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1.
Gold nanoparticles have shown excellent activity for selective oxidation of alcohols; such catalytic systems are highly dependent on the initial activation of the substrates, which must occur on the catalyst surface in heterogeneous catalysts. In many cases, an extra base addition is required, although the basicity of the support may also be of significant importance. Here, we explored the intrinsic basicity of magnesium-based enrichments on CoFe2O4 magnetic nanoparticles for the oxidation of benzyl alcohol using molecular oxygen as oxidant. The MgO and Mg(OH)2 enrichments enabled gold impregnation, which was not possible on the bare CoFe2O4 nanoparticles. The Au/MgO/CoFe2O4 and Au/Mg(OH)2/CoFe2O4 catalysts reached 42% and 18% conversion, respectively without base promotion, in 2.5 hour and 2 bar of O2. When the catalysts were tested with sub-stoichiometric amounts of base, they became more active (>70% of conversion) and stable in successive recycling experiments without metal leaching, under the same reaction conditions. We also showed the oxide phases of the enrichments performed using Rietveld refinements and how the Mg(OH)2 phase interferes with the activity of MgO-based materials.

Gold nanoparticles have shown excellent activity for selective oxidation of alcohols; such catalytic systems are highly dependent on the initial activation of the substrates, which must occur on the catalyst surface in heterogeneous catalysts.  相似文献   

2.
In this work, we have successfully prepared core–shell nanoparticles (Fe3O4@PDA) wrapped with Ag using a simple and green synthesis method. Without an external reducing agent, silver nanoparticles (Ag NPs) with good dispersibility were directly reduced and deposited on a polydopamine (PDA) layer. Fe3O4@PDA@Ag showed excellent catalytic activity and recyclability for 4-nitrophenol, and also exhibited good catalytic selectivity for organic dyes (MO and MB). This simple and green synthesis method will provide a platform for other catalytic applications.

In this work, we have successfully prepared core–shell nanoparticles (Fe3O4@PDA) wrapped with Ag using a simple and green synthesis method.  相似文献   

3.
Herein, we report the preparation of magnetic CoFe2O4 nanoparticles and CoFe2O4/graphene oxide (GO) hybrids and evaluate their catalytic activity as heterogeneous peroxymonosulfate (PMS) activators for the decomposition of rhodamine B. The surface morphologies and structures of both CoFe2O4 nanoparticles and CoFe2O4/GO hybrids were investigated by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), Fourier transform infrared spectroscopy (FTIR) and nitrogen adsorption–desorption isotherms. The magnetic properties of the samples were assessed using a SQUID magnetometer at 298 K. Catalytic oxidation experiments demonstrated that CoFe2O4/GO hybrids exhibited much better catalytic activity than CoFe2O4 nanoparticles or CoFe2O4/reduced graphene oxide (rGO) hybrids, suggesting that GO plays an important role in CoFe2O4/GO hybrids in the decomposition of rhodamine B. The influence of various reaction conditions such as temperature, concentration of PMS, pH and decomposition time of rhodamine B over the CoFe2O4/GO catalyst were investigated and optimized. The rhodamine B degradation process was found to fit a pseudo-first order kinetics model. The catalyst could be easily separated from the reaction mixture by applying an external magnet. In particular, the as-prepared CoFe2O4/GO hybrid exhibited good reusability and stability in successive degradation experiments in PMS solution.

Herein, we report the preparation of magnetic CoFe2O4 nanoparticles and CoFe2O4/graphene oxide (GO) hybrids and evaluate their catalytic activity as heterogeneous peroxymonosulfate (PMS) activators for the decomposition of rhodamine B.  相似文献   

4.
A composite of Ni nanoparticles incorporated in Kryptofix 22 conjugated magnetic nano-graphene oxide, CoFe2O4@GO–K 22·Ni, was synthesized via the grafting of Kryptofix 22 moieties on the magnetic nano-graphene oxide surface, followed by reaction of the nanocomposite with nickel nitrate. The Kryptofix 22 host material unit cavities can stabilize the Ni nanoparticles effectively and prevent their aggregation and separation from the surface. Characterization of the catalysts by FT-IR, FE-SEM, TGA, ICP, EDX, XRD, VSM and BET aided understanding the catalyst structure and morphology. This catalyst was efficiently applied for the synthesis of 1,4-benzodiazepine derivatives. The main advantages of the method are mild reaction conditions, inexpensive catalyst, it is environmentally benign, has high to excellent yields and shorter reaction times. This organometallic catalyst can be easily separated from a reaction mixture and was successfully examined for six runs with a slight loss of catalytic activity.

