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1.
以磷钼酸、 2-氨基吡啶、 五氧化二钒、 氯化锌和氯化镍等为主要原料, 采用水热方法合成了2个簇基超分子化合物[H3PMo12O40]2[C5H6N2]6(1)和[H2PMo12V2O42][C5H6N2]5·3H2O(2)(C5H6N2=2-氨基吡啶). 通过元素分析、 红外光谱、 紫外-可见光谱、 X射线光电子能谱、 热重分析、 X射线单晶衍射及X射线粉末衍射等手段对化合物进行了结构表征. 结构分析显示, 簇单元不同的2个超分子化合物以各自独特的堆积方式形成三维超分子网络. 利用苯乙烯的环氧化反应研究了2个化合物的催化性能.  相似文献   

2.
钠具有资源丰富、成本低廉等优势,因此钠离子电池被认为是未来替代锂离子电池的最佳候选者之一。然而,寻找合适的电极材料是当前制备高性能钠离子电池面临的难题之一。在众多候选材料中,钒酸盐材料通过引入阳离子增加钒的配位数,使得材料结构的稳定性得到提高,从而改善了钠离子电池的电化学性能。本文研究了一种原位相分离法合成V_2O_5/Fe_2V_4O_(13)纳米复合材料。通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)、傅里叶变换红外光谱(FTIR)等对电极材料形貌、组成和结构进行了表征。实验结果显示,V_2O_5/Fe_2V_4O_(13)纳米复合材料相对于V2O5纳米线材料,结构更加稳定,在0.1 A·g~(-1)电流密度下,初始放电容量由295.4 m Ah·g~(-1)提升到342 m Ah·g~(-1),循环100圈容量保持率由26.6%提高到65.8%,获得了更加优异的倍率性能(在1.0 A·g~(-1)电流密度下,容量由44 m Ah·g~(-1)提高到160 m Ah·g~(-1))。因此,V_2O_5/Fe_2V_4O_(13)纳米复合材料的研究为开拓新型高性能钠离子电池负极材料拓宽了思路。  相似文献   

3.
将DNA功能化多壁碳纳米管(MWCNTs)复合材料修饰于玻碳基底(GC)表面制得DNA-MWCNTs/GC电极,并在此基础上电沉积负载Pt纳米颗粒构建了一种新型无酶H2O2传感电极. 利用扫描电子显微镜(SEM)表征制得的修饰电极,同时通过循环伏安法和计时电流法研究了该传感电极的H2O2响应性能. 结果表明,该传感电极的H2O2检测在0.04 ~ 18.07 mmol·L-1浓度范围内成线性相关,检出限3.85 μmol·L-1(S/N = 3),且有良好的重现性、稳定性与选择性.  相似文献   

4.
H3PW12O40/TiO2 nanometer photocatalyst was prepared by one step hydrothermal synthesis from H3PW12O40′nH2O and Ti(OBu)4,simultaneously realizing the load and modification of H3PW12O40.The catalyst was ...  相似文献   

5.
The compound [Zn(H2O)4]2[H2As6V15O42(H2O)]·2H2O (1) has been synthesized and characterized by elemental analysis, IR, ESR, magnetic measurement, third-order nonlinear property study and single crystal X-ray diffraction analysis. The compound 1 crystallizes in trigonal space group R3, a=b=12.0601(17) Å, c=33.970(7) Å, γ=120°, V=4278.8(12) Å3, Z=3 and R1(wR2)=0.0512 (0.1171). The crystal structure is constructed from [H2As6V15O42(H2O)]4− anions and [Zn(H2O)4]2+ cations linked through hydrogen bonds into a network. The [H2As6V15O42(H2O)]6− cluster consists of 15 VO5 square pyramids linked by three As2O5 handle-like units.  相似文献   

