N-doped Cu2O with the tunable Cu0 and Cu+ sites for selective CO2 electrochemical reduction to ethylene.

The electrochemical carbon dioxide reduction reaction (CO2RR) to high value-added fuels or chemicals driven by the renewable energy is promising to alleviate global warming. However, the selective CO2 reduction to C2 products remains challenge. Cu-based catalyst with the specific Cu0 and Cu+ sites is important to generate C2 products. This work used nitrogen (N) to tune amounts of Cu0 and Cu+ sites in Cu2O catalysts and improve C2-product conversion. The controllable Cu0/Cu+ ratio of Cu2O catalyst from 0.16 to 15.19 was achieved by adjusting the N doping amount using NH3/Ar plasma treatment. The major theme of this work was clarifying a volcano curve of the ethylene Faraday efficiency as a function of the Cu0/Cu+ ratio. The optimal Cu0/Cu+ ratio was determined as 0.43 for selective electroreduction CO2 to ethylene. X-ray spectroscopy and density functional theory (DFT) calculations were employed to elucidate that the strong interaction between N and Cu increased the binding energy of NCu bond and stabilize Cu+, resulting in a 92.3% reduction in the potential energy change for *CO-*CO dimerization. This study is inspiring in designing high performance electrocatalysts for CO2 conversion.

Optimization of nitrogen-doped sludge char preparation and mechanism study for catalytic oxidation of NO at room temperature.

Catalytic oxidation of NO at room temperature was carried out over nitrogen (N)-doped sludge char (SC) prepared from pyrolysis of municipal sewage sludge, and urea was adopted as nitrogen source. The effects of different N-doping methods (one-step and two-step method), dried sludge (DS)/urea mass ratios (5:1, 4:1, 3:1, 2:1, and 1:1), SC preparation procedures (pyrolysis only, pyrolysis with acid washing, and pyrolysis with KOH activation and acid washing), and different pyrolysis temperatures (500, 600, 700, and 800°C) on the catalytic oxidation of NO were compared to optimize the procedure for SC preparation. The results indicated that N-doping could obviously promote the catalytic performance of SC. The one-step method with simultaneous sludge pyrolysis (at 700°C), KOH activation, and N-doping (DS/urea of 3:1) was the optimal procedure for preparing the N-doped SC with the NO conversion rate of 54.7%, whereas the optimal NO conversion rate of SC without N-doping was only 47.3%. Urea worked both as carbon and nitrogen source, which could increase about 2.9%-16.5% of carbon and 24.8%-42.7% of nitrogen content in SC pyrolyzed at 700°C. N-doping significantly promoted microporosity of SC. The optimal N-doped SC showed specific surface areas of 571.38 m2/g, much higher than 374.34 m2/g of the optimal SC without N-doping. In addition, N-doping also increased amorphousness and surface basicity of SC through the formation of N-containing groups. Finally, three reaction paths, i.e. microporous reactor, active sites, and basic site control path, were proposed to explain the mechanism of N-doping on promoting the catalytic performance of NO.

Precise Regulation Strategy for Fluorescence Wavelength of Aggregation-Induced Emission Carbon Dots.

Aggregation-induced emission (AIE) carbon dot (CDs) in solid state with tunable multicolor emissions have sparked significant interest in multidimensional anti-counterfeiting. However, the realization of solid-state fluorescence (SSF) by AIE effect and the regulation of fluorescence wavelength in solid state is a great challenge. In order to solve this dilemma, the AIE method to prepare multi-color solid-state CDs with fluorescence wavelengths ranging from bright blue to red emission is employed. Specifically, by using thiosalicylic acid and carbonyl hydrazine as precursors, the fluorescence wavelength can be accurately adjusted by varying the reaction temperature from 150 to 230 °C or changing the molar ratio of the precursors from 1:1 to 1:2. Structural analysis and theoretical calculations consistently indicate that increasing the sp2 domains or doping with graphite nitrogen both cause a redshift in the fluorescence wavelength of CDs in the solid state. Moreover, with the multi-dimensional and adjustable fluorescence wavelength, the application of AIE CDs in the fields of multi-anti-counterfeiting encryption, ink printing, and screen printing is demonstrated. All in all, this work opens up a new way for preparing solid-state multi-color CDs using AIE effect, and further proposes an innovative strategy for controlling fluorescence wavelengths.

