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1.
ChemSusChem ; : e202401049, 2024 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-38963775

RESUMO

Developing efficient metal-free catalysts for lignin valorization is essential but challenging. In this study, a cost-effective strategy is employed to synthesize a P, N co-doped carbon catalyst through hydrothermal and carbonization processes. This catalyst effectively cleaved α-O-4, ß-O-4, and 4-O-5 lignin linkages, as demonstrated with model compounds. Various catalysts were prepared at different carbonization temperatures and thoroughly characterized using techniques such as XRD, RAMAN, FTIR, XPS, NH3-TPD, and HRTEM. Attributed to higher acidity, the P5NC-500 catalyst exhibited the best catalytic activity, employing H2O2 as the oxidant in water. Additionally, this metal-free technique efficiently converted simulated lignin bio-oil, containing all three linkages, into valuable monomers. Density Functional Theory calculations provided insight into the reaction mechanism, suggesting substrate and oxidant activation by P-O-H sites in the P5NC-500, and by N-C-O-H in the CN catalyst. Moreover, the catalyst's recyclability and water utilization enhance its environmental compatibility, offering a highly sustainable approach to lignin valorization with potential applications in various industries.

2.
Artigo em Inglês | MEDLINE | ID: mdl-38982793

RESUMO

Carbon-based magnetic nanocomposites as promising lightweight electromagnetic wave (EMW) absorbents are expected to address critical issues caused by electromagnetic pollution. Herein, Fe3O4 nanoparticles embedded into a 3D N-rich porous carbon nanohoneycomb (Fe3O4@NC) were developed via the pyrolysis of an in-situ-polymerized compound of m-phenylenediamine initiated by FeCl2 in the presence of NaCl crystals as templates. Results demonstrate that Fe3O4@NC features highly dispersed Fe3O4 nanoparticles into an ultrahigh specific pyridinic-N doping carbon matrix, resulting in excellent impedance matching characteristics and electromagnetic wave absorbing capability with the biggest effective absorption bandwidth (EAB) of up to 7.1 GHz and the minimum reflective loss (RLmin) of up to -65.5 dB in the thin thickness of 2.5 and 2.3 mm, respectively, which also outperforms the majority of carbon-based absorbers reported. Meanwhile, its high absorption performance is further demonstrated by an ethylene propylene diene monomer wave absorbing patch filled with 8.0 wt % Fe3O4@NC, which can completely shield a 5G signal in a mobile phone. In addition, theory calculation reveals that there is a strongest dx2-Pz orbital hybridization interaction between Fe3O4 clusters and pyridinic-N dopants in the carbon network, compared with other kinds of N dopants, which can not only generate more dipoles of carbon networks but also increase net magnetic moments of Fe3O4, thereby leading to a coupling effect of efficient dielectric and magnetic losses. This work provides new insights into the precise design and synthesis of carbon-based magnetic composites with specific interface interactions and morphological effects for high-efficiency EMW absorption materials.

3.
Food Chem ; 459: 140338, 2024 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-38996633

RESUMO

It is highly desirable to develop a low-cost and rapid detection method for trace levels of carbendazim fungicide residues, which would be beneficial for improving human health and mitigating environmental issues. Herein, isolated single tungsten atoms were implanted onto well-organized metal-organic framework (MOF)-derived N-doped carbons to form W-N-C single-site heterojunctions with ultrahigh electrocatalytic activity. The coupling of W-N-C with Cu3(HHTP)2, an electronically conductive MOF with a large surface area and porous structure, exhibited enhanced electrocatalytic performance for the oxidation of carbendazim (CBZ) when they were used for decorating graphene nanoplatelet flexible electrode arrays fabricated via template-assisted scalable filtration. A wide linear range (3.0 nM-50 µM) with an ultra-low detection limit of 0.97 nM and fast response was achieved for CBZ analysis. Moreover, the sensing platform has been utilised to monitor CBZ levels in vegetable samples with satisfactory recovery rates of 97.2-102% and a low relative standard deviation of 1.9%.