6.
在0 到12 mL·L-1 (体积分数φ=0.00%-1.20%) 范围内考察了不同H2S 浓度对25% (质量分数, w)MoO3/Al2O3和5% (w) CoO-25%MoO3/Al2O3催化剂甲烷化性能的影响. 结果表明, 5%CoO-25%MoO3/Al2O3的甲烷化活性随H2S浓度的增加单调上升, 而25%MoO3/Al2O3对H2S浓度并不敏感. 对比这两种催化剂发现, 只有在H2S浓度高于0.40% (φ) 时, 在25%MoO3/Al2O3中添加Co助剂才会有促进作用; H2S浓度低于0.40% (φ)时, Co助剂会抑制25%MoO3/Al2O3催化剂的甲烷化活性. 分别对反应前后的催化剂表征发现, H2S浓度的改变不会对两种催化剂的物理结构产生明显的影响, 而是通过影响催化剂表面的金属硫化物活性位来影响催化剂的甲烷化性能. 耐硫甲烷化反应体系中较高的硫含量下Co助剂才表现出对25%MoO3/Al2O3催化剂的促进作用. 该研究明确了在MoO3/Al2O3催化剂中添加Co助剂的硫化氢浓度范围, 为工业上选择合适的催化剂提供了依据.  相似文献   

7.
Customizing core-shell nanostructures is considered to be an efficient approach to improve the catalytic activity of metal nanoparticles. Various physiochemical and green methods have been developed for the synthesis of core-shell structures. In this study, a novel liquid-phase hydrogen reduction method was employed to form core-shell Pt@Au nanoparticles with intimate contact between the Pt and Au particles, without the use of any protective or structure-directing agents. The Pt@Au core-shell nanoparticles were prepared by depositing Au metal onto the Pt core; AuCl4− was reduced to Au(0) by H2 in the presence of Pt nanoparticles. The obtained Pt@Au core-shell structured nanoparticles were characterized by transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDX), high-resolution TEM, fast Fourier transform, powder X-ray diffraction (PXRD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), and H2-temperature programmed reduction (H2-TPR) analyses. The EDX mapping results for the nanoparticles, as obtained from their scanning transmission electron microscopy images in the high-angle annular dark-field mode, revealed a Pt core with Au particles grown on its surface. Fourier transform measurements were carried out on the high-resolution structure to characterize the Pt@Au nanoparticles. The lattice plane at the center of the nanoparticles corresponded to Pt, while the edge of the particles corresponded to Au. With an increase in the Au content, the intensity of the peak corresponding to Pt in the FTIR spectrum decreased slowly, indicating that the Pt nanoparticles were surrounded by Au nanoparticles, and thus confirming the core-shell structure of the nanoparticles. The XRD results showed that the peak corresponding to Pt shifted gradually toward the Au peak with an increase in the Au content, indicating that the Au particles grew on the Pt seeds; this trend was consistent with the FTIR results. Hence, it can be stated that the Pt@Au core-shell structure was successfully prepared using the liquid-phase hydrogen reduction method. The catalytic activity of the nanoparticles for the oxidation of toluene was evaluated using a fixed-bed reactor under atmospheric pressure. The XPS and H2-TPR results showed that the Pt1@Au1/Al2O3 catalyst had the best toluene oxidation activity owing to its lowest reduction temperature, lowest Au 4d & 4f and Pt 4d & 4f binding energies, and highest Au0/Auδ+ and Pt0/Pt2+ proportions. The Pt1@Au2Al2O3 catalyst showed high stability under dry and humid conditions. The good catalytic performance and high selectivity of Pt@Au/Al2O3 for toluene oxidation could be attributed to the high concentration of adsorbed oxygen species, good low-temperature reducibility, and strong interaction.  相似文献   

