Rational Design of Quasi-1D Multicore-Shell MnSe@N-Doped Carbon Nanorods as High-Performance Anode Material for Sodium-Ion Batteries.

Sodium-ion batteries (SIBs) are considered one of the promising candidates for energy storage devices due to the low cost and low redox potential of sodium. However, their implementation is hindered by sluggish kinetics and rapid capacity decay caused by inferior conductivity, lattice deterioration, and volume changes of conversion-type anode materials. Herein, we report the design of a multicore-shell anode material based on manganese selenide (MnSe) nanoparticle encapsulated N-doped carbon (MnSe@NC) nanorods. Benefiting from the conductive multicore-shell structure, the MnSe@NC anodes displayed prominent rate capability (152.7 mA h g-1 at 5 A g-1) and long lifespan (132.7 mA h g-1 after 2000 cycles at 5 A g-1), verifying the essence of reasonable anode construction for high-performance SIBs. Systematic in situ microscopic and spectroscopic methods revealed a highly reversible conversion reaction mechanism of MnSe@NC. Our study proposes a promising route toward developing advanced transition metal selenide anodes and comprehending electrochemical reaction mechanisms toward high-performance SIBs.

Regulating RuxMoy Nanoalloys Anchored on Porous Nitrogen-Doped Carbon via Domain-Confined Etching Strategy for Neutral Efficient Ammonia Electrosynthesis.

Neutral electrochemical nitrate (NO3-) reduction to ammonia involves sluggish and complex kinetics, so developing efficient electrocatalysts at low potential remains challenging. Here, we report a domain-confined etching strategy to construct RuxMoy nanoalloys on porous nitrogen-doped carbon by optimizing the Ru-to-Mo ratio, achieving efficient neutral NH3 electrosynthesis. Combining in situ spectroscopy and theoretical simulations demonstrated a rational synergic effect between Ru and Mo in nanoalloys that reinforces *H adsorption and lowers the energy barrier of NO3- hydrodeoxygenation for NH3 production. The resultant Ru5Mo5-NC surpasses 92.8% for NH3 selectivity at the potential range from -0.25 to -0.45 V vs RHE under neutral electrolyte, particularly achieving a high NH3 selectivity of 98.3% and a corresponding yield rate of 1.3 mg h-1 mgcat-1 at -0.4 V vs RHE. This work provides a synergic strategy that sheds light on a new avenue for developing efficient multicomponent heterogeneous catalysts.

Nitrogen-Doped Carbon Dots Modified Fe-Co Sulfide Nanosheets as High-Efficiency Electrocatalysts toward Oxygen Evolution Reaction.

Developing high-efficiency and stable oxygen evolution reaction (OER) electrocatalysts is an imperative requirement to produce green and clean hydrogen energy. In this work, the FeCoSy /NCDs composite with nitrogen-doped carbon dots (NCDs) modified Fe-Co sulfide (FeCoSy ) nanosheets is prepared by using a facile and mild one-pot solvothermal method. Benefiting from the low crystallinity and the synergistic effect between FeCoSy and NCDs, the optimal FeCoSy /NCDs-3 composite exhibits an overpotential of only 284 mV at 10 mA cm-2 , a small Tafel value of 52.1 mV dec-1 , and excellent electrochemical durability in alkaline solution. Remarkably, unlike ordinary metal sulfide electrocatalysts, the morphology, components, and structure of the FeCoSy /NCDs composite can be well retained after OER test. The NCDs modified FeCoSy composite with excellent electrocatalytic performance provides an effective approach to boost metal sulfide electrocatalysts for practical application.

Constructing Gold Single-Atom Catalysts on Hierarchical Nitrogen-Doped Carbon Nanocages for Carbon Dioxide Electroreduction to Syngas.