4.
ACS Appl Mater Interfaces ; 16(28): 36401-36412, 2024 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-38958058

RESUMO

Combining the merits of the dendrite-free formation of a Mg anode and the fast kinetics of Li ions, the Mg-Li hybrid ion batteries (MLIBs) are considered an ideal energy storage system. However, the lack of advanced cathode materials limits their further practical application. Herein, we report a dual strategy of morphology optimization and interlayer expansion for the construction of hierarchical flower-like VS2 architecture coated by N-doped amorphous carbon layers. This tailored hierarchical flower-like structure coupled with homogeneous N-doped amorphous carbon layers cooperatively provide more active sites and buffer volume changes, thus realizing the enhancement of capacity and structural stability. Moreover, the enlarged interlayer spacing caused by the cointercalation of polyvinylpyrrolidone and ammonium ions can effectively promote the charge transfer rate and facilitate the rapid ion diffusion, as further demonstrated by electrochemical results and theoretical calculations. These features endow the hierarchical flower-like VS2 cathode with superior specific energy density (644.4 Wh kg-1, average voltage of 1.2 V vs Mg2+/Mg) and excellent rate capability (181.1 mAh g-1 at 2000 mA g-1). Systematic ex situ characterization measurements are employed to reveal the ion storage mechanism, which confirms that Li+ storage plays a leading role in the capacity contribution of MLIBs. Our strategy is in favor of providing useful insights to design and construct MLIBs with high energy density and excellent rate performance.

5.
Mikrochim Acta ; 191(8): 459, 2024 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-38985347

RESUMO

A renewable electrochemical screen-printed electrode (SPE) is proposed based on magnetic bamboo-like nitrogen-carbon (N-C) nanotubes loaded with nickel-cobalt alloy (NiCo) nanoparticles (NiCo@N-CNTs) for the determination of ractopamine (RAC). During the preparation of NiCo@N-CNTs, Co-MOF-67 (ZIF-67) was firstly synthesized, and then blended with dicyandiamide and nickel acetate, followed by a one-step pyrolysis procedure to prepare NiCo@N-doped carbon nanotubes. The surface morphology, structure, and chemical composition of NiCo@N-CNTs were characterized by SEM, TEM, XRD, XPS, and EDS. The electrocatalytic and electrochemical behavior of NiCo@N-CNTs were investigated by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). The results demonstrated that NiCo@N-CNTs possessed remarkable conductivity and electrocatalysis to the oxidation of ractopamine (RAC). By using screen-printed electrode (SPE), NiCo@N-CNTs, and a designed base support, a magnetic RAC sensor (NiCo@N-CNTs/SPE) was successfully constructed. It presented a detection linear range of 0.05-80 µM with a detection limit of 12 nM (S/N = 3). It also exhibited good sensitivity, reproducibility, and practicability in spiked real pork samples. Since the adhesion of NiCo/N-CNTs on SPE was controlled by magnet, the NiCo@N-CNTs was easily detached from the SPE surface by magnetism and thus displayed excellent renewability. This work broadened insights into portable devices for on-site and real-time analysis.

6.
Mikrochim Acta ; 191(7): 416, 2024 06 24.
Artigo em Inglês | MEDLINE | ID: mdl-38913162

RESUMO

To realize the reutilization of waste Myrica rubra in the analytical field, we synthesized Myrica rubra-based N-doped carbon dots (MN-CDs) and further anchored them onto the surface of Fe3S4 to fabricate Fe3S4@MN-CD nanocomposites. The as-fabricated nanocomposites possessed higher peroxidase-mimetic activity than its two precursors, resulting from the synergistic effect between them, and could catalyze colorless 3,3',5,5'-tetramethylbenzidine (TMB) into deep blue oxTMB with a strong 652-nm absorption. Under optimized conditions (initial solution pH, 3.5; incubation temperature, 35 ℃; Fe3S4@MN-CD concentration, 50 µg mL-1, and 652-nm absorption), Fe3S4@MN-CDs were employed for colorimetric assay of p-aminophenol (p-AP) with wide linear range (LR, 2.9-100 µM), low detection limit (LOD, 0.87 µM), and satisfactory recoveries (86.3-105%) in environmental waters. Encouragingly, this colorimetric assay provided the relative accuracy of 97.0-99.4% as compared with  conventional HPLC-UV detection. A portable smartphone-based colorimetric application was developed by combining the Fe3S4@MN-CD-based visually chromogenic reaction with a "Thing Identify" APP software. Besides, we engineered an image-capturing device feasible for field use, in which the internal-compact sealing prevented external light source from entering photography chamber, thereby reducing light interference, and also the bottom light source enhanced the intensity of blue imaging. This colorimetric platform exhibited satisfactory LR (1-500 µM), low LOD (0.3 µM), and fortification recoveries (86.6-99.6%). In the chromogenic reaction catalyzed by Fe3S4@MN-CDs, ·O2- played a key role in concomitant with the participation of •OH and h+. Both the colorimetric assay and smartphone-based intelligent sensing show great promising in on-site monitoring of p-AP under field conditions.