8.
A pure inorganic [P2Mo5O23]6- based cobalt complex [H8(H2O)16][Co(H2O)4(HP2Mo5O23)2] with a sandglass-like shape was synthesized and characterized by means of single-crystal X-ray diffraction, powder X-ray diffraction(PXRD), infrared spectroscopy(IR), thermogravimetry/differential scanning calorimetry(TG/DSC), ultraviolet-visible spectroscopy(UV-Vis) and cyclic voltammogram(CV). Single-crystal X-ray diffraction analysis reveals that the asymmetric unit of compound 1 consists of a half cobalt ion, one [P2Mo5O23]6- anion, two coordinated water molecules and eight lattice water molecules. It is especially intriguing to note that two [P2Mo5O23]6- clusters are symmetrical about the Co ion, like a sandglass. And a chair-like water cluster with an unprecedented centrosymmetric [H8(H2O)16]8+ can be observed in compound 1. Additionally, the electrochemical and catalytic properties of compound 1 were also investigated.  相似文献   

9.
采用分步浸渍法制备了系列Mg改性的Co/γ-Al_2O_3-TiO_2催化剂,通过X射线衍射(XRD)、紫外可见漫反射光谱(DR-UV-vis)、N_2吸附-脱附(BET)、X射线光电子能谱(XPS)和H_2程序升温还原(H_2-TPR)等技术对催化剂进行表征,并考察了其对丙烷燃烧的催化性能。结果表明,Co在原始γ-Al_2O_3-TiO_2载体和Mg改性MgO/γ-Al_2O_3-TiO_2载体上均以Co_3O_4的形式存在;Mg掺入后与Al_2O_3作用形成MgAl_2O_4尖晶石,改善了载体的织构性质,提升了Co_3O_4在催化剂载体表面的暴露数量和分散程度。此外,MgAl_2O_4与Co_3O_4相互作用提升了Co_3O_4颗粒表面Co~(3+)/Co~(2+)和O_(ads)/O_(latt)的比例,并削弱了Co-O键键能,从而提升了其对丙烷的催化燃烧活性。当Mg负载量为15%(质量分数)时,在Co/MgO(15%)/γ-Al_2O_3-TiO_2催化剂上进行丙烷燃烧,丙烷90%转化率的温度比无Mg掺杂的Co/γ-Al_2O_3-TiO_2催化剂的降低了45℃,并且连续反应40 h其活性保持稳定。  相似文献   

10.
Different from the traditional pyrometallurgical recovery process of Li and Co from spent lithium-ion batteries, a new recovery method for Li and Co was established by converting LiCoO2 into water-soluble metal sulfates by roasting a mixture of LiCoO2 and NaHSO4·H2O. The evolution law of the mixture with increased roasting temperature was investigated by thermogravimetry-differential scanning calorimetry(TG-DSC), in situ X-ray diffraction(XRD), XRD, and X-ray photoelectron spectroscopy(XPS). The results show that the phase transition of LiCoO2 mixed with NaHSO4·H2O with increased temperature proceeded as follows:LiCoO2, NaHSO4·H2O→LiCoO2, NaHSO4→Li1-xCoO2, LiNaSO4, Na2S2O7, Na2SO4→Li1-xCoO2, Co3O4, LiNaSO4, Na2SO4→Co3O4, LiNaSO4. The reaction mechanism of this roasting process may be as follows:LiCoO2+NaHSO4·H2O→1/2Li2SO4+ 1/2Na2SO4+1/3Co3O4+1/12O2+3/2H2O, Li2SO4+Na2SO4=2LiNaSO4.  相似文献   

