首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 218 毫秒
1.
Heterogeneous Au-Pt nanostructures have been synthesized using a sacrificial template-based approach. Typically, monodispersed Au nanoparticles are prepared first, followed by Ag coating to form core-shell Au-Ag nanoparticles. Next, the galvanic replacement reaction between Ag shells and an aqueous H(2)PtCl(6) solution, whose chemical reaction can be described as 4Ag + PtCl(6)(2-)→ Pt + 4AgCl + 2Cl(-), is carried out at room temperature. Pure Ag shell is transformed into a shell made of Ag/Pt alloy by galvanic replacement. The AgCl formed simultaneously roughens the surface of alloy Ag-Pt shells, which can be manipulated to create a porous Pt surface for oxygen reduction reaction. Finally, Ag and AgCl are removed from core-shell Au-Ag/Pt nanoparticles using bis(p-sulfonatophenyl)phenylphosphane dihydrate dipotassium salt to produce heterogeneous Au-Pt nanostructures. The heterogeneous Au-Pt nanostructures have displayed superior catalytic activity towards oxygen reduction in direct methanol fuel cells because of the electronic coupling effect between the inner-placed Au core and the Pt shell.  相似文献   

2.
Core-shell Au-Pt nanoparticles with intimate contact of Pt and Au were prepared by a displacement reaction without formation of monometallic Au nanoparticles. The Au-Pt nanoparticles were dispersed on carbon (Au@Pt/C) and were used to catalyze methanol electrooxidation in acidic solutions at room temperature. The core-shell nanostructure was confirmed by transmission electron microscopy and X-ray photoelectron spectroscopy, and specific catalytic activities were evaluated by CO anodic stripping voltammetry in 0.5 M H(2)SO(4) and by cyclic voltammetry in 1 M CH(3)OH + 0.5 M H(2)SO(4). The Au@Pt/C catalyst demonstrated enhanced specific activity in methanol electrooxidation and showed multiple CO stripping peaks which were all negatively shifted with respect to a similarly prepared Ag@Pt/C catalyst. The activity enhancement is attributed to the presence of Au underneath a very thin Pt shell where electron exchange between Au and Pt had promoted the formation of active oxygen species on Pt, which facilitated the removal of inhibiting CO-like reaction intermediates.  相似文献   

3.
制备了不同Pt/Au原子比的活性炭负载Au-Pt催化剂(Au-Pt/C),研究了Au/Pt原子比对Au-Pt/C催化剂氧还原电催化性能和抗甲酸性能的影响.结果表明,与Au/C催化剂相比,Au-Pt/C具有更好的电催化性能.当Pt/Au原子比从0/50增加到2/48时,Au-Pt/C催化剂表现出良好的氧还原电催化性能和抗...  相似文献   

4.
Au-Pt bimetallic nanoclusters on a thin film of Al(2)O(3)/NiAl(100) undergo significant structural evolution on variation of the temperature. Au and Pt deposited sequentially from the vapor onto thin-film Al(2)O(3)/NiAl(100) at 300 K form preferentially bimetallic nanoclusters (diameter ≦ 6.0 nm and height ≦ 0.8 nm) with both Au and Pt coexisting at the cluster surface, despite the order of metal deposition. These bimetallic clusters are structurally ordered, have a fcc phase and grow with their facets either (111) or (001) parallel to the θ-Al(2)O(3)(100) surface. Upon annealing the clusters to 400-500 K, the Au atoms inside the clusters migrate toward the surface, resulting in formation of a structure with a Pt core and an Au shell. Annealing the sample to 500-650 K reorients the bimetallic clusters--all clusters have their (001) facets parallel to the oxide surface--and induces oxidation of Pt. Such annealed bimetallic clusters become encapsulated with the aluminium-oxide materials and a few Au remain on the surface.  相似文献   

5.
核-壳结构Au-Pt纳米粒子的光谱表征和电催化性能   总被引:7,自引:0,他引:7  
用化学还原法合成了核-壳结构Au-Pt纳米粒子.紫外可见光谱(UV-Vis)、电化学循环伏安(CV)和透射电子显微镜(TEM)表征结果指出,所合成的核-壳结构Au-Pt纳米粒子为球形,平均直径为27 nm.以CO为分子探针,结合透射红外光谱研究,发现CO以孪生吸附态形式(COT)吸附在Au-Pt纳米粒子上,在2110 cm-1和2063 cm-1附近分别给出对称和反对称红外吸收峰. CV研究结果指出Au-Pt/GC电极对CO的氧化有较高的催化活性,起始氧化电位较本体Pt电极提前了0.45 V,峰电位提前了0.11 V.  相似文献   