Assuntos
Aminofenóis , Carbono , Colorimetria , Limite de Detecção , Pontos Quânticos , Smartphone , Poluentes Químicos da Água , Colorimetria/métodos , Aminofenóis/química , Aminofenóis/análise , Carbono/química , Poluentes Químicos da Água/análise , Pontos Quânticos/química , Materiais Biomiméticos/química , Benzidinas/química , Peroxidase/química
7.
ChemSusChem ; : e202400997, 2024 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-38923349

RESUMO

The design and construction of highly efficient electrocatalysts for overall water splitting and urea electrolysis are significantly important for promoting energy conversion and realizing green hydrogen production. In this work, we constructed a multi-phase heterojunction through a simple hydrothermal and phosphorization process. The P-doped NiFe2O4 (P-NiFe2O4) nanoparticles were uniformly anchored on the bamboo-like N-doped carbon nanotubes (NCNTs) grown via a NiFe-alloy autocatalysis. The electronic structure and coordination environment of active species were optimized by the synergistic action of P doping, well-dispersed ultrafine NiFe2O4, and NCNTs matrix with good conductivity, enhancing their quantity and activity for electrocatalysis. Consequently, the P-NiFe2O4/NCNTs/NiFe exhibits excellent HER and OER activities with an overpotential of 111 and 266 mV at 10 mA cm-2 in 1 M KOH, respectively. The symmetrical overall water-splitting cell using P-NiFe2O4/NCNTs/NiFe as both anode and cathode delivers 10 mA cm-2 at a voltage of 1.604 V in 1 M KOH. Notably, the two-electrode cell requires a low voltage of 1.467 V to achieve a current density of 10 mA cm-2 in 1 M KOH solution with 0.6 M urea. This designed catalysts display outstanding reaction kinetics and catalytic stability. This work provides useful guidance for applying transition metal-based catalysts for hydrogen production.

8.
Chemosphere ; 361: 142432, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38797204

RESUMO

With the increase of Cu (II) content, its bioaccumulation becomes a potential pollution to the environment. It is necessary to design an economical and efficient material to remove Cu (II) without causing other environmental hazards. A novel material of alginate composite bead (ALG@NCDs) was synthesized by embedding N-doped carbon dots into pure alginate bead for the adsorption of Cu (II) from wastewater and contaminated soil. The initial concentration, the amount of adsorbent, temperature, adsorption time, and pH value were optimized for the adsorption of Cu (II). According to the Langmuir isothermal adsorption model, the maximum adsorption amount of the material to Cu (II) was 152.44 mg/g. The results of selective adsorption showed that ALG@NCDs had higher affinity to Cu (II) than to Pb (II), Co (II), Ni (II), and Zn (II). After five adsorption-desorption experiment, adsorption capacity of the ALG@NCDs was kept 89% of the initial adsorption capacity. Its Cu (II) adsorption mechanism was studied by density functional theory calculations. In addition, the material could effectively adsorb Cu (II) and release the phytonutrient Ca (II) simultaneously when applied to actual wastewater and soil. The fabricated ALG@NCDs would be a promising material for the adsorption of Cu (II) from wastewater or soil.