Electrocatalysis of Co/CoxOy nanofilms supported by synchronously nitrogen-doped Ketjenblack carbon towards oxygen reduction reaction.

Developing a highly active and stable non-precious metal catalyst for oxygen reduction reaction (ORR) is of great practical significance for advancing fuel cell technology. In this work, a continuous two-step hydrothermal reaction followed by high temperature pyrolysis were employed to achieve in situ N-doping preferentially into Ketjenblack carbon (KB-N) and composite of KB-N and Co/CoxOy nanofilms (Co/CoxOy-NFs) as Co/CoxOy-NFs@KB-N. The N-doped state strongly affects the ORR activity of catalyst. All prepared Co/CoxOy-NFs@KB-N catalysts exhibit observably improved ORR activity compared with the basal KB-N and N-doped Co/CoxOy-NFs, in which the optimal Co/CoxOy-NFs@KB-N catalyst demonstrate the positive Eonset (0.864 V) and E1/2 (0.788 V) vs. RHE, the low Tafel slope (69.27 mV dec-1), implying quick ORR kinetics. And, the Co/CoxOy-NFs@KB-N catalyst exhibits highly electrochemical durability. The KB-N substrate can purify Co valence in CoO component, promote amorphization of CoO crystalline structure and enhance the interaction between Co/CoxOy-NFs and KB-N in Co/CoxOy-NFs@KB-N catalyst. Thus electronic effect, structural effect and synergistic effect can strengthen O2 adsorption, provide enough adsorbed sites and accelerate electron transfer, resulting in prominent ORR performance of Co/CoxOy-NFs@KB-N catalyst.

Green Protocol for the Synthesis of Luminescent Carbon Nanodots Derived from Murraya Koenigii Leaves and Urea: Enhancing Photoluminescence for Advanced Bioimaging.

We have synthesized Murraya Koenigii leaves powder-derived carbon nanodots (CNDs) by hydrothermal method. A tribute to our commitment to environmental sustainability is the unique composition of our CNDs, which are made entirely of natural carbon sources and a green solvent, water. Our further efforts to improve performance led us to start making nitrogen-doped CNDs. By using urea as a non-toxic source of nitrogen, we observed a substantial increase in fluorescence intensity, extending the usefulness and potential of these nanomaterials. We investigated the optical properties using UV-Vis and fluorescence spectroscopy. The other parameters, like structural and size-shape morphology, were analyzed using FTIR, XRD, and HR-TEM, respectively. The fluorescence spectroscopy demonstrated their capability to exhibit wavelength-dependent photoluminescence (PL), highlighting the potential of these CNDs for cell bioimaging applications. The fluorescence properties affirm their suitability for biomedical applications, as they do not involve any inherent risk to cells.

Unraveling the Ionic Storage Mechanism of Flexible Nitrogen-Doped MXene Films for High-Performance Aqueous Hybrid Supercapacitors.

2D MXene nanomaterials have excellent potential for application in novel electrochemical energy storage technologies such as supercapacitors and batteries, but the existing pure MXene is difficult to meet the practical needs. Although the electrochemical properties of modified MXene have been improved, the unclear ion storage mechanism still hinders the development of MXene-based electrode materials. Herein, the study develops flexible self-supported nitrogen-doped Ti3C2 (Py-Ti3C2) films by the highly mobile, high nitrogen content, oxygen-free pyridine-assisted solvothermal method, and then deeply investigates the energy storage mechanism of hybrid supercapacitors in four aqueous electrolytes (H2SO4, Li2SO4, Na2SO4, and MgSO4). The experimental results suggest that the Py-Ti3C2 film electrode exhibits a pseudocapacitance-dominated energy storage mechanism. Particularly, the specific capacity of the Py-Ti3C2 in 1 M H2SO4 (506 F g-1 at 0.1 A g-1) is 4-5 times higher than other electrolytes (≈110 F g-1), which could be attributed to the substantially higher ionic diffusion coefficient of H+ than those of Li+, Na+, Mg2+ with small ionic size, high ionic conductivity, and fast pseudocapacitance response. Theoretical analysis further confirms that Py-Ti3C2 has strengthened conductivity and electrical double-layer capacitance performance. Meanwhile, it has lower free energy for protonation and deprotonation of functional groups, which gives excellent pseudocapacitance performance.