6.
This paper describes a rapid, simple and one-step method for preparing silica coated gold (Au@SiO2) nanoparticles with fine tunable silica shell thickness and surface functionalization of the prepared particles with different groups. Monodispersed Au nanoparticles with a mean particle size of 16 nm were prepared by citrate reduction method. Silica coating was carried out by mixing the as prepared Au solution, tetraethoxysilane (TEOS) and ammonia followed by microwave (MW) irradiation. Although there are several ways of coating Au nanoparticles with silica in the literature, each of these needs pre-coating step as well as long reaction duration. The present method is especially useful for giving the opportunity to cover the colloidal Au particles with uniform silica shell within very short time and forgoes the use of a silane coupling agent or pre-coating step before silica coating. Au@SiO2 nanoparticles with wide range of silica shell thickness (5-105 nm) were prepared within 5 min of MW irradiation by changing the concentration of TEOS only. The size uniformity and monodispersity were found to be better compared to the particles prepared by conventional methods, which were confirmed by dynamic light scattering and transmission electron microscopic techniques. The prepared Au@SiO2 nanoparticles were further functionalized with amino, carboxylate, alkyl groups to facilitate the rapid translation of the nanoparticles to a wide range of end applications. The functional groups were identified by XPS, and zeta potential measurements.  相似文献   

7.
Poly(N‐vinyl‐2‐pyrolidone) protected Pt‐core bimetallic Pt/Au‐shell (Pt@Pt/Au) nanoparticles were prepared by multi‐step reduction of HAuCl4 and H2PtCl6 alternately by hydrogen adsorbed on platinum atom. Transmission electronic microscopy (TEM) and x‐ray diffraction (XRD) were used to characterize Pt@Pt/Au nanoparticles. The structure of the shell of the nanoparticles seems to be the Au‐Pt solid solution.  相似文献   

8.
In order to develop a chemical technique for the recovery of gold (Au) and platinum (Pt) in the metallic state from spent catalysts, e.g., catalysts for environmental protection and automobile and petroleum catalysts, the coprecipitation behaviors of Au(III) and Pt(IV) complex ions with Fe(OH)(2) as a scavenging and reducing agent were investigated. The Au(III) complex ions were found to be stoichiometrically and rapidly reduced to metallic Au due to electron transfer in acidic aqueous solution prior to coprecipitation with Fe(OH)(2). Conversely, Pt(IV) complex ions were reduced only after coprecipitation with Fe(OH)(2) due to electron transfer through a Pt(IV)-O-Fe(II) bond on the solid Fe(OH)(2). Using this chemical technique, Au and Pt can be selectively and effectively recovered in the metallic state.  相似文献   

9.
The synthesis, structure, spectroscopic characterization and electrical resistivity of the [EtV](2)[Fe(4)Pt(CO)(16)], [EtV][Fe(3)Pt(3)(CO)(15)].THF, [EtV][Fe(4)Au(CO)(16)](2)2.THF (EtV=1,1'-diethyl-4,4'-bipyridilium cation) and [NEt(4)](2)[Fe(4)Au(CO)(16)] is reported. The crystal structure of [EtV](2)[Fe(4)Pt(CO)(16)] is based on infinite stacks of [(EtV)(*+)](2) pi-dimers rotated by 90 degrees and isolated [Fe(4)Pt(CO)(16)](2-) ions. Within each pi-dimer, the [EtV](*+) radical ions are perfectly eclipsed and the distance between their mean planes is 3.275 A. The EPR spectrum of the solid material at room temperature clearly indicates the presence of a significantly populated triplet state of the pi-dimer, by showing signals both at Deltam=1 and Deltam=2. The solid-state structure of [EtV][Fe(3)Pt(3)(CO)(15)].THF is based on the ionic packing of [EtV](2+) and [Fe(3)Pt(3)(CO)(15)](2-) ions, inferred from a comparison of their molecular parameters with literature data. Significant electron transfer could have been expected to give [EtV](*+)[Fe(3)Pt(3)(CO)(15)](*-) on the basis of their formal redox potentials. In spite of their different stoichiometries, the structures of [EtV][Fe(4)Au(CO)(16)](2).2 THF and [NEt(4)](2)[Fe(4)Au(CO)(16)] both contain an isomer of the monoanion [Fe(4)Au(CO)(16)](-) in solution (previously characterized in the solid state as a [NMe(3)CH(2)Ph](2)[Fe(4)Au(CO)(16)]Cl mixed salt). Resistivity measurements on pellets of powdered samples of the above compounds indicate that their tetrasubstituted ammonium salts, and complex [EtV][Fe(4)Au(CO)(16)](2)2.THF, largely behave as insulators. However, the [EtV](2)[Fe(4)Pt(CO)(16)] and [EtV][Fe(3)Pt(3)(CO)(15)].THF samples respectively display resistivities 3 and 4 orders of magnitude less than those of their corresponding ammonium salts and could be classified as semiconductor materials.  相似文献   