Precious-metal single-atom catalysts (SACs), featured by high metal utilization and unique coordination structure for catalysis, demonstrate distinctive performances in the fields of heterogeneous and electrochemical catalysis. Herein, gold SACs are constructed on hierarchical nitrogen-doped carbon nanocages (hNCNC) via a simple impregnation-drying process and first exploited for electrocatalytic carbon dioxide reduction reaction (CO2RR) to produce syngas. The as-constructed Au SAC exhibits the high mass activity of 3319 A g-1 Au at -1.0 V (vs reversible hydrogen electrode, RHE), much superior to the Au nanoparticles supported on hNCNC. The ratio of H2/CO can be conveniently regulated in the range of 0.4-2.2 by changing the applied potential. Theoretical study indicates such a potential-dependent H2/CO ratio is attributed to the different responses of HER and CO2RR on Au single-atom sites coordinating with one N atom at the edges of micropores across the nanocage shells. The catalytic mechanism of the Au active sites is associated with the smooth switch between twofold and fourfold coordination during CO2RR, which much decreases the free energy changes of the rate-determining steps and promotes the reaction activity.

Two-Step Catalytic Against Polysulfide Shuttling to Enhance Redox Conversion for Advanced Lithium-Sulfur Batteries.

The development of lithium-sulfur batteries is seriously hindered by the shuttle effect of lithium polysulfides (LiPSs) and the low electrical conductivity of sulfur. To solve these problems, efficient catalysts can be used to improve the conversion rate of LiPSs and the conductivity of sulfur cathode. Herein, annealed melamine foam supported MoSe2 (NCF@MoSe2) is used as interlayer and the MoSe2/MoP heterojunction obtained by phosphating MoSe2 is further used as the catalyst material for metal fusion with a sulfur element. The interlayer can not only improve the electrical conductivity and effectively adsorb and catalyze LiPSs, but more importantly, the MoSe2/MoP heterojunction can also effectively adsorb and catalyze LiPSs, so that the batteries have a dual inhibition shuttling effect strategy. Furthermore, the rapid anchor-diffusion transition of LiPSs, and the suppression of shuttling effects by catalyst materials are elucidated using theoretical calculations and in situ Raman spectroscopy. The two-step catalytic strategy exhibits a high reversibility of 983 mAh g-1 after 200 cycles at 0.5 C and a high-rate capacity of 889 mAh g-1 at 5 C. This work provides a feasible solution for the rational design of interlayer and heterojunction materials and is also conducive to the development of more advanced Li-S batteries.

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

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

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.

Revealing Energy Density in Porous Carbon Supercapacitors Using Hydroquinone Sulfonic Acid as Cathodic and Alizarin Red S as Anodic Redox Electrolytes.

Exploration of innovative strategies aiming to boost energy densities of supercapacitors without sacrificing the power density and long-term stability is of great importance. Herein, highly porous nitrogen-doped carbon spheres (NPCS) are decorated onto the graphite sheets (GSs) through a hydrothermal route, followed by a chemical activation. The capacitive performance of the NPCS is then enhanced by hydroquinone sulfonic acid (HSQA) incorporation in both cathodic electrolyte and electrode materials. Later, NPCS are decorated with polypyrrole (PPY), in which HSQA takes a versatile role as conjugated polymer dopant and cathodic redox additive. The capacitive performance of the negative electrodes is enhanced by incorporating of alizarin red S (ARS) as anodic redox additive. Finally, PPY(HQSA)@NPCS-GS//NPCS-GS asymmetric supercapacitor is assembled and tested in dual redox electrolyte system containing HQSA-cathodic and ARS-anodic electrolytes. This device delivers a remarkable energy density of 60.37 Wh kg-1, which is close or even better than lead acid batteries. Thus, the present work provides a novel pathway to develop high energy supercapacitors using redox active electrolytes for next-generation energy storage applications.

Engineering Non-precious Trifunctional Cobalt-Based Electrocatalysts for Industrial Water Splitting and Ultra-High-Temperature Flexible Zinc-Air Battery.