Tangerine peel-derived nitrogen-doped carbon dots incorporated chitosan/pullulan-based active packaging film for bread packaging.

Citrus peel waste carbon dots based on nitrogen-doped (N-TanCD) were developed by a hydrothermal strategy to deliver active packaging fillers and characterized by transmission electron microscopy, photoluminescence, and Fourier transform infrared analyses. The addition of N-TanCD into chitosan-pululan (CS/Pul@N-TanCD) polymer blend amplified the tensile strength of the composite film by 22.8 %, whereas the antioxidant activities against DPPH and ABTS reached 62.7 % and 91.6 %, respectively. The proposed film showed blocked 98.8 % of UV-A and 100 % of UV-B without affecting the film's transparency. The CS/Pul@N-TanCD film lowered the contamination of L. monocytogenes and E. coli by more than 4 and 5 log CFU/mL, respectively. Sliced bread was packaged using CS/Pul-based films and stored for 12 days at 50 % relative humidity and 25 °C to investigate changes in the quality of the bread. It was found that bread packaged with CS/Pul film integrated with N-TanCD maintained excellent bread quality relating to appearance, moisture content, hardness, weight loss, and total viable bacterial count.

Tailoring tea residue-derived nitrogen-doped activated carbon for CO2 adsorption: influence of activation temperature and activating agents.

Embracing CO2 mitigation strategies, such as state-of-the-art CO2 capture technologies, is essential for effectively reducing atmospheric carbon levels and advancing global efforts toward a more sustainable future. In this context, adsorption sequestering techniques utilising carbon materials have emerged as promising candidates for CO2 capture. These materials have been extensively researched with a range of tuning methods to optimise their physicochemical features. In this study, an alteration of the N-doped activated carbon was successfully performed, utilizing tea residue as the carbon precursor and ammonia as the nitrogen source, facilitated through an impregnation procedure. With the objective of discovering the effect of diverse activation parameters on prepared adsorbent physicochemical properties, several selections of activating agents (AA) were investigated: KOH, H3PO4, ZnCl2, and NaOH, together with broad thermal activation temperature from 873 to 1173 K. The best-performed adsorbents from the respective AC group were subjected to several characterisation analyses and found to the enhanced structural features, heteroatom doped-rich surface (i.e. N and O); together with AA-induced metal/mineral functionalization, the NaOH-used AC (NAC-N-1173) was the optimum-performed adsorbent with a promising 4.12 mmol/g CO2 uptake capacity, higher than other prepared adsorbent including N-doped tea residue-derived char and commercialized AC with 175 and 325% higher, respectively.

Recent Advances in Developing High-Performance Anode for Potassium-Ion Batteries based on Nitrogen-Doped Carbon Materials.

Owing to the low potential (vs K/K+), good cycling stability, and sustainability, carbon-based materials stand out as one of the optimal anode materials for potassium-ion batteries (PIBs). However, achieving high-rate performance and excellent capacity with the current carbon-based materials is challenging because of the sluggish reaction kinetics and the low capacity of carbon-based anodes. The doping of nitrogen proves to be an effective way to improve the rate performance and capacity of carbon-based materials as PIB anode. However, a review article is lacking in systematically summarizing the features and functions of nitrogen doping types. In this sense, it is necessary to provide a fundamental understanding of doped nitrogen types in nitrogen-doped(N-doped) carbon materials. The types, functions, and applications of nitrogen-doped carbon-based materials are overviewed in this review. Then, the recent advances in the synthesis, properties, and applications of N-doped carbon as both active and modification materials for PIBs anode are summarized. Finally, doped nitrogen's main features and functions are concluded, and critical perspectives for future research in this field are outlined.

A Universal Synthesis of Single-Atom Catalysts via Operando Bond Formation Driven by Electricity.