In this study, a competent and efficient methodology for the synthesis of benzodiazepine over magnetically retrievable novel CoFe2O4@GO–K 22 anchored Ni is reported.  相似文献   

5.
The purpose of this work was to prepare a new Ni–carboxamide complex supported on CoFe2O4 nanoparticles (CoFe2O4/SiO2–NH2@carboxamide–Ni). The carboxamide host material unit generated cavities that stabilized the nickel nanoparticles effectively and prevented the aggregation and separation of these particles on the surface. This compound was appropriately characterized using FT-IR spectroscopy, FE-SEM, ICP-OES, EDX, XRD, TGA analysis, VSM, and X-ray atomic mapping. The catalytic oxidation of sulfides and oxidative coupling of thiols in the presence of the designed catalyst was explored as a highly selective catalyst using hydrogen peroxide (H2O2) as a green oxidant. The easy separation, simple workup, excellent stability of the nanocatalyst, short reaction times, non-explosive materials as well as appropriate yields of the products are some outstanding advantages of this protocol.

The preparation of a Ni–carboxamide complex supported on CoFe2O4 for the oxidation of sulfides and oxidative coupling of thiols.  相似文献   

6.
We report a facile solvothermal synthesis of novel octahedral CoFe2O4–reduced graphene oxide (RGO) hybrid and pure CoFe2O4 that were used as heterogeneous photo-Fenton catalysts for the degradation of organic dyes in water. We investigated the structures, morphologies and catalytic activity of both the CoFe2O4 nanoparticles and CoFe2O4–RGO hybrids. The morphology of CoFe2O4 nanoparticles displays size-dependent shapes changing from granular (or sheet) to octahedral shapes with the introduction of RGO. Compared with bare CoFe2O4, the octahedral CoFe2O4–RGO hybrids serve as novel bifunctional materials displaying higher saturation magnetization values and excellent heterogeneous activation of H2O2 at nearly neutral pH. The high saturation magnetization (41.98 emu g−1) of CoFe2O4–RGO hybrids aids their separation from the reaction mixture. In addition, the remarkable enhancement in the photo-Fenton activity of the CoFe2O4–RGO hybrids under visible light irradiation was attributed to the graphene/CoFe2O4 heterojunction, which aided the separation of excited electrons and holes. Furthermore, the CoFe2O4–RGO hybrids exhibited better removal efficiency for cationic methylene blue (MB) dye than for anionic methyl orange (MO) dye. Meanwhile, the CoFe2O4–RGO hybrids displayed acceptable photocatalytic stability, and we proposed an activation mechanism of H2O2 by the octahedral CoFe2O4–RGO hybrids.

Schematic illustration of an active heterogeneous photo-Fenton mechanism based on CoFe2O4–RGO hybrids.  相似文献   

7.
Precious metal nanometric catalysts are widely used in the removal of harmful substances. In the process of synthesis and catalytic reaction, it is particularly important to study green and simple synthesis methods and high catalytic efficiency. In this paper, a green one-step method was used to synthesize the Fe(OH)3/Fe2O3@Au composite catalyst, in which Au was single atom-dispersed. The removal of 4-nitrophenol (4-NP), a typical dangerous chemical widely existing in factory waste gas, waste water and automobile exhaust gas, was catalysed by Fe(OH)3/Fe2O3@Au. The catalytic performance of Fe(OH)3/Fe2O3@Au with different synthesis conditions (different amounts of MES, NaBH4, FeSO4, Au and Pt) on the 4-NP reduction reaction were systematically studied. Finally, the stability and recyclability of Fe(OH)3/Fe2O3@Au composite nanocatalyst were investigated thoroughly.