Assuntos
Carbono , Cobre , Nitrogênio , Poluentes do Solo , Águas Residuárias , Poluentes Químicos da Água , Adsorção , Cobre/química , Águas Residuárias/química , Carbono/química , Nitrogênio/química , Poluentes Químicos da Água/química , Poluentes do Solo/química , Poluentes do Solo/análise , Biomassa , Hidrogéis/química , Solo/química , Teoria da Densidade Funcional , Alginatos/química
9.
Talanta ; 277: 126252, 2024 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-38805948

RESUMO

COVID-19 as an infectious disease with rapid transmission speed is caused by severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), so, early and accurate diagnostics of COVID-19 is quite challenging. In this work, the selective and sensitive self-enhanced ECL method to detect of SARS-CoV-2 protein was designed with magnetic N-doped carbon derived from dual-ligand metal-organic frameworks (MOF) (CoO@N-C) with the primary and tertiary amino groups as a novel coreactant that covalently combined with Ru(bpy)2(phen-NH2)2+ as electrochemiluminescence (ECL) emitter. Mixed-ligand strategy and selected nitrogen-containing ligands, 4,4',4''-((1,3,5-triazine-2,4,6-triyl) tris-(azanediyl)) tribenzoic acid (H3TATAB) with 2-aminoterephthalic acid (BDC-NH2) were used for synthesis of the proposed MOF. Also, magnetic CoO@N-C with high synergistically charge transfer kinetics and good stability can be used as an effective platform/coreactor on the ITO electrode which load more Ru-complex as signal producing compound and SARS-CoV-2 N protein antibody to increase the sensitivity of the immunosensor. Furthermore, (CoO@N-C) as coreactor improved the ECL signal of the Ru (II)-complex more than 2.1 folds compared to tripropylamine. In view of these competences, the novel "on-off" ECL biosensor performed with great stability and repeatability for detection of SARS-CoV-2 protein, which exhibited a broad linearity from 8 fg. mL-1 to 4 ng. mL-1 (6 order of magnitude) and an ultra-low limit of detection 1.6 fg. mL-1. Finally, this proposed method was successfully applied to detect of SARS-CoV-2 N protein in serum sample with satisfactory results, indicating the proposed immunosensor has the potential for quick analysis of SARS-CoV-2.


Assuntos
Técnicas Biossensoriais , COVID-19 , Carbono , Técnicas Eletroquímicas , Medições Luminescentes , Estruturas Metalorgânicas , SARS-CoV-2 , SARS-CoV-2/imunologia , SARS-CoV-2/isolamento & purificação , Estruturas Metalorgânicas/química , Humanos , Carbono/química , Técnicas Eletroquímicas/métodos , Ligantes , COVID-19/diagnóstico , Medições Luminescentes/métodos , Técnicas Biossensoriais/métodos , Limite de Detecção , Imunoensaio/métodos , Nitrogênio/química
10.
Adv Sci (Weinh) ; 11(28): e2401730, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38696659

RESUMO

Sodium ion batteries (SIBs) are considered as the ideal candidates for the next generation of electrochemical energy storage devices. The major challenges of anode lie in poor cycling stability and the sluggish kinetics attributed to the inherent large Na+ size. In this work, Bi nanosphere encapsulated in N-doped carbon nanowires (Bi@N-C) is assembled by facile electrospinning and carbonization. N-doped carbon mitigates the structure stress/strain during alloying/dealloying, optimizes the ionic/electronic diffusion, and provides fast electron transfer and structural stability. Due to the excellent structure, Bi@N-C shows excellent Na storage performance in SIBs in terms of good cycling stability and rate capacity in half cells and full cells. The fundamental mechanism of the outstanding electrochemical performance of Bi@N-C has been demonstrated through synchrotron in-situ XRD, atomic force microscopy, ex-situ scanning electron microscopy (SEM) and density functional theory (DFT) calculation. Importantly, a deeper understanding of the underlying reasons of the performance improvement is elucidated, which is vital for providing the theoretical basis for application of SIBs.

