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1.
A novel adsorbent zeolite/N-doped porous activated carbon (ZAC) was prepared by the synthesis of zeolite and mesoporous carbon to remove ammonia nitrogen (NH4+–N) and chemical oxygen demand (COD) from aqueous solution. The impacts of adhesives, molding pressure, synthetic temperature and ratio on ZAC preparation were investigated. The prepared adsorbent was characterized by BET surface area measurement, scanning electron microscopy and X-ray diffraction. The adsorption kinetics was better depicted by the pseudo-second-order model than the pseudo-first-order model and the isotherm fitted well with the Langmuir model. The adsorption process was endothermic, spontaneous and favorable according to thermodynamic data. The adsorbent has much potential in the simultaneous removal of COD and NH4+–N from wastewater.

A novel adsorbent zeolite/N-doped porous activated carbon (ZAC) was prepared by the synthesis of zeolite and mesoporous carbon to remove ammonia nitrogen (NH4+–N) and chemical oxygen demand (COD) from aqueous solution.  相似文献   

2.
A series of AuPd/C catalysts were prepared and tested for the first time for active and stable dehydrogenation of a formic acid–ammonium formate (FA–AF) mixture. The catalysts with different Au-to-Pd molar ratios were prepared using a facile simultaneous reduction method and characterized using transmission electron microscopy (TEM), high-resolution TEM, energy dispersive X-ray spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. It was found that the catalytic activity and stability of the Au3Pd1/C catalyst was the best. The initial turnover frequency for the dehydrogenation of the FA–AF mixture over the Au3Pd1/C catalyst can reach 407.5 h−1 at 365 K. The reaction order with respect to FA and AF is 0.25 and 0.55, respectively. The apparent activation energy of dehydrogenation is 23.3 ± 1.3 kJ mol−1. The catalytic activity of the Au3Pd1/C catalyst remains ca. 88.0% after 4 runs, which is much better than the single Pd/C catalyst. The mechanism for the dehydrogenation is also discussed.

The Au3Pd1/C catalyst shows better performance in a formic acid–ammonium formate mixture and the mechanism of dehydrogenation is discussed.  相似文献   

3.
The compatible catalytic structure of NiCo2O4 was modified into multi-shelled hollow spheres by one-pot synthesis, followed by heat treatment. X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and Brunauer–Emmet–Teller (BET) and N2 adsorption–desorption approaches were used for the characterizations of nanoparticles and multi-shelled hollow porous structures and the morphologies and crystal structures of these hollow spheres, respectively. Differential scanning calorimetry (DSC) was adopted for comparing the thermal decomposition performances of ammonium perchlorate (AP) catalyzed by adding different contents of multi-shelled NiCo2O4 hollow spheres. Impressively, the experimental results showed that the NiCo2O4 hollow spheres exhibited more excellent catalytic activity than NiCo2O4 nanoparticles as a result of their large specific surface areas, good adsorption capacity and many active reduction sites. The decomposition temperature of AP with multi-shelled NiCo2O4 hollow spheres could be reduced up to 322.3 °C from 416.3 °C. Furthermore, a catalytic mechanism was proposed for the thermal decomposition of AP over multi-shelled NiCo2O4 hollow spheres based on electron transfer processes.

Double-shelled NiCo2O4 hollow spheres synthesized by a facile hydro-thermal method showed excellent catalytic properties for the thermal decomposition of AP.  相似文献   

4.
High performance methane gas sensors have become more and more essential in different fields such as coal mining, kitchens and industrial production, which necessitates the design and synthesis of highly sensitive materials. Herein, mesoporous SnO2 hollow spheres with high surface area (>90 m2 g−1) are prepared by a progressive inward crystallization routine, showing a high response of 1.31 to 250 ppm CH4 at a working temperature of 400 °C. Furthermore, loading noble metal Pd onto the surface of SnO2 hollow spheres by an adsorption–calcination process improves the response to 4.88 (250 ppm CH4) at the optimal dosage of 1 wt% Pd. Meanwhile, the working temperature decreases to 300 °C, showing the prominent spillover effect of catalytic Pd and PdO–SnO2 heterostructure sensitization as evidenced by the binding energy shift in the X-ray photoelectron spectroscopy (XPS) analysis. The response/recovery time is as short as 3/7 s and the sensitivity is stable for a test period as long as 15 weeks. All these performances show the promise of the highly porous Pd-loaded SnO2 hollow spheres for high performance methane sensors.