11.
Aseries of Ni catalysts supported on alumina with different Ce contents(1.0%-6.0%, mass fraction) was prepared by the impregnation method and used for dry reforming of methane(DRM) at a relatively low temperature of 650 oC. The promotion effect of Ce with different loading amounts on the physicochemical properties of the catalysts was systematically characterized by transmission electron microscopy(TEM), X-ray diffraction(XRD), N2 adsorption-desorption, thermo elemental IRIS Intrepid inductively coupled plasma atomic emission spectrometer (ICP-AES), UV-visible diffuse reflectance spectroscopy(UV-Vis DRS), Fourier transformation infrared(FTIR) spectra, H2-temperature programmed reduction(H2-TPR) analysis, H2-temperature programmed desorption(H2-TPD), and the X-ray photoelectron spectroscopy(XPS) techniques. The results indicate that all the catalysts mainly exist in the NiAl2O4 phase after being calcined at 750 oC with small Ni particle sizes due to the strong metal-support interaction derived from the reduction of the NiAl2O4 phase. The Ce-promoted catalysts show better catalytic performance as well as the resistance against sintering of Ni particles and deposition of carbon compared to the Ni/Al2O3 catalyst. The Ni-6Ce/Al2O3 exhibits the best catalytic stability and coke resistance among the four catalysts studied, which is due to its small Ni nanoparticles sizes, excellent reducibility as well as high amount of active oxygen species. In a 400 h stability test for DRM reaction at 650 oC, Ni-6Ce/Al2O3 exhibits less coke deposition and small growth of Ni nanoparticles. This work provides a simple way to preparing the Ni-Ce/Al2O3 catalyst with enhanced catalytic performance in DRM. The Ni-6Ce/Al2O3 catalyst has great potential for industrial application due to its anti-sintering ability and resistance to carbon deposition.  相似文献   

12.
采用共沉淀法,用助剂TiO2对CuO-ZnO-Al2O3催化剂改性,TiO2由钛酸正丁酯水解而得,并考察了其在CO2催化加氢制甲醇反应中的催化性能.在反应温度260℃、压力2.6 MPa、H2∶CO2 =3∶1(体积比)、SV=3600 mL/(g·h)条件下,与空白样CuO-ZnO-Al2O3比较,结果显示,TiO2...  相似文献   

13.
Mixtures of NaHSO4·H2O and LiCoO2 extracted from spent lithium-ion batteries were prepared with molar ratios of 1:1, 1:2 and 1:3. The chemical evolution of the LiCoO2 and NaHSO4·H2O mixtures during the roasting process was investigated by means of thermogravimetric analysis and differential scanning calorimetry (TG-DSC), X-ray diffraction(XRD), scanning electron microscopy(SEM), and X-ray photoelectron spectroscopy (XPS). The results show that the chemical reactions in the LiCoO2 and NaHSO4·H2O mixtures proceed during the roasting process. The Li element in the product of the roasting process is in the form of LiNa(SO4). With the increase of the proportion of NaHSO4·H2O in the mixtures, the Co element evolves as follows: LiCoO2→Co3O4→ Na6Co(SO4)4→Na2Co(SO4)2. The roasting products exhibit dense structures and irregular shapes, and the bonding energy of Co increases.  相似文献   

14.
采用溶胶-凝胶法制备了不同Pr掺杂量的Pr6O11-TiO2载体, 并以浸渍法制备了V2O5-MoO3/Pr6O11-TiO2催化剂. 活性评价结果表明, 该催化剂在220~400 ℃范围内具有良好的脱硝效率和N2选择性以及较强的抗SO2和H2O性能. 表征结果表明, 掺杂Pr可以提高V2O5-MoO3/TiO2催化剂的比表面积、 表面化学吸附氧物种浓度、 桥式硝酸盐物种和Brönsted酸位数量, 从而提高了催化剂上NOx的选择性催化还原(NH3-SCR)活性.  相似文献   

15.
采用模板法制备了CuO-CeO2-SiO2和稀土掺杂的CuO-Ce0.9M0.1O2-SiO2 (M=La, Pr, Nd)催化剂. 运用X射线衍射(XRD), N2吸附-脱附, 透射电镜(TEM), 拉曼(Raman)光谱, X射线光电子能谱(XPS)和氢气-程序升温还原(H2-TPR)等手段对催化剂的结构进行表征, 并考察稀土掺杂对氯化氢催化氧化制氯气性能的影响. 结果表明, 稀土掺杂进入CeO2晶格中形成良好的固溶体结构, 获得更小的晶粒尺寸和更高的比表面积, 并且显著提高了固溶体的表面氧空位浓度. 稀土掺杂显著影响了催化剂的氯化氢催化氧化活性, 活性顺序为: CuOCe0.9La0.1O2-SiO2>CuO-Ce0.9Nd0.1O2-SiO2>CuO-Ce0.9Pr0.1O2-SiO2>CuO-CeO2-SiO2, 固溶体氧空位浓度的高低与氯化氢氧化活性直接相关. 通过与Ce0.9M0.1O2-SiO2催化剂的结构和性能的对比, 发现氧空位浓度的提高并不能增强在固溶体表面发生的氯化氢氧化反应. 动力学测试显示, 稀土掺杂后, 氧分子的吸附成为反应过程的决速步骤. 但在V(O2):V(HCl)=1 条件下, 更高的氧空位浓度导致了固溶体更低的氯化氢氧化反应速率. 结合机理分析认为, CuO-Ce0.9M0.1O2-SiO2催化剂更高的氧空位浓度增强了固溶体表面的“氧溢流”, 加快了氯化氢氧化的整体反应速率, 这是CuO-Ce0.9M0.1O2-SiO2具备高活性的关键.  相似文献   