Single-atom catalysts (SACs), featuring highly uniform active sites, tunable coordination environments, and synergistic effects with support, have emerged as one of the most efficient catalysts for various reactions, particularly for electrochemical CO2 reduction (ECR). However, the scalability of SACs is restricted due to the limited choice of available support and problems that emerge when preparing SACs by thermal deposition. Here, an in situ reconstruction method for preparing SACs is developed with a variety of atomic sites, including nickel, cadmium, cobalt, and magnesium. Driven by electricity, different oxygen-containing metal precursors, such as MOF-74 and metal oxides, are directly atomized onto nitrogen-doped carbon (NC) supports, yielding SACs with variable metal active sites and coordination structures. The electrochemical force facilitates the in situ generation of bonds between the metal and the supports without the need for additional complex steps. A series of MNxOy (M denotes metal) SACs on NC have been synthesized and utilized for ECR. Among these, NiNxOy SACs using Ni-MOF-74 as a metal precursor exhibit excellent ECR performance. This universal and general SAC synthesis strategy at room temperature is simpler than most reported synthesis methods to date, providing practical guidance for the design of the next generation of high-performance SACs.

π-Extension of a Multiple Resonance Core: Double Helical and Heptagon-Embedded Nanographenes.

Multiple resonance (MR) boron-nitrogen doped polycyclic aromatic hydrocarbons (BN-PAHs) have shown compelling thermally activated delayed fluorescence (TADF), surpassing those of their hydrocarbon analogues. However, the structural variety of π-extended BN-PAHs remains narrow. In this study, we synthesized three double helical BN-doped nanographenes (BN-NGs), 2 a-2 c, and three heptagon-embedded BN-NGs, 1 a-1 c, by π-extension of the MR core. During the formation of 2 a, a nanographene with one heptagon (1 a) was obtained, whereas further dehydrocyclization of the [6]helicene units within 2 b and 2 c led to heptagon structures, yielding other two BN-NGs containing double heptagons (1 b and 1 c). These BN-NGs (2 a-2 c and 1 a-1 c) showed pronounced redshifts of 100-190 nm compared to the parent MR core, while preserving the TADF characteristics and prolonging the delayed fluorescence lifetime to the millisecond level. Furthermore, the integration of a heptagon ring into 1 a-1 c expanded the conjugation, reduced the oxidation potentials, and yielded a more flexible framework compared to those of 2 a-2 c. The enantiomers of 2 a-2 c, 1 a, and 1 c were resolved and their chiroptical properties were studied. Notably, 1 a and 1 c exhibited increased chiroptical dissymmetry factors.

Formation, Structure, Electronic, and Transport Properties of Nitrogen Defects in Graphene and Carbon Nanotubes.

The substitutional doping of nitrogen is an efficient way to modulate the electronic properties of graphene and carbon nanotubes (CNTs). Therefore, it could enhance their physical and chemical properties as well as offer potential applications. This paper provides an overview of the experimental and theoretical investigations regarding nitrogen-doped graphene and CNTs. The formation of various nitrogen defects in nitrogen-doped graphene and CNTs, which are identified by several observations, is reviewed. The electronic properties and transport characteristics for nitrogen-doped graphene and CNTs are also reviewed for the development of high-performance electronic device applications.

Surface-anchored N-based functional groups driven photoactivity of SrTiO3.

Surface modification, including the anchoring of functional groups is a popular method to increase the photocatalytic activity of semiconductor photocatalysts. These species can trap excited electrons, thus prolonging the life of the charge carriers. N-containing functional groups are suitable for this purpose due to their high electron density. Here, we report a facile synthesis method for preparing interfacial N-based functional groups-modified and nitrogen-doped SrTiO3 photocatalysts. Among the modified samples (with 0.42-11.14 at.% nominal nitrogen content), the one with 7.71 at.% nitrogen showed 6.4 times higher photooxidation efficiency for phenol and 2.2 times better photoreduction efficiency for CO2 conversion than the unmodified SrTiO3 reference. Characterization results showed that using a low amount of nitrogen source resulted in low but measurable nitrogen doping, which did not significantly affect the photocatalytic activity. The formation of surface amine groups was significant even at lower initial nitrogen concentrations, while higher amounts of nitrogen source gradually resulted in the incorporation of nitrogen in higher amounts. Surface amine groups decreased the recombination of charge carriers, resulting in increased photocatalytic activity.