This work reports a simple, rapid, effective and reliable CH4 sensor based on Pd-loaded SnO2 hollow spheres with high surface area and porosity, which is of great importance to gas sensing performance.  相似文献   

5.
Bifunctional electrocatalysts with high catalytic property for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are vital for high-performance zinc–air batteries (ZnABs). In this study, an efficient bifunctional electrocatalyst with hollow structure (C–N/Co (1/2)) has been successfully prepared through carbonization of ZIF-8@ZIF-67 and evaporation of Zn ions at high temperature. With Co nanoparticles encapsulated by an N-doped porous carbon matrix, the catalyst exhibits excellent stability in aqueous alkaline solution over an extended period and good tolerance to the methanol crossover effect. The integration of an N-doped graphitic carbon outer shell and Co nanoparticles enables high ORR and OER activity, as evidenced by ZnAB using the catalyst C–N/Co (1/2) in an air cathode.

An efficient bifunctional electrocatalyst with hollow structure (C–N/Co (1/2)) has been obtained through carbonization of ZIF-8@ZIF-67, which showed high ORR and OER activity, as evidenced by ZnAB using catalyst of C–N/Co (1/2) in air cathode.  相似文献   

6.
Electrocatalysts for the oxygen reduction reaction (ORR) are crucial in metal–air batteries, fuel cells and other electrochemical devices. In this study, iron and nitrogen co-doped carbon sphere electrocatalysts were synthesized by electrospinning and thermal treatment. According to the results, the catalyst marked as Fe–N/MCS-181 (Fe, N-doped mesoporous carbon spheres, iron nitrate nonahydrate as the iron source) has not only the highest iron content, which reaches up to 0.13%, but also a spherical shape. And its pore sizes are 11 and 35 nm. For the electrochemical performance, the onset potential (Eonset) of Fe–N/MCS-181 is −0.018 V, while the half-wave potential (E1/2) of Fe–N/MCS-181 is −0.145 V, which is better than the commercial Pt/C catalyst (E1/2 is −0.18 V). The durability of the Fe–N/MCS-181 catalyst is better than commercial Pt/C. After 10 000 s, the retention ratio of current density is 86.4%, while that of the commercial Pt/C catalyst is 84.2%. At the same time, the methanol tolerance of the Fe–N/MCS-181 catalyst is also excellent. After adding methanol, the current density of the Fe–N/MCS-181 catalyst has no obvious change. This study provides an easy method to fabricate a highly efficient and durable Fe, N-doped carbon catalyst for the oxygen reduction reaction.

Fe, N-doped carbon spheres as high-efficiency ORR catalysts were prepared by a facile electrospinning process.  相似文献   

7.
TiO2 hollow fibers (THF) were prepared by a template method using kapok as a biotemplate and subsequently decorated by plasmonic Au nanoparticles using a solution plasma process. The THF exhibited an anatase phase and a hollow structure with a mesoporous wall. Au nanoparticles with a diameter of about 5–10 nm were uniformly distributed on the THF surface. Au nanoparticles-decorated TiO2 hollow fibers (Au/THF) have enhanced photocatalytic activity toward methylene blue degradation under visible light-emitting diode (Vis-LED) as compared to pristine THF and P25. This could be attributed to combined effects including effective light-harvesting by a hollow structure, large surface area due to a mesoporous wall of THF, and visible-light absorption and efficient charge separation induced by Au nanoparticles. The Au/THF also showed good recyclability and separation ability.