The process of the catalytic reduction of 4-nitrophenol based on single atom-dispersed Au loaded with ultrathin Fe(OH)3/Fe2O3 nanosheets.  相似文献   

8.
In this paper, CoFe2O4/graphene catalysts and N-doped graphene/CoFe2O4 (CoFe2O4/graphene-N) catalysts were prepared using the hydrothermal crystallization method for the selective catalytic reduction of NOx by NH3. The results of the test showed that CoFe2O4/graphene catalysts exhibited the best denitrification activity when the loading was at 4% and the conversion rate of NOx reached 99% at 250–300 °C. CoFe2O4/graphene-N catalysts presented a better denitrification activity at low temperature than CoFe2O4/graphene catalysts, and the conversion rate of NOx reached more than 95% at 200–300 °C. The intrinsic mechanism of CoFe2O4/graphene-N catalysts in promoting SCR activity was preliminarily explored. The physicochemical properties of the samples were characterized using XRD, TEM, N2 adsorption, XPS, NH3-TPD, and H2-TPR. The results indicated that nitrogen doping can improve the dispersion of CoFe2O4, and it also increased the acidic sites and the redox performance conducive to improving the denitrification activity of the catalysts. In addition, CoFe2O4/graphene-N catalysts demonstrated a better resistance to water and sulfur than CoFe2O4/graphene catalysts.

N-doped graphene/CoFe2O4 presented better denitrification activity than CoFe2O4/graphene due to the more uniform distribution of CoFe2O4 and acidic sites etc.  相似文献   

9.
Photoluminescent (PL) metal and metal oxide nanoclusters (NCs), with a size of just several nanometers, are a separate class of nanomaterials abundant with new attractive optical, physical, and chemical properties and biocompatibility. However, the synthesis of PL magnetic NCs via attachment of PL NCs to iron oxide-based nanoparticles (NPs) is still problematic. Motivated by this, herein, we report the development of a microwave-driven conjugation approach of red-fluorescent gold nanoclusters (BSA@AuNCs) to superparamagnetic NPs. Synthesized CoFe2O4@AuNCs possess strong photoluminescence in water and ethanol media as well as good colloidal and optical stability, and magnetization response. High-resolution transmission electron microscopy (HRTEM), steady-state and time-resolved photoluminescence spectroscopy, X-ray powder diffraction (XRD), and magnetic measurements from ambient to cryogenic temperatures were applied for structural characterization and evaluation of optical and magnetic properties of the synthesized species.

We report the study of gold clusters'' attachment to magnetic nanoparticles by microwave processing for red-luminescent magnetic species formation.  相似文献   

10.
A magnetically separable CoFe2O4/Cu(OH)2 nanocomposite was prepared and characterized by various techniques such as FESEM, EDS, TEM, XRD, VSM and FT-IR. This novel composite was used as a heterogeneous catalyst for the regioselective synthesis of β-hydroxy-1,4-disubstituted-1,2,3-triazoles from sodium azide, terminal alkynes and structurally different epoxides in water at 60 °C. The formation of the product proceeds in one pot through a mechanism that involves an in situ generated organic azide intermediate, followed by rapid ring closure with the alkyne component. The simple procedure, short reaction times, perfect regioselectivity, high product yields, and use of a benign solvent and nontoxic catalyst are among the considerable advantages of this protocol. Furthermore, the catalyst was easily separated using an external magnet and reused several times without any significant loss of catalytic activity or magnetic properties.

Magnetically separable CoFe2O4/Cu(OH)2 nanocomposite was prepared and used as a novel heterogeneous catalyst for synthesis of β-hydroxy-1,4-disubstituted-1,2,3-triazoles from epoxides.  相似文献   

11.
Nitrogen-doped graphene quantum dots (N-GQDs), which are less than 10 nm in size, are an interesting member of the nanocarbon materials family. N-GQDs nanostructures have been broadly applied in various fields, such as drug-gene delivery systems, photocatalytic reactions, and catalysts, owing to their unique properties. However, N-GQDs have rarely been introduced as a catalyst in organic synthesis. Herein, CoFe2O4 nanocomposites with diverse morphologies are fabricated in various conditions (e.g. green routes, various pH adjusters, temperatures). Due to further active sites on the surface of the nanocomposites, morphology engineering can be effective in catalytic activities. Following the synthesis, the catalytic activity of the engineered CoFe2O4 nanocomposites was screened, and it presented the order of spherical > rod > prism > cubic. The uniform spherical morphology provides more accessible active sites. Then, the novel nano-sized N-GQDs/CoFe2O4 magnetic spherical composite was readily fabricated by a green, low-cost, and easy hydrothermal route. The engineered composite was applied as an efficient magnetic nanocatalyst for the MW-assisted one-pot synthesis of new and known quinoline-3-carbonitrile derivatives (83–96%) in the shortest reaction time (60–90 s). Furthermore, the green route, easy separation of the nanocatalyst, and reusability (7 runs) without noticeable loss of catalytic efficiency are other advantages.