Developing efficient, robust, and cost-effective trifunctional catalysts for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) at high current density and high temperature is crucial for water splitting at industry-level conditions and ultra-high-temperature Zinc-air battery (ZAB). Herein, cobalt nanoparticles well-integrated with nitrogen-doped porous carbon leaves (Co@NPCL) by direct annealing of core-shell bimetallic zeolite imidazolate frameworks is synthesized. Benefiting from the homogeneous distribution of metallic Co nanoparticles, the conductive porous carbon, and the doped N species, the as-fabricated Co@NPCL catalysts exhibit outstanding trifunctional performances with low overpotentials at 10 mA cm-2 for HER (87 mV) and OER (276 mV), long-lasting lifetime of over 2000 h, and a high half-wave potential of 0.86 V versus RHE for ORR. Meanwhile, the Co@NPCL catalyst can serve as both cathode and anode for water splitting at industrial conduction, and exhibit a stable cell voltage of 1.87 V to deliver a constant catalytic current of 500 mA cm-2 over 60 h. Moreover, the excellent trifunctional activity of Co@NPCL enables the flexible ZAB to operate efficiently at ultra-high temperature of 70 °C, delivering 162 mW cm-2 peaks power density and an impressive stability for 4500 min at 2 mA cm-2.

Nitrogen-Doped Carbon and Metal-Nitrogen-Carbon Materials as Cathode Hosts for Li-S Batteries: Experimental Study and Mechanism Analysis.

Both nitrogen-doped carbon (NC) and metal-nitrogen-carbon (MNC) materials have been extensively investigated in lithium-sulfur batteries to alleviate the "shuttle effect". MNC are generally synthesized using NC as the parent material, wherein nitrogen atoms in NC serve as the "bridge" to coordinate with metal atoms. So far, an important scientific issue has not been settled: does the introduction of metal sites into NC certainly enhance the Li-S battery performance? In this work, NC and MNC materials derived from the same precursor, a nitrogen-rich porous polymer, are systematically compared as cathode hosts for Li-S battery through theoretical calculations and experimental investigation. Li-S cell with NC as the cathode sulfur host exhibits better cycle performance at low current densities (0.1 and 0.2C), whereas MNC materials predominate at higher current densities (such as 1C and 2C). Based on theoretical calculation and experimental results, it is concluded that the introduction of metal sites into NC through nitrogen bonding promoted the catalytic capability for faster sulfur redox reaction kinetics, whereas the adsorption energy toward polysulfides decreased. This work provides important guidance for more targeted design of advanced materials for lithium-sulfur battery application in the future.

NiCo2O4 Nanowires Immobilized on Nitrogen-Doped Ti3C2Tx for High-Performance Wearable Magnesium-Air Batteries.

Flexible magnesium (Mg)-air batteries provide an ideal platform for developing efficient energy-storage devices toward wearable electronics and bio-integrated power sources. However, high-capacity bio-adaptable Mg-air batteries still face the challenges in low discharge potential and inefficient oxygen electrodes, with poor kinetics property toward oxygen reduction reaction (ORR). Herein, spinel nickel cobalt oxides (NiCo2O4) nanowires immobilized on nitrogen-doped Ti3C2Tx (NiCo2O4/N-Ti3C2Tx) are reported via surface chemical-bonded effect as oxygen electrodes, wherein surface-doped pyridinic-N-C and Co-pyridinic-N moieties accounted for efficient ORR owing to increased interlayer spacing and changed surrounding environment around Co metals in NiCo2O4. Importantly, in polyethylene glycol (PVA)-NaCl neutral gel electrolytes, the NiCo2O4/N-Ti3C2Tx-assembled quasi-solid wearable Mg-air batteries delivered high open-circuit potential of 1.5 V, good flexibility under various bent angles, high power density of 9.8 mW cm-2, and stable discharge duration to 12 h without obvious voltage drop at 5 mA cm-2, which can power a blue flexible light-emitting diode (LED) array and red smart rollable wearable device. The present study stimulates studies to investigate Mg-air batteries involving human-body adaptable neutral electrolytes, which will facilitate the application of Mg-air batteries in portable, flexible, and wearable power sources for electronic devices.

Nitrogen-Doped Starbons®: Methodology Development and Carbon Dioxide Capture Capability.