16.
采用分步共沉淀法制备了不同Al2O3含量(0%-15% (w))的CuO/Fe2O3催化剂, 并进行水煤气变换反应(WGSR)评价测试. 制得的催化剂中含有复合物CuFe2O4, 其晶粒尺寸, 氧化还原性质和表面Cu分散通过相应表征手段加以研究. X 射线粉末衍射(XRD), 拉曼(Raman)光谱, N2物理吸附, N2O分解和CO2程序升温脱附(CO2-TPD)等表征技术说明适量Al2O3的加入可以促进尖晶石CuFe2O4发生由四方相向立方相的转变, 阻止催化剂中Cu烧结, 增大表面Cu分散, 增加弱碱性位点的数量. 此外, 采用H2程序升温还原(H2-TPR)技术探究改性的CuO/Fe2O3催化剂的还原性能. 关联结果发现, Al2O3掺杂在增大铜物种的耗氢量, 降低其还原温度方面起着重要的作用. 即Al2O3的添加促进CuO/Fe2O3催化剂中铜铁物种之间的协同作用. 结合活性测试和表征结果,适量的Al2O3 (10%(w))改性的催化剂具有较小的Cu颗粒尺寸、较大的Cu分散、较强的还原性能、较多数量的弱碱性位点, 因此具有更好的初始活性和热稳定性.  相似文献   

17.
Developing enzyme-free sensors with high sensitivity and selectivity for H2O2 and glucose is highly desirable for biological science.Especially,it is attractive to exploit noble-metal-free nanomaterials with large surface area and good conductivity as highly active and selective catalysts for molecular detection in enzyme-free sensors.Herein,we successfully fabricate hollow frameworks of Co3O4/N-doped carbon nanotubes(Co3O4/NCNTs)hybrids by the pyrolysis of metal-organic frameworks followed by calcination in the air.The as-prepared novel hollow Co3O4/NCNTs hybrids exhibit excellent electrochemical performance for H2O2 reduction in neutral solutions and glucose oxidation in alkaline solutions.As sensor electrode,the Co3O4/NCNTs show excellent non-enzymatic sensing ability towards H2O2 response with a sensitivity of 87.40μA(mmol/L)^-1 cm^-2,a linear range of 5.00μmol/L-11.00 mmol/L,and a detection limitation of 1μmol/L in H2O2 detection,and a good glucose detection performance with 5μmol/L.These excellent electrochemical performances endow the hollow Co3O4/NCNTs as promising alternative to enzymes in the biological applications.  相似文献   

18.
采用水热法合成了一种微球状的CuS/Ag2S纳米复合物. 通过透射电子显微镜、 紫外-可见吸收光谱和拉曼光谱等对其形貌及光学性质进行了表征; 考察了其类过氧化物酶性质, 并通过表面增强拉曼散射原位监测了类过氧化物酶催化反应. 以3,3',5,5'-四甲基联苯胺(TMB)为底物进行显色反应, 结果表明, 在H2O2存在下CuS/Ag2S 纳米复合物具有类过氧化物酶的性质, 可以将无色的TMB氧化成蓝色的oxTMB. 基于此实现了对微量H2O2的检测.  相似文献   