Supermolecule-Opitimized Defect Engineering of Rich Nitrogen-Doped Porous Carbons for Advanced Zinc-Ion Hybrid Capacitors.

Pitch-based porous carbons with adjustable surface chemical property and controllable pore structure are regarded as promising cathode materials for aqueous zinc-ion hybrid capacitors (ZIHCs), while its disordered carbon matrix and microstructure as well as insufficient surface defects often result in low Zn2+-storage capacity and poor rate capability of ZIHCs. Herein, a synergetic strategy of self-assembled supermolecule and enriched defective carbon engineering was developed to achieve ultrahigh edge-nitrogen doping for ZIHCs. The crystallite defects and surface structure of porous carbon could be effectively achieved through grafting electronegative oxygen-containing small molecules and high-level nitrogen-containing functional groups between modified polycyclic aromatic hydrocarbon and supermolecule framework. The optimized three-dimensional carbon structure delivered high capacity of 218 mAh g-1 at 0.2 A g-1, fast charge/discharge capability, enhanced energy density (165.4 Wh kg-1) and superior cycling stability (95 % retention after 10000 cycles as cathode of ZIHCs). This provided new insight into the controllable synthesis of carbon cathodes for ZIHCs and expects to prepare functional porous carbon by supermolecules and special precursors.

Combining Nitrogen Doping and Vacancies for Tunable Resonant States in Graphite.

We investigate the combination of nitrogen doping and vacancies in highly ordered pyrolytic graphite (HOPG), to engineer defect sites with adjustable electronic properties. We combine scanning tunneling microscopy and spectroscopy and density functional theory calculations to reveal the synergistic effects of nitrogen and vacancies in HOPG. Our findings reveal a remarkable shift of the vacancy-induced resonance peak from an unoccupied state in pristine HOPG to an occupied state in nitrogen-doped HOPG. This shift directly correlates with the shift of the charge neutrality point resulting from the n-doping induced by substitutional nitrogen. These results open new avenues for defect engineering in graphite or graphene and achieving novel functionalities for chemical activity or electronic properties.

Corrosion-Resistant Ultrathin Cu Film Deposited on N-Doped Amorphous Carbon Film Substrate and Its Use for Crumpleable Circuit Board.

Copper (Cu) is widely used as an industrial electrode due to its high electrical conductivity, mechanical properties, and cost-effectiveness. However, Cu is susceptible to corrosion, which degrades device performance over time. Although various methods (alloying, physical passivation, surface treatment, etc.) are introduced to address the corrosion issue, they can cause decreased conductivity or vertical insulation. Here, using the nitrogen-doped amorphous carbon (a-C:N) thin film is proposed as a substrate on which Cu is directly deposited. This simple method significantly inhibits corrosion of ultrathin Cu (<20 nm) films in humid conditions, enabling the fabrication of ultrathin electronic circuit boards without corrosion under ambient conditions. This study investigates the origin of corrosion resistance through comprehensive microscopic/spectroscopic characterizations and density-functional theory (DFT) calculations: i) diffusion of Cu atoms into the a-C:N driven by stable C-Cu-N bond formation, ii) diffusion of N atoms from the a-C:N to the Cu layer heading the top surface, which is the thermodynamically preferred location for N, and iii) the doped N atoms in Cu layer suppress the inclusion of O into the Cu lattice. By leveraging the ultrathinness and deformability of the circuit board, a transparent electrode and a crumpleable LED lighting device are demonstrated.

Activated persulfate for efficient bisphenol A degradation via nitrogen-doped Fe/Mn bimetallic biochar.

To achieve the purpose of treating waste by waste, in this study, a nitrogen-doped Fe/Mn bimetallic biochar material (FeMn@N-BC) was prepared from chicken manure for persulfate activation to degrade Bisphenol A (BPA). The FeMn@N-BC was characterized by scanning electron microscopy (SEM), X-ray diffract meter (XRD), fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectrometer (XPS) and found that N doping can form larger specific surface area. Catalytic degradation experiments showed that Fe/Mn bimetal doping not only accelerated the electron cycling rate on the catalyst surface, but also makes the biochar magnetic and easy to separate, thus reducing environmental pollution. Comparative experiments was concluded that the highest degradation efficiency of BPA was achieved when the mass ratios of urea and chicken manure, Fe/Mn were 3:1 and 2:1, respectively, and the pyrolysis temperature was 800 °C, which can almost degrade all the BPA in 60 min. FeMn@N-BC/PS system with high catalytic efficiency and low consumables is promising for reuse of waste resources and the remediation of wastewater.