11.
Small ; : e2402927, 2024 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-38794873

RESUMO

Na3V2(PO4)3 is a promising high-voltage cathode for aqueous zinc-ion batteries (ZIBs) and organic sodium-ion batteries (SIBs). However, the poor rate capability, specific capacity, and cycling stability severely hamper it from further development. In this work, Na3V2(PO4)3 (NVP) with vanadium nitride (VN) quantum dots encapsulated by nitrogen-doped carbon (NC) nanoflowers (NVP/VN@NC) are manufactured as cathode using in situ nitridation, carbon coating, and structural adjustment. The outer NC layer increases the higher electronic conductivity of NVP. Furthermore, VN quantum dots with high theoretical capacity not only improve the specific capacity of pristine NVP, but also serve as abundant "pins" between NVP and NC to strengthen the stability of NVP/VN@NC heterostructure. For Zn-ion storage, these essential characteristics allow NVP/VN@NC to attain a high reversible capacity of 135.4 mAh g-1 at 0.1 A g-1, and a capacity retention of 91% after 2000 cycles at 5 A g-1. Meanwhile, NVP/VN@NC also demonstrates to be a stable cathode material for SIBs, which can reach a high reversible capacity of 124.5 mAh g-1 at 0.1 A g-1, and maintain 92% of initial capacity after 11000 cycles at 5 A g-1. This work presents a feasible path to create innovative high-voltage cathodes with excellent reaction kinetics and structural stability.

12.
Nanomaterials (Basel) ; 14(9)2024 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-38727338

RESUMO

The catalytic oxidation of alcohols is an important transformation in the chemical industry. Carbon materials with a large surface area and N doping show great promise as metal-free catalysts for the reaction. In this study, a rich N-containing covalent triazine framework polymerized by cyanuric chloride and p-phenylenediamine was used to synthesize N-doped porous carbon with the assistance of a pore-forming agent-NaCl. First, the mass ratio of the polymer/NaCl was optimized to 1:9. Then, the influence of the pyrolysis temperatures (700-1000 °C) on the materials was studied in detail. It was found that the carbon materials were gradually exfoliated by molten salt at high temperatures. XRD and Raman characterizations showed them with a certain graphitization. The optimal doped carbon CNN-1-9-900 achieved the highest surface area of 199.03 m2g-1 with the largest pore volume of 0.29 cm3g-1. Furthermore, it had a high N content of 9.9 at% with the highest relative proportion of pyridinic/graphitic N. Due to the synergistic effect between the surface area and pyridinic/graphitic N, CNN-1-9-900 showed the best performance for benzyl alcohol oxidation with TBHP at moderate conditions, and the process also worked for its derivatives.

13.
Molecules ; 29(10)2024 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-38792210

RESUMO

A Fe-Co dual-metal co-doped N containing the carbon composite (FeCo-HNC) was prepared by adjusting the ratio of iron to cobalt as well as the pyrolysis temperature with the assistance of functionalized silica template. Fe1Co-HNC, which was formed with 1D carbon nanotubes and 2D carbon nanosheets including a rich mesoporous structure, exhibited outstanding oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalytic activities. The ORR half-wave potential is 0.86 V (vs. reversible hydrogen electrode, RHE), and the OER overpotential is 0.76 V at 10 mA cm-2 with the Fe1Co-HNC catalyst. It also displayed superior performance in zinc-air batteries. This method provides a promising strategy for the fabrication of efficient transition metal-based carbon catalysts.

14.
ACS Appl Mater Interfaces ; 16(22): 29060-29068, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38767933

RESUMO

Highly efficient electrochemical CO2-to-CO conversion is a promising approach for achieving carbon neutrality. While nonmetallic carbon electrocatalysts have shown potential for CO2-to-CO utilization in H-type cells, achieving efficient conversion in flow cells at an industrial scale remains challenging. In this study, we present a cost-effective synthesis strategy for preparing ultrathin 2D carbon nanosheet catalysts through simple amine functionalization. The optimized catalyst, NCNs-2.5, demonstrates exceptional CO selectivity with a maximum Faradaic efficiency of 98% and achieves a high current density of 55 mA cm-2 in a flow cell. Furthermore, the catalyst exhibits excellent long-term stability, operating continuously for 50 h while maintaining a CO selectivity above 90%. The superior catalytic activity of NCNs-2.5 is attributed to the presence of amine-N active sites within the carbon lattice structure. This work establishes a foundation for the rational design of cost-effective nonmetallic carbon catalysts as sustainable alternatives to metals in energy conversion systems.