Plasmonic Au nanoparticles-decorated TiO2 hollow fibers with enhanced visible-light photocatalytic activity have been successfully prepared by a two-step process: (i) template method using kapok and (ii) solution plasma process.  相似文献   

8.
In this work, we developed a thiol-functionalized poly(3,4-ethylenedioxythiophene) hollow sphere (poly(EDOT-MeSH)/Au) polymer through a simple one-pot self-assembly method using polyvinylpyrrolidone (PVP) as a soft template. The monomer was used as both a reductant and a stabilizer to decorate gold nanoparticles (Au NPs). FTIR, XRD, EDX, SEM and TEM analyses were used to characterize the composite hollow spheres. The chemical bond between S and Au was confirmed by XPS. The electrochemical performance of the composite hollow spheres was determined by cyclic voltammetry (CV) and an ampere response timing current test. The results revealed that the poly(EDOT-MeSH)/Au hollow-sphere-based electrochemical sensor possesses excellent conductivity and high redox reversibility with detection limits (S/N = 3) of 0.2, 0.02, 0.08 and 0.05 μM in the linear ranges of 0.1–650 μM, 0.05–100 μM and 0.1–600 μM for the determination of ascorbic acid (AA), dopamine (DA), uric acid (UA) and nitrate ions (NO2), respectively. The preparation method for these composites will further the development of this type of conducting polymer/gold nano-composite material modified electrochemical sensor for biological species.

In this work, we developed a thiol-functionalized poly(3,4-ethylenedioxythiophene) hollow sphere (poly(EDOT-MeSH)/Au) polymer through a simple one-pot self-assembly method using polyvinylpyrrolidone (PVP) as a soft template.  相似文献   

9.
Rhodium nanoparticles (≈3–5 nm) were incorporated into the 3D mesoporous TUD-1 material by using sol–gel technique. The prepared catalyst shows high activity in the liquid phase conversion of cyclohexene to cyclohexane at room temperature (298 K), 1 atm H2 pressure, and under solvent-free conditions. Rhodium nanoparticles exhibited high stability, reusability and negligible leaching.

Total conversion of cyclohexene to cyclohexane was achieved in a liquid phase hydrogenation reaction at room temperature, 1 atm H2 pressure and solvent-free system.  相似文献   

10.
A new strategy for controlled synthesis of a MOF composite with a core–shell structure, ZIF-8@resorcinol–urea–formaldehyde resin (ZIF@RUF), is reported for the first time through in situ growth of RUF on the surface of ZIF-8 nanoparticles via an organic–organic self-assembly process by using hexamethylenetetramine as a formaldehyde-releasing source to effectively control the formation rate of RUF, providing the best opportunity for RUF to selectively grow around the nucleation seeds ZIF-8. Compared with the widely reported method for MOF composite synthesis, our strategy not only avoids the difficulty of incorporating MOF crystals into small pore sized materials because of pore limitation, but also effectively guarantees the formation of a MOF composite with a MOF as the core. After carbonization, a morphology-retaining N-doped hierarchical porous carbon characterized by its highly developed microporosity in conjunction with ordered mesoporosity was obtained. Thanks to this unique microporous core–mesoporous shell structure and significantly enhanced porosity, simultaneous improvements of CO2 adsorption capacity and kinetics were achieved. This strategy not only paves a way to the design of other core–shell structured MOF composites, but also provides a promising method to prepare capacity- and kinetics-increased carbon materials for CO2 capture.

New strategy for controlled synthesis of core–shell structured ZIF-8 composite and hierarchical N-doped carbon via an effective in situ self-assembly process.  相似文献   

11.
PS@TiO2@Ag spheres with triple-level core–shell nanostructures were prepared via a versatile coating procedure based on an electroless-plating-like solution deposition (EPLSD) method. A peroxo-titanium-complex (PTC) aqueous solution was used as the precursor to react with an aniline monomer in the EPLSD preparation. Aniline plays an important role in the TiO2 layer anchoring process through the swollen effects of the PS cores. As extended, peroxo-metal-complex (PMC) with the d0 configuration can be introduced onto PS spheres to form varieties of PS@metal oxide core–shell structures by this method under mild conditions. Ag layers were then modified onto the PS@TiO2 spheres via the photocatalytic method. By the extraction of the PS cores, hollow TiO2 and TiO2@Ag spheres could be obtained. The photochemical degradation of methylene blue (MB) under UV light irradiation was performed on the composite nanostructures.