Carbon quantum dots from carbohydrate-rich residue of birch obtained following lignin-first strategy.

Carbon quantum dots (CQDs) were successfully synthesized from carbohydrate-rich residue of birch obtained following the lignin-first strategy. The optical and physicochemical properties of the CQDs were studied, along with their potential for photocatalytic pollutant degradation. By combining solvothermal and chemical oxidation methods, the product yield of CQDs from carbohydrate-rich residue reached 8.1 wt%. Doping nitrogen enhances the graphitization of CQDs and introduces abundant amino groups to the surface, thereby boosted the quantum yield significantly from 8.9 % to 18.7 %-19.3 %. Nitrogen-doped CQDs exhibited efficient photocatalytic degradation of methylene blue, reaching 37 % within 60 min, with a kinetic degradation rate of 0.00725 min-1. This study demonstrates that carbohydrate-rich residue obtained from lignin-first strategy are ideal precursors for synthesizing CQD with high mass yield and quantum yield by combining solvothermal treatment and chemical oxidation methods, offering a novel approach for the utilization of whole biomass components following the lignin-first strategy.

Tunable Doping Strategy for Few-Layer MoS2 Field-Effect Transistors via NH3 Plasma Treatment.

Molybdenum disulfide (MoS2) is a promising candidate for next-generation transistor channel materials, boasting outstanding electrical properties and ultrathin structure. Conventional ion implantation processes are unsuitable for atomically thin two-dimensional (2D) materials, necessitating nondestructive doping methods. We proposed a novel approach: tunable n-type doping through sulfur vacancies (VS) and p-type doping by nitrogen substitution in MoS2, controlled by the duration of NH3 plasma treatment. Our results reveal that NH3 plasma exposure of 20 s increases the 2D sheet carrier density (n2D) in MoS2 field-effect transistors (FETs) by +4.92 × 1011 cm-2 at a gate bias of 0 V, attributable to sulfur vacancy generation. Conversely, treatment of 40 s reduces n2D by -3.71 × 1011 cm-2 due to increased nitrogen doping. X-ray photoelectron spectroscopy, Raman spectroscopy, and photoluminescence analyses corroborate these electrical characterization results, indicating successful n- and p-type doping. Temperature-dependent measurements show that the Schottky barrier height at the metal-semiconductor contact decreases by -31 meV under n-type conditions and increases by +37 meV for p-type doping. This study highlights NH3 plasma treatment as a viable doping method for 2D materials in electronic and optoelectronic device engineering.

Nitrogen-Doped Porous Carbons Derived from Peanut Shells as Efficient Electrodes for High-Performance Supercapacitors.

The doping of porous carbon materials with nitrogen is an effective approach to enhance the electrochemical performance of electrode materials. In this study, nitrogen-doped porous carbon derived from peanut shells was prepared as an electrode for supercapacitors. Melamine, urea, urea phosphate, and ammonium dihydrogen phosphate were employed as different nitrogen dopants. The optimized electrode material PA-1-1 prepared by peanut shells, with ammonium dihydrogen phosphate as a nitrogen dopant, exhibited a N content of 3.11% and a specific surface area of 602.7 m2/g. In 6 M KOH, the PA-1-1 electrode delivered a high specific capacitance of 208.3 F/g at a current density of 1 A/g. Furthermore, the PA-1-1 electrode demonstrated an excellent rate performance with a specific capacitance of 170.0 F/g (retention rate of 81.6%) maintained at 20 A/g. It delivered a capacitance of PA-1-1 with a specific capacitance retention of 98.8% at 20 A/g after 5000 cycles, indicating excellent cycling stability. The PA-1-1//PA-1-1 symmetric supercapacitor exhibited an energy density of 17.7 Wh/kg at a power density of 2467.0 W/kg. This work not only presents attractive N-doped porous carbon materials for supercapacitors but also offers a novel insight into the rational design of biochar carbon derived from waste peelings.