Five nitrogen sources (glycine, ß-alanine, urea, melamine and nicotinamide) and three heating methods (thermal, monomodal microwave and multimodal microwave) are used to prepare nitrogen-doped Starbons® derived from starch. The materials are initially produced at 250-300 °C (SNx 300y ), then heated in vacuo to 800 °C to produce nitrogen-doped SNx 800y 's. Melamine gives the highest nitrogen incorporation without destroying the Starbon® pore structure and the microwave heating methods give higher nitrogen incorporations than thermal heating. The carbon dioxide adsorption capacities of the nitrogen-doped Starbons® determined gravimetrically, in many cases exceed those of S300 and S800. The carbon dioxide, nitrogen and methane adsorption isotherms of the most promising materials are measured volumetrically. Most of the nitrogen-doped materials show higher carbon dioxide adsorption capacities than S800, but lower methane and nitrogen adsorption capacities. As a result, the nitrogen-doped Starbons® exhibit significantly enhanced carbon dioxide versus nitrogen and methane versus nitrogen selectivities compared to S800.

Selectively Extending the Curved Side of N-Doped Hexa-peri-hexabenzocoronene.

A curved nanographene, conceptually by insertion of nitrogen into a trapezoidal planar nanographene at the edge was synthesized by π-extension of the nitrogen-doped hexa-peri-hexabenzocoronene. This aza-doped nanographene exhibited a π-electronic concave face containing a nonaromatic azepine ring in the middle with a size of 14.0 Å length and 4.0 Å depth, which represents an unprecedented half-side concave geometry of curved nanographene. The bent π-extension exhibited a low degree of conjugation suggested by calculation results. Due to the unique 3D structure and electron-rich property, this nanographene showed pronounced intermolecular charge transfer with C60.

Core-shell ZnO@CoO nitrogen doped nano-composites as highly sensitive electrochemical sensor for organophosphate pesticides detection.

Core-shell ZIF-8@ZIF-67 was synthesized by growing a cobalt-based ZIF-67 on a ZIF-8 seed particle. Herein, through selective etching of the ZIF-8@ZIF-67 core and subsequent direct carbonization, core-shell hollow ZnO@CoO nitrogen-doped nanoporous carbon (HZnO@CoO-NPC) nanocomposites were prepared. HZnO@CoO-NPCs possessed a high nitrogen content, large surface area, high degree of graphitization and excellent electrical conductivity, all of which were attributed to successfully integrating the unique advantages of ZIF-8 and ZIF-67. HZnO@CoO-NPCs were used to assemble acetylcholinesterase (AChE) biosensors for organophosphorus pesticides (OPs) detection. The low detection limit of 2.74 × 10-13 M for chlorpyrifos and 7.6 × 10-15 M for parathion-methyl demonstrated the superior sensing performance. The results showed that the electrochemical biosensor constructed by HZnO@CoO-NPC provided a sensitive and efficient electrochemical strategy for OPs detection.

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

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

Well-dispersed Pt/Nb2O5on zeolitic imidazolate framework derived nitrogen-doped carbon for efficient oxygen reduction reaction.

In this work, an advanced hybrid material was constructed by incorporating niobium pentoxide (Nb2O5) nanocrystals with nitrogen-doped carbon (NC) derived from ZIF-8 dodecahedrons, serving as a support, referred to as Nb2O5/NC. Pt nanocrystals were dispersed onto Nb2O5/NC using a simple impregnation reduction method. The obtained Pt/Nb2O5/NC electrocatalyst showed high oxygen reduction reaction (ORR) activity due to three-phase mutual contacting structure with well-dispersed Pt and Nb2O5NPs. In addition, the conductive NC benefits electron transfer, while the induced Nb2O5can regulate the electronic structure of Pt element and anchor Pt nanocrystals, thereby enhancing the ORR activity and stability. The half-wave potential (E1/2) for Pt/Nb2O5/NC is 0.886 V, which is higher than that of Pt/NC (E1/2= 0.826 V). The stability examinations demonstrated that Pt/Nb2O5/NC exhibited higher electrocatalytic durability than Pt/NC. Our work provides a new direction for synthesis and structural design of precious metal/oxides hybrid electrocatalysts.