Sustainable fabrication of spherical N-GQDs/CoFe2O4 nanocomposites as a novel magnetically retrievable catalyst for the synthesis of quinoline-3-carbonitrile derivatives has been developed.  相似文献   

12.
In this work, Au/GdPO4-rods were found to be good catalysts for CO oxidation with a low content of Au. The dopant of CePO4 could influence the activity of Au/GdPO4 due to the synergistic effect. GdPO4 and CePO4 nanorods were obtained by a hydrothermal process and the Au/GdPO4-rod and Au/Ce-GdPO4-rod catalysts were prepared by deposition–precipitation synthesis. The samples were extensively characterized by transmission electron microscopy (TEM), inductively coupled plasma (ICP), powder X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), ultraviolet-visible spectroscopy (UV-Vis), Fourier transform infrared spectroscopy (FT-IR), temperature programmed desorption (O2-TPD, CO-TPD, and CO2-TPD) and N2 adsorption–desorption. The results showed that Au/GdPO4 with a low Au content possessed good activity for CO oxidation. When the content of Ce is 25 at%, 0.5% Au/Ce-GdPO4-rods can convert CO completely at 65 °C, and the catalyst showed better high-temperature resistance than 0.5% Au/GdPO4-rods. 0.5% Au/Ce-GdPO4-rods also showed good stability at reaction temperatures of 55 and 65 °C with CO conversions of 90% and 100% after continuous operation for 12 h. They also showed no deactivation after 50 h at a relative high reaction temperature of 200 °C.

A CePO4–GdPO4 composite was prepared by a general ultrasound method and could be a good support for gold nanocatalysts. Au/CePO4–GdPO4 catalysts with a low content of gold showed good catalytic activity, high temperature resistance and stability for CO oxidation.  相似文献   

13.
CoFe3O4 nanoparticles supported on multi-walled carbon nanotubes (MWCNTs-CoFe3O4) were synthesized by the co-precipitation method as a novel catalyst for degradation of diclofenac (DCF). The comparative experiments indicated that MWCNTs-CoFe3O4 has a better catalytic activity in degradation of DCF and activation of peroxymonosulfate (PMS) compared to other catalytic systems. This can be attributed to the interaction of MWCNTs with CoFe3O4 in accelerating the absorption process and activating the PMS (Ea = 22.93 kJ mol−1). The removal efficiencies of DCF and total organic carbon (TOC) were 99.04% and 50.11%, under optimum conditions, e.g., pH of 7, PMS dosage of 4 mM, DCF concentration of 30 mg L−1, catalyst dosage of 500 mg L−1, and reaction time of 120 min. The oxidation of DCF was fitted by the pseudo-first-order kinetic model and the constant rate was increased by increasing the pH, temperature, dosage of PMS and catalyst. The production of reactive species was studied using scavengers such as TBA and ethanol and the results showed that sulfate radical is the reactive species responsible for the degradation of DCF. The MWCNTs-CoFe3O4 catalyst showed high stability and reusability based on five successful repeated reactions, X-ray diffraction and energy dispersive X-ray spectroscopy analysis. Based on the intermediates detected by gas chromatography-mass spectrometry (GC-MS), the possible pathways for DCF catalytic oxidation were proposed. The results explained that the PMS/MWCNTs-CoFe3O4 system is a promising method for treating DCF solution due to high efficiency, good reusability of catalyst and greater PMS activation.