15.
Small ; : e2311260, 2024 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-38634299

RESUMO

Vapor-based deposition techniques are emerging approaches for the design of carbon-supported metal powder electrocatalysts with tailored catalyst entities, sizes, and dispersions. Herein, a pulsed CVD (Pt-pCVD) approach is employed to deposit different Pt entities on mesoporous N-doped carbon (MPNC) nanospheres to design high-performance hydrogen evolution reaction (HER) electrocatalysts. The influence of consecutive precursor pulse number (50-250) and deposition temperature (225-300 °C) are investigated. The Pt-pCVD process results in highly dispersed ultrasmall Pt clusters (≈1 nm in size) and Pt single atoms, while under certain conditions few larger Pt nanoparticles are formed. The best MPNC-Pt-pCVD electrocatalyst prepared in this work (250 pulses, 250 °C) reveals a Pt HER mass activity of 22.2 ± 1.2 A mg-1 Pt at -50 mV versus the reversible hydrogen electrode (RHE), thereby outperforming a commercially available Pt/C electrocatalyst by 40% as a result of the increased Pt utilization. Remarkably, after optimization of the Pt electrode loading, an ultrahigh Pt mass activity of 56 ± 2 A mg-1 Pt at -50 mV versus RHE is found, which is among the highest Pt mass activities of Pt single atom and cluster-based electrocatalysts reported so far.

16.
Small Methods ; : e2400174, 2024 Apr 09.
Artigo em Inglês | MEDLINE | ID: mdl-38594890

RESUMO

Non-flow aqueous zinc-bromine batteries (AZBBs) are highly attractive owing to their lightweight construction and largely reduced cost compared with the flow ones. Yet, their development is restricted by the sluggish reaction kinetics of Br2/Br-, the shuttle of soluble polybromide species (Brn -, n is odd), and the poor stability of Zn-based anode. Herein, an effective alkaline-neutral electrolyte decoupling system is constructed to mitigate these issues, where nitrogen-doped carbon felt with high catalytic activity to Br2/Br- reaction is developed for cathode, a cost-effective cation exchange membrane (CEM) of polyethersulfone/sulfonated polyether ether ketone (PES/SPEEK-M) that can stop Brn - is used as separator, and glucose that can inhibit dendrites is introduced as anolyte additive. The constructed flowless AZBB mainly consists of two separate redox couples, including Zn/Zn(OH)4 2- in alkaline anolyte and Br2/Br- in neutral media, where non-cations (e.g. OH-, Zn(OH)4 2-, H2O,  and Brn -) can be restricted to their respective chamber by the PES/SPEEK-M while cations can pass by. In the optimized system, good electrochemical performance is achieved, mainly including a surprising discharge voltage of 2.01 V, a high average Coulombic efficiency of 96.7%, and a good cycling life of ≈1000 cycles without obvious capacity decay at a fixed charge capacity of 2 mAh cm-2.

17.
J Colloid Interface Sci ; 668: 243-251, 2024 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-38678880

RESUMO

Properly design and fabricate capable electrocatalysts with 3D hierarchical hollow framework to realize cost-effective and efficacious overall water splitting (OWS) are particularly meaningful for the large-scale arrangement of pivotal energy technology. In this study, P-doped NiCo2O4 nanoparticles encapsulated in N-doped carbon hierarchical hollow nanoflowers (P-NiCo2O4@NCHHNFs) were constructed using the hydrothermal-pyrolysis-phosphorization approach. This fascinating architecture can not merely serve as a conductive pathway for electron transfer, but at the same time effectively inhibited the aggregation and corrosion of the NiCo2O4 nanoparticles. Additionally, the P doping not only regulates electronic structure configuration to boost the intrinsic activity of the catalyst, but also enhance electrochemical surface areas to reveal more accessible active sites. Attributing to these characteristics, the as-prepared P-NiCo2O4@NCHHNFs exhibit preeminent electrocatalytic performance with low overpotentials of 283 mV and 162 mV for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) (at 10 mA cm-2), respectively. Specifically, by using the P-NiCo2O4@NCHHNFs as bifunctional catalysts, a low potential of 1.56 V (at 10 mA cm-2) is sufficient to drive overall water splitting with splendid durability. This study proposed an innovative strategy for the conceiving and fabricating high-performance catalysts via heteroatom-doping.