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

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

A Simple Method for Synthesizing Nitrogen-Doped Carbon Quantum Dots for Fluorescent "Turn off" Mercury (II) Ion Sensing.

Here, straightforward and environmentally friendly fluorescent nitrogen doped carbon quantum dots (N-CQDs) with a high blue fluorescence emission at 455 nm are used for ultrasensitive Hg2+ ion detection. Folic acid and urea are used as carbon sources in the carbonization process. Two broad absorption bands at around 280 and 370 nm from UV-Vis spectrum and characteristic absorption peaks from infrared spectrum confirms the successful synthesis of the N-CQDs. Energy dispersive X-Ray analysis confirmed the elemental composition of the N-CQDs. Transmission electron microscopy showed the homogeneous globular morphology of the N-CQDs with an average particle size of 65 nm. Zeta potential measurement established the stability and surface charge of N-CQDs. Dynamic light scattering measurement showed the average size of N-CQDs. With the addition of Hg2+ ion to N-CQDs, the blue fluorescence emission is quenched. Moreover, the N-CQDs can be applied to real water sample such as pond water, river water, and tap water. The detection limit is approximately calculated to be 12 nM and linear range is 0-30 parts per billion.

Exploring the structural characteristics and adsorption capabilities of cost-effective N- doped activated carbon derived from waste biomass for CO2 adsorption.

In this work, ACs were originated from two different bio-waste sources of Date and Jujube seeds (DS and JS). The influence of the precursor type as well as KOH chemical activator ratio on the structural properties and CO2 adsorption performances of synthesized ACs were assessed. Impact of pre-treatment of raw material via functionalization with urea on the performance of prepared adsorbents was also evaluated. Functionalized DS-based AC possessed the highest surface area and largest micropore volume equal to 864 m2/g and 0.33 cm3/g, respectively. CO2 adsorption behavior of ACs was experimentally evaluated via TGA at different adsorption temperatures of 25 and 50 °C and CO2 concentrations of 10 and 90 vol% under atmospheric pressure. Based on the TGA results, functionalized and non-functionalized DS-prepared ACs with KOH: biochar weight ratio of 2:1, demonstrated great CO2 capture capacity up to 1.3 and 1.2 mmol/g, respectively under realistic condition of 10 vol% CO2 and 25 °C. The urea-nitrogenation and KOH-activation as economical and simple approaches sensitively assisted preparation of a novel and promising N-doped porous AC from bio-waste resources which can be exploited for superior CO2 capture applications.

Electron transfer enhanced catalytic activity of nitrogen doped reduced graphene oxide supported CuCo2O4 towards the fast reduction of 4-nitrophenol in water.

There has been a growing interest in the design and development of graphene based composite materials with superior performances for environmental catalytic applications. But in most of the studies the synthesis conditions require elevated temperatures and expensive working setups (high temperature furnaces, autoclaves, inert atmosphere conditions etc.). In this reported work, the nitrogen doped reduced graphene oxide supported CuCo2O4 (NG/CuCo2O4) composites were prepared through a simple one pot synthesis method under mild conditions (∼95 °C and air atmosphere) and successfully employed as catalysts for the reduction of toxic 4-nitrophenol (4NP). The characterization results revealed the successful formation of NG/CuCo2O4 composites with a possible charge transfer interaction between nitrogen doped reduced graphene oxide support of CuCo2O4. The NG/CuCo2O4 hybrids exhibited robust catalytic activity in 4NP reduction with an activity factor of 261.5 min-1 g-1. A 4NP conversion percentage which is as high as 99.5% was achieved within 11 min using the NG/CuCo2O4 catalyst. The detailed kinetic analysis confirmed the Langmuir-Hinshelwood model for the NG/CuCo2O4 catalysed 4NP reduction. The nitrogen doped reduced graphene oxide support modified the electronic levels of CuCo2O4 nanoparticles through electron transfer interactions and enhanced the catalytic activity of CuCo2O4 in NG/CuCo2O4 through improved adsorption of reactant ions and effective generation of active hydrogen species. The good reusability and stability along with profound activity of NG/CuCo2O4 catalyst makes it a promising material for wide scale catalytic applications.