems. A diverse set of porous carbons are prepared using biomass as a precursor and KOH as the activation agent. It is found that direct carbonization and/or KOH activation induce a negative surface charge, whereas intense nitrogen-doping results in an inverse surface charge for all biomass-derived carbons, characterized by the potential of zero charge (Epzc). Density functional theory calculations suggest that the carboxyl group and quaternary N contribute most among other functional groups to the negative and positive charges, respectively. A Epzc-matching asymmetric CDI system is constructed employing negatively charged and positively charged carbons as the cathode and anode, respectively. This configuration, coupled with precise optimization of the cathode-to-anode mass ratio (m-/m+), unlocks a high adsorption capacity of 17.2 mg g−1 for NaCl, surpassing the symmetric system by 84.7 %. Further fine tuning of the m-/m+ ratio results in a removal capacity of 167.4 mg g−1 for Cu2+ ions, which is the highest reported for carbonaceous materials to date.

Negatively Charged Hydrophobic Carbon Nano-Onion Interfacial Layer Enabling High-Rate and Ultralong-Life Zn-Based Energy Storage.

Zn-based electrochemical energy storage (EES) systems are attracting more attention, whereas their large-scale application is restricted by the dendrite and parasitic reaction-caused unstable Zn anodes. Herein, a negatively charged hydrophobic carbon nano-onion (CNO) interfacial layer is proposed to realize ultrastable and high-rate Zn anodes, enabling high-performance Zn-based EES. For the CNO interfacial layer, its hydrophobicity not only blocks active water but also reduces the Zn2+ desolvation barrier, and meanwhile, the negatively-charged CNO nanoparticles adsorb Zn2+ and repel SO4 2- to homogenize Zn2+ flux, accelerate Zn2+ desolvation and suppress the self-corrosion of Zn anodes. Besides, the conductive CNO interfacial layer increases the surface area for the Zn deposition to reduce local current density. Consequently, under the modulation of the CNO interfacial layer, Zn plating/stripping exhibits impressive reversibility with an average Coulombic efficiency of 99.4% over 800 cycles, and Zn anodes present significantly enhanced electrochemical stability and rate performance, whose operation lifetime exceeds 2000h at 1mAcm-2 and 350h even at 10mAcm-2 . Moreover, high-rate and ultralong-life Zn-ion hybrid supercapacitors are achieved with the CNO interfacial layer-modulated Zn anode and activated CNO cathode. This work provides new thinking in regulating the Zn deposition interface to realize high-performance Zn-based EES.