PS@TiO2@Ag spheres with a core–shell nanostructure were prepared by electroless-plating-like solution deposition (EPLSD) method, which can be alternatively extended to prepare PS@metal(1) oxide@metal(2) composite spheres and their relative hollow spheres.  相似文献   

12.
Transition metal oxides are commonly used in electrochemical energy storage materials, but there are still many drawbacks that impede a wide range of applications. Heteroatom doping can significantly improve its performance. Herein, we have successfully prepared highly uniform N-doped NiCo2O4@C hollow nanostructures for supercapacitors by a two-step hydrothermal treatment associated with successive annealing process. Prepared N-doped NiCo2O4@C materials exhibited an admirable specific capacitance of 1028 F g−1 at a current density of 3 A g−1, with 625 F g−1 remaining even at high current density of 20 A g−1. Besides, this composite showed good electrochemical stability with capacity retention of 84% after 5000 cycles repetitive galvanostatic charge–discharge test at 10 A g−1. An asymmetric supercapacitor was assembled by the N-doped NiCo2O4@C electrode, attached activate carbon (AC) as a counter electrode, exhibiting a high energy density of 26.67 W h kg−1 at a power density of 402 W kg−1. The improvement of electrochemical performance is ascribed to the co-doping of nitrogen and carbon atoms. These results indicate that N-doped NiCo2O4@C can be employed as an ideal electrode material for electrochemical energy storage.

Procedure for fabricating N-doped NiCo2O4@C hollow nanostructures.  相似文献   

13.
Nitrogen co-doping with ruthenium mesoporous carbons (Ru–N-MC) was prepared by co-impregnation of sucrose and urea on a RuCl3/SiO2 template followed by a thermal carbonization process. The turnover frequency (TOF) of the Ba/Ru–N-MC catalyst in ammonia synthesis is 0.16 s−1 under reaction conditions of 400 °C, pressure of 10 MPa and space velocity of 10 000 h−1. The superior catalytic performance of the Ba/Ru–N-MC is proposed to originate from the strong metal-support interaction between Ru nanoparticles (NPs) and carbon support. In addition to the activity, the Ba/Ru–N-MC catalyst exhibits a long-term stability for 35 h without significant deactivation.

A highly active and stable mesoporous Ba/Ru–N-MC catalyst for ammonia synthesis was prepared by an in situ thermal carbonization method with nitrogen co-doping with ruthenium NPs.  相似文献   

14.
Iron oxide based magnetic nanoparticles (MNPs) as typical theranostic nanoagents have been popularly used in various biomedical applications. Conventional core–shell MNPs are usually synthesized from inside to outside. This method has strict requirements on the interface properties of magnetic cores and the precursors of the coating shell. The shape and size of MNPs are significantly influenced by that of the pre-synthesized magnetic cores. Most core–shell MNPs have only single T2W MRI imaging ability. Herein, we propose a new synthetic strategy for core-mesoporous shell structural MNPs, where hollow mesoporous nanospheres which exhibit an intrinsic property for both CT imaging and drug loading were used as the shell and the magnetic cores were produced in the cavity of the shell. A new type of MNPs, Fe3O4@ZrO2 nanoparticles (M-MZNs), were developed using this facile outside-to-inside way, where multiple Fe3O4 nanoparticles grew inside the cavity of the mesoporous hollow ZrO2 nanospheres through chemical coprecipitation. The obtained MNPs not only exhibited superior magnetic properties and CT/MR imaging ability but also high drug loading capacity. In vitro experiment results revealed that M-MZNs-PEG loaded with doxorubicin (DOX) presented selective growth inhibition against cancer cells due to pH-sensitive DOX release and enhanced endocytosis by cancer cells under a magnetic field. Furthermore, the proposed MNPs exhibited CT/MRI dual modal imaging ability and effective physical targeting to tumor sites in vivo. More importantly, experiments of magnetic targeting chemotherapy on tumor bearing mice demonstrated that the nanocomposites significantly suppressed tumor growth without obvious pathological damage to major organs. Henceforth, this study provides a new strategy for CT/MRI dual-modal imaging guided and magnetic targeting cancer therapy.