The MWCNTs-CoFe3O4 as a novel catalyst showed high catalytic activity in activation of proxymonosulfate for degradation of diclofenac.  相似文献   

14.
Ultrathin two-dimensional (2D) metal–organic framework (MOF) nanosheets were prepared by a facile sonication exfoliation of MOF membranes from interfacial growth. The stacked form of nanosheets constituting the MOF membranes was significantly different to that of its layered MOF counterparts. This led to decreased interaction between nanosheets, so they could exfoliate readily from the MOF membranes. Moreover, Au nanoparticles were introduced to form nanocomposites. Enhanced catalytic activity and long-term stability of these nanocomposites were observed by a model reaction of the reduction of 4-nitrophenol to 4-aminophenol. This preparation method could be extended to other 2D MOF nanosheets and their nanocomposites.

Cu-MOF nanosheets were prepared by sonication exfoliation and the Au/Cu-MOF nanocomposites exhibited higher catalytic activity than pure Au NPs.  相似文献   

15.
In this work, a novel catalytic system for facilitating the organic multicomponent synthesis of 9-phenyl hexahydroacridine pharmaceutical derivatives is reported. Concisely, this catalyst was constructed from acacia gum (gum arabic) as a natural polymeric base, iron oxide magnetic nanoparticles (Fe3O4 NPs), and sulfone functional groups on the surface as the main active catalytic sites. Herein, a convenient preparation method for this nanoscale composite is introduced. Then, essential characterization methods such as various spectroscopic analyses and electron microscopy (EM) were performed on the fabricated nano-powder. The thermal stability and magnetic properties were also precisely monitored via thermogravimetric analysis (TGA) and vibrating-sample magnetometry (VSM) methods. Then, the performance of the presented catalytic system (Fe3O4@acacia–SO3H) was further investigated in the referred organic reaction by using various derivatives of the components involved in the reaction. Optimization, mechanistic studies, and reusability screening were carried out for this efficient catalyst as well. Overall, remarkable reaction yields (94%) were obtained for the various produced derivatives of 9-phenyl hexahydroacridine in the indicated optimal conditions.

We designed and fabricated a novel catalytic system with high heterogeneity and magnetic features to facilitate the MCR synthetic reactions of 9-phenyl hexahydroacridine pharmaceutical derivatives.  相似文献   

16.
CoFe2O4/ZnO magnetic nanocatalysts were synthesized using a low-frequency ultrasound-assisted technique to enhance the optical, morphological, magnetic and catalytic properties of ZnO. The as-synthesized nanocatalysts were characterized by XRD, Raman, TEM, DR-UV-Vis and VSM analyses in order to confirm the expected modifications of the resulting nanocatalysts. The Raman spectral analysis revealed substitutional Zn2+ in the CoFe2O4/ZnO nanocatalyst. The as-synthesized material was tested for its catalytic activity in the degradation of Acid Blue (AB113), a known textile pollutant. The CoFe2O4 and CoFe2O4/ZnO nanocatalysts revealed the efficient catalytic degradation of AB113 in ambient conditions. The nanocatalyst dosage and the initial concentration of AB113 were varied by fixing one parameter as constant in order to determine the maximum catalytic efficiency with the minimum catalyst loading for AB113 degradation. The CoFe2O4/ZnO nanocatalyst demonstrated 10-fold enhanced mineralization of AB113 compared to the individual bare nanocatalysts, which could be achieved within 3 hours of catalytic degradation of AB113. The magnetic CoFe2O4/ZnO nanocatalyst was found to be stable for six consecutive recycles of AB113 degradation, which indicates that the catalytic efficiency of the nanocatalyst was retained after various numbers of cycles.

CoFe2O4/ZnO magnetic nanocatalysts were synthesized using a low-frequency ultrasound-assisted technique to enhance the optical, morphological, magnetic and catalytic properties of ZnO.  相似文献   

17.
A S–N co-doped CoFe2O4@rGO@TiO2 (CFGT-S/N) nanocomposite was successfully synthesized via a facile vapor-thermal method. XRD, XPS, FT-IR and FETEM results confirmed that N and S were co-doped into the lattice of TiO2. Photocatalytic tests indicated that CFGT-S/N exhibited excellent UV-Vis photocatalytic activity for decompositions of different organic dyes, including methyl orange (MO), rhodamine B (RhB) and methylene blue (MB). Particularly, the photocatalytic degradation rate of MO was about 33% higher than that when using P25 under visible light irradiation. The higher UV-Vis light photocatalytic activity of CFGT-S/N can be attributed to the synergetic effects of the strong absorption of visible light, the narrow band gap, improved separation of photo-generated electron/hole pairs, and the enhancement of the enrichment of pollutant dye molecules by S, N co-doping, CoFe2O4 and rGO. Moreover, this photocatalyst was superparamagnetic, which enables it to be easily recovered by an external magnetic field, and maintained stable photocatalytic efficiency over five cycles. Hence, CFGT-S/N with its highly efficient, recoverable and stable photocatalytic properties shows great potential for environmental treatment.