18.
Mikrochim Acta ; 191(5): 290, 2024 Apr 29.
Artigo em Inglês | MEDLINE | ID: mdl-38683258

RESUMO

A core-shell ZIF-67@ZIF-8-derived Co nanoparticles embedded in N-doped carbon nanotube polyhedra (Co/C-NCNP) hybrid nanostructure was prepared by a pyrolysis method. The synthesized Co/C-NCNP was modified on the screen-printed carbon electrode and used for the portable wireless sensitive determination of breviscapine (BVC) by differential pulse voltammetry. The Co/C-NCNP had a large surface area and excellent catalytic activity with increasing Co sites to combine with BVC for selective determination, which led to the improvement of the sensitivity of the electrochemical sensor. Under optimized conditions, the constructed sensor had linear ranges from 0.15 to 20.0 µmol/L and 20.0 to 100.0 µmol/L with the limit of detection of 0.014 µmol/L (3S0/S). The sensor was successfully applied to BVC tablet sample analysis with satisfactory results. This work provided the potential applications of zeolitic imidazolate framework-derived nanomaterials in the fabrication of electrochemical sensors for the sensitive detection of drug samples.

19.
Chempluschem ; 89(7): e202300785, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38436555

RESUMO

This work presents the synthesis of N-doped nanoporous carbon materials using the Ionic Liquid (IL) 1-butyl-3-methylimidazolium tricyanomethanide [BMIM][TCM] as a fluidic carbon precursor, employing two carbonization pathways: templated precursor and pyrolysis/activation. Operando monitoring of mass loss during pyrolytic and activation treatments provides insights into chemical processes, including IL decomposition, polycondensation reactions and pore formation. Comparatively low mass reduction rates were observed at all stages. Heat treatments indicated stable pore size and increasing volume/surface area over time. The resulting N-doped carbon structures were evaluated as electrocatalysts for the oxygen reduction reaction (ORR) and adsorbents for gases and organic vapors. Materials from the templated precursor pathway exhibited high electrocatalytic performance in ORR, analyzed using Rotating Ring-Disk electrode (RRDE). Enhanced adsorption of m-xylene was attributed to wide micropores, while satisfactory CO2 adsorption efficiency was linked to specific morphological features and a relatively high content of N-sites within the C-networks. This research contributes valuable insights into the synthesis and applications of N-doped nanoporous carbon materials, highlighting their potential in electrocatalysis and adsorption processes.

20.
J Colloid Interface Sci ; 663: 609-623, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38430831

RESUMO

The matching of long cycle life, high power density, and high energy density has been an inevitable requirement for the development of efficient anode materials for lithium-ion capacitors (LICs). Here, we introduce an N-doped carbon nanotube hollow polyhedron structure (Co3O4-CNT-800) with high specific surface area and active sites, which is anchored with two-dimensional (2D) Ti3C2Tx nanosheets with metallic conductivity and abundant surface functional groups by electrostatic adsorption to form a hierarchical multilevel hollow semi-covered framework structure. Benefiting from the synergistic effect between Co3O4-CNT-800 and Ti3C2Tx, the composites exhibit superior energy storage efficiency and long cycling stability. The Co3O4-CNT-800/Ti3C2Tx electrodes exhibit a high specific capacity of 817C/g at a current density of 0.5 A/g under the three-electrode system, and the capacity retention rate is 91 % after 5000 cycles at a current density of 2 A/g. Additionally, we assembled Co3O4-CNT-800/Ti3C2Tx as the anode and Activated carbon (AC) cathode to form LIC devices, which showed an electrochemical test result of 90.01 % capacitance retention after 8000 cycles at 2 A/g, and the maximum power density of the LIC was 3000 W/kg and the maximum energy density was 121 Wh/kg. This work pioneered the combination of N-doped carbon nanotube hollow polyhedron structure with two-dimensional Ti3C2Tx, which provides an effective strategy for preparing LIC negative electrode materials with high specific capacitance and long cycling stability.

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