Magnetic mesoporous zirconia nanoparticle was synthesized by producing multiple iron oxide cores inside the cavity of mesoporous ZrO2 hollow nanospheres and was used for CT/MRI dual-modal imaging and magnetic targeting chemotherapy.  相似文献   

15.
Oxygen reduction reaction (ORR) with efficient activity and stability is significant for fuel cells. Herein, platinum (Pt) nanoparticles dispersed on nitrogen-doped reduced graphene oxide (N-rGO) were prepared by a hydrothermal and carbonized approach for the electrocatalysis of ORR. Polyvinylpyrrolidone plays a significant role in the reduction and dispersion of platinum particles (about 2 nm). The obtained Pt–N-rGO hybrids exhibited superior activity with an electron transfer number of ∼4.0, onset potential 0.90 eV of ORR, good stability and methanol tolerance in alkaline media. These results reveal the interactions between Pt–N-rGO and oxygen molecules, which may represent an oxygen modified growth in catalyst preparation. The excellent electrocatalysis may lead to the decreased consumption of expensive Pt and open up new opportunities for applications in lithium air batteries.

We developed a facile, yet general approach to prepare ultrafine Pt nanoparticles loaded on N-doped reduced graphene (Pt–N-rGO) composites, which showed excellent oxygen reduction reaction performance.  相似文献   

16.
Microwave absorbents with specific morphology and structure have fundamental significance for tuning microwave absorption (MA). Herein, N-doped carbon sphere nanoparticles and hollow capsules were successfully fabricated via oxidative polymerization of dopamine in different mixed solutions, without any template preparation or etching process. Compared to solid particles, the microwave absorbents consisting of N-doped carbon with a hollow structure showed enormously enhanced MA performance, exhibiting a broad effective absorption bandwidth (from 12.7 GHz to 17.9 GHz) and a minimum reflection loss of −27.2 dB with a sample thickness of 2.0 mm. This work paves an attractive way for simple and eco-friendly preparation of advanced light weight microwave absorbents.

N-doped carbon particles were prepared through environmentally friendly and convenient methods. N-doped carbon capsules exhibit the best microwave absorption ability compared to their spherical counterparts.  相似文献   

17.
In situ electrochemical activation as a new pre-treatment method is extremely effective for enhanced electrocatalytic performances for different applications. With the help of this method, in situ surface modification of electrocatalyst is achieved without using pre-made seeds or complex synthesis procedure. Herein, with the purpose of finding an in situ and simple electrochemical activation protocol, the green synthesis of Au/Pd nanoparticles (AuPd) by means of polyoxometalate (POM) is reported. Structural analysis of the AuPd nanohybrid unveil the Au-core/Pd-shell structure which surrounded by POM. We propose a novel cathodic electrochemical activation in phosphate buffer solution which can greatly boost the electrocatalytic activity of the as-prepared AuPd and Pd electrocatalyst not only for hydrogen evolution reaction (HER) as a model of electro-reduction, but also for methanol and ethanol electro-oxidation reaction (MOR & EOR). For the HER in 1 M NaOH solution, after the electrochemical activation, the needed potential to drive a geometrical current density of 10 mA cm−2 significantly decreases from – 400 mV vs. the reversible hydrogen electrode (RHE) to −290 mV vs. RHE. For the EOR and MOR, electrochemically activated AuPd realized 3.4- and 2.9- fold increase in mass current density (mA mgPd−1) with respect to the pristine AuPd electrocatalyst, respectively.