A magnetic recoverable S–N co-doped CoFe2O4@rGO@TiO2 (CFGT-S/N) nanocomposite was synthesized via a facile vapor-thermal method. CFGT-S/N is an excellent UV-Vis photocatalyst because of the synergetic effects of S, N co-doping, the introduction of CoFe2O4 and rGO.  相似文献   

18.
A novel strategy for the synthesis of highly stable gold nanoparticles (GNPs) was designed by reducing HAuCl4 with NaBH4 in an aqueous solution of water-soluble ionic cellulose composed of dimethylimidazolium cations and phosphite-bound cellulose anions. NMR and UV-Vis analysis along with the measurement of the zeta potential suggest that the exceptionally high stability of GNPs originates from the strong interaction of GNPs with the phosphite groups of the ionic cellulose. The thus prepared GNPs exhibit excellent catalytic activity for the reduction of 4-nitrophenol to 4-aminophenol, a model hydrogenation reaction.

Gold nanoparticles (GNP) were highly stabilized by water soluble ionic cellulose by the strong interaction of GNP with the phosphite groups and showed extremely high catalytic activity for the reduction of 4-nitrophenol to 4-aminophenol.  相似文献   

19.
Here we present a magnetic recyclable photo-Fenton catalyst CoFe2O4@PPy with uniform morphology and excellent dispersibility prepared via simple in situ Fenton oxidization polymerization. The CoFe2O4 core provides good magnetic recyclability for the catalysts as well as the ion source for catalyzed decomposition of H2O2 in PPy coating. The optimal catalytic effect can be obtained by adjusting the ratio of CoFe2O4 and PPy. Methylene blue, Methyl orange and Rhodamine B (RhB) employed as model pollutants certificated that the catalyst exhibits a wide range of photodegradability. The decoloration rates reach nearly 100% in the photodegradation of 10 mg L−1 RhB after 2 h visible-light irradiation and only low toxicity small molecules are detected by LC-MS. Moreover, the catalytic activity remains after 5 cycles with decoloration rates up to 90%. The degradation measurement in the presence of scavengers of reactive species reveals that the positive holes (h+) and hydroxyl radical (·OH) are the main reactive oxygen species in the CoFe2O4@PPy system. The performance enhancement may be attributed to the combination of improved Fenton activity by coordinated Fe2+ and PPy redox pairs and photo-catalytic activity by broaden adsorption and photo-generated charge separation.

Here we present a magnetic recyclable photo-Fenton catalyst CoFe2O4@PPy with uniform morphology and excellent dispersibility prepared via simple in situ Fenton oxidization polymerization.  相似文献   

20.
The green synthesis of palladium nanoparticles (Pd NPs) for catalysis and biological applications has been gaining great interest. To replace complex plant extracts, lentinan (LNT) may be a good reducing and stabilizing agent. In this work, a simple and green method using LNT to reduce and stabilize palladium Pd NPs was verified. The resulting LNT stabilized palladium nanoparticles (Pdn-LNT NPs) were characterized by UV-Vis spectroscopy, DLS, TEM, and XPS. The results indicated that Pd NPs inside of Pdn-LNT NPs had a small size (2.35–3.32 nm). Pdn-LNT NPs were stable in solution for 7 days. In addition, Pdn-LNT NPs had higher catalytic activity towards the reduction of 4-nitrophenol than other catalysts. More importantly, Pdn-LNT NPs had negligible cytotoxicity towards cells and showed good antioxidant activity. Taken together, the prepared Pdn-LNT NPs have great potential bio-related applications.

Lentinan stabilized palladium nanoparticles had high catalytic activity, negligible cytotoxicity and good antioxidant activity.  相似文献   

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