10.
The reaction of Pt(2)(dba)(3) (dba = bis-dibenzylidene acetone) dispersed in room temperature 1-n-butyl-3-methylimidazolium (BMI) hexafluorophosphate ionic liquid with molecular hydrogen (4 atm) at 75 degrees C leads to stable and isolable nanometric Pt(0) particles. The X-ray diffraction analysis (XRD) of the material indicated that it is constituted of Pt(0). Transmission electron microscopy (TEM) analysis of the particles dispersed in the ionic liquid shows the formation of [Pt(0)](n) nanoparticles of 2.0-2.5 nm in diameter. A detailed examination of the nanoparticles imbibed in the ionic liquid and their environment shows an interaction of the BMI.PF(6) ionic liquid with the Pt(0) nanoparticles. The isolated [Pt(0)](n) nanoparticles can be redispersed in the ionic liquid or in acetone or used in solventless conditions for liquid-liquid biphasic, homogeneous, or heterogeneous hydrogenation of alkenes and arenes under mild reaction conditions (75 degrees C and 4 atm). The recovered platinum nanoparticles can be reused as a solid or redispersed in the ionic liquid several times without any significant loss in catalytic activity.  相似文献   

11.
To prepare silica-coated hematite particles without agglomeration, the effects of solid fraction, ion content in solution, and designed layer thickness on agglomeration and dispersion behavior after silica coating were examined. Since the ion concentration remained high in suspension after the hematite particles were prepared, these particles formed aggregates by the compression of an electric double layer on the hematite and silica layer produced a solid bridge between primary hematite particles. Silica bridge formation and agglomeration were almost completely prevented by decreasing the ion concentration and solid fraction of the hematite particles. Furthermore, the effects of the silica-layer thickness and structure on the reduction of hematite to iron under hydrogen gas flow and the iron core stability under air were discussed. When the solid fraction was low in suspension to prevent agglomeration during coating, a densely packed structure of nanoparticles formed by heterogeneous nucleation was observed on the silica-layer surface. Since this structure could not completely prevent oxide diffusion, the layer thickness was increased to 40 nm to obtain a stable iron core under air. Although a dense uniform layer was produced at a high solid fraction during coating, its thickness was reduced to 20 nm to completely reduce hematite to iron.  相似文献   

12.
In this work, we utilize the galvanic displacement synthesis and make it a general and efficient method for the preparation of Au-M (M = Au, Pd, and Pt) core-shell nanostructures with porous shells, which consist of multilayer nanoparticles. The method is generally applicable to the preparation of Au-Au, Au-Pd, and Au-Pt core-shell nanostructures with typical porous shells. Moreover, the Au-Au isomeric core-shell nanostructure is reported for the first time. The lower oxidation states of Au(I), Pd(II), and Pt(II) are supposed to contribute to the formation of porous core-shell nanostructures instead of yolk-shell nanostructures. The electrocatalytic ethanol oxidation and oxygen reduction reaction (ORR) performance of porous Au-Pd core-shell nanostructures are assessed as a typical example for the investigation of the advantages of the obtained core-shell nanostructures. As expected, the Au-Pd core-shell nanostructure indeed exhibits a significantly reduced overpotential (the peak potential is shifted in the positive direction by 44?mV and 32?mV), a much improved CO tolerance (I(f)/I(b) is 3.6 and 1.63 times higher), and an enhanced catalytic stability in comparison with Pd nanoparticles and Pt/C catalysts. Thus, porous Au-M (M = Au, Pd, and Pt) core-shell nanostructures may provide many opportunities in the fields of organic catalysis, direct alcohol fuel cells, surface-enhanced Raman scattering, and so forth.  相似文献   

13.
基于SnO2为修饰层的Au-Pt / SnO2 / Au复合电极研究   总被引:1,自引:0,他引:1  
用真空镀膜法在Au电极上沉积SnO2薄膜,在HAuCl4和H2PtCl4的混合溶液中利用直接还原法,将Au-Pt双金属纳米颗粒组装在SnO2 / Au电极上,得到Au-Pt / SnO2 / Au复合电极。采用SEM、TEM、XPS及CV曲线测定对Au-Pt / SnO2 / Au复合电极进行了表征。结果表明:复合电极上双金属纳米颗粒分布均匀,粒子粒径约为25 nm左右。SnO2作为修饰层以配位键与双金属纳米粒子结合。Au-Pt / SnO2 / Au复合电极具有良好对甲醇氧化的电化学性能。  相似文献   

14.
The catalytic performance of cluster-derived PtFe/SiO(2) bimetallic catalysts for the oxidation of CO has been examined in the absence and presence of H(2) (PROX) and compared to that of Pt/SiO(2). PtFe(2)/SiO(2) and Pt(5)Fe(2)/SiO(2) samples were prepared from PtFe(2)(COD)(CO)(8) and Pt(5)Fe(2)(COD)(2)(CO)(12) organometallic cluster precursors, respectively. FTIR data indicate that both clusters