19.
Two new layered lanthanide sulfates,[C10H10N2][Pr2(SO4)4(H2O)2](1)and[H5O2][Sm(SO4)2(H2O)3](2)were synthesized via solvothermal reaction and structurally characterized by single-crystal X-ray diffraction(XRD), infrared(IR) spectroscopy, thermal analysis, fluorescent spectra and inductively coupled plasma(ICP). Crystal data for compound 1, triclinic, P space group, a=0.8052(4) nm, b=0.9438(4) nm, c=1.4990(7) nm, α=79.450(5)°, β= 83.703(5)°, γ=74.048(5)°, V=1.0746(9) nm3, Z=2; for compound 2, monoclinic, P21/c space group, a=0.6599(11) nm, b=1.8940(3) nm, c=0.8765(14) nm, β=96.596(2)°, V=1.0883(3) nm3, Z=4. Structure analysis indicates that both the compounds exhibit a 2D corrugated layer structure, with protonated 4,4'-bipyridine cations and water dimmers (H5O2)+ located between the inorganic layers of compounds 1 and 2, respectively. Luminescent properties of compounds 1 and 2 were further investigated.  相似文献   

20.
In this study, a novel silicon carbide/platinum/cadmium sulfide (SiC/Pt/CdS) Z-scheme heterojunction nanorod is constructed using a simple chemical reduction-assisted hydrothermal method, in which Pt nanoparticles are anchored at the interface of SiC nanorods and CdS nanoparticles to induce an electron-hole pair transfer along the Z-scheme transport path. Multiple characterization techniques are used to analyze the structure, morphology, and properties of these materials. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) results show that the SiC/Pt/CdS materials with good crystal structure are successfully synthesized. Transmission electron microscopy reveals that Pt nanoparticles grow between the interfaces of SiC nanorods and CdS nanoparticles. UV-Vis diffuse reflectance spectroscopy shows that the as-prepared Z-scheme heterojunction samples have a wider light absorption range in comparison with pristine CdS materials. Photoluminescence spectroscopy and the transient photocurrent response further demonstrate that the SiC/Pt/CdS nanorod sample with an optimal molar ratio possesses the highest electron-hole pair separation efficiency. The loading amount of CdS on the surface of SiC/Pt nanorods is effectively adjusted by controlling the molar ratio of SiC and CdS to achieve the optimal performance of the SiC/Pt/CdS nanorod photocatalysts. The optimal H2 evolution capacity is achieved at SiC : CdS = 5 : 1 (molar ratio) and the maximum H2 evolution rate reaches a high value of 122.3 µmol·h−1. In addition, scanning electron microscopy, XRD, and XPS analyses show that the morphology and crystal structure of the SiC/Pt/CdS photocatalyst remain unchanged after three cycles of activity testing, indicating that the SiC/Pt/CdS nanocomposite has a stable structure for H2 evolution under visible light. To prove the Z-scheme transfer mechanism of electron-hole pairs, selective photo-deposition technology is used to simultaneously carry out the photo-reduction deposition of Au nanoparticles and photo-oxidation deposition of Mn3O4 nanoparticles in the photoreaction. The experimental results indicate that during photocatalysis, the electrons in the conduction band of CdS participate mainly in the reduction reaction, and the holes in the valence band of SiC are more likely to undergo the oxidation reaction. The electrons in the conduction band of SiC combine with the holes in the valence band of CdS to form a Z-scheme transport path. Therefore, a possible Z-scheme charge migration path in SiC/Pt/CdS nanorods during photocatalytic H2 production is proposed to explain the enhancement in the activity. This study provides a new strategy for synthesizing a Z-scheme photocatalytic system based on SiC nanorods. Based on the characterization results, it is determined that SiC/Pt/CdS nanocomposites are highly efficient, inexpensive, easy to prepare, and are stable structures for H2 evolution under visible light with outstanding commercial application prospects.  相似文献   

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