In situ electrochemical activation as a new pre-treatment method is extremely effective for enhanced electrocatalytic performances for different applications.  相似文献   

18.
Lithium–oxygen (Li–O2) batteries as promising energy storage devices possess high gravimetric energy density and low emission. However, poor reversibility of electrochemical reactions at the cathode significantly affects the electrochemical properties of nonaqueous Li–O2 batteries, and low charge–discharge efficiency also results in short cycle-life. In this work, functional air cathodes containing mesoporous tungsten carbide nanoparticles for improving the reversibility of positive reactions in Li–O2 cells are designed. Mesoporous tungsten carbides are synthesized with mesoporous carbon nitride as the reactive template and carbon source. And mesoporous tungsten carbides in cathode materials display better electrochemical performance in Li–O2 cells in comparison with mesoporous carbon nitride and hard carbon. Tungsten carbide-1 (WC-1) with larger specific surface area promotes reversible formation and decomposition of Li2O2 at the cathode and lower charge overpotential (about 0.93 V) at 100 mA g−1, which allows the Li–O2 cell to run up to 100 cycles. In addition, synergistic interaction between WC-1 and LiI could further decrease the charging overpotentials of Li–O2 cells and improve the charge–discharge performances of the Li–O2 cells. These results indicate that mesoporous electrocatalysts can be utilized as promising functional materials for Li–O2 cells to decrease overpotentials.

Tungsten carbide with large specific surface area catalyzes reversible formation/decomposition of Li2O2 with low overpotential in a Li–O2 cell.  相似文献   

19.
In this study, mesoporous SiO2 nanoparticles (MSNs) were synthesized via a sol–gel method and modified with (3-chloropropyl) trimethoxysilane to make them hydrophobic (MMSNs). The material was characterized via SEM, TEM, FT-IR, DLS, BET and contact angle measurements. The MMSNs have good foam stability, so that the foam properties of the added particles have been increased by 38.4% in an oil/SDS solution. Simultaneously, it becomes a promising material for foam stabilization in order to enhance the oil recovery because it is bio-compatibile and environment friendly. Also, it provides a novel application-stable foam for mesoporous materials.

In this study, mesoporous SiO2 nanoparticles (MSNs) were synthesized via a sol–gel method and modified with (3-chloropropyl) trimethoxysilane to make them hydrophobic (MMSNs).  相似文献   

20.
Porous micro/nanostructure electrode materials have always contributed to outstanding electrochemical energy storage performances. Co9S8 is an ideal model electrode material with high theoretical specific capacity due to its intrinsic two crystallographic sites of cobalt ions. In order to improve the conductivity and specific capacitance of Co9S8, nickel ions were introduced to tune the electronic structure of Co9S8. The morphology design of the mesoporous hollow sphere structure guarantees cycle stability and ion diffusion. In this work, NixCo9−xS8 mesoporous hollow spheres were synthesized via a facile partial ion-exchange of Co9S8 mesoporous hollow spheres without using a template, boosting the capacitance to 1300 F g−1 at the current density of 1 A g−1. Compared with the pure Co9S8 and Ni-Co9S8-30%, Ni-Co9S8-60% exhibited the best supercapacitor performance, which was ascribed to the maximum Ni ion doping with morphology and structure retention, enhanced conductivity and stabilization of Co3+ in the structure. Therefore, Ni/Co–Zn batteries were fabricated by using a Zn plate as the anode and Ni-Co9S8-60% as the cathode, which deliver a high energy density of 256.5 W h kg−1 at the power density of 1.69 kW kg−1. Furthermore, the Ni/Co–Zn batteries exhibit a stable cycling after 3000 repeated cycles with capacitance retention of 69% at 4 A g−1. This encouranging result might provide a new perspective to optimize Co9S8-based electrodes with superior supercapacitor and Ni/Co–Zn battery performances.

Mesoporous NiCo9S8-0.6 hollow spheres as a high-performance supercapacitor and aqueous Ni/Co–Zn battery.  相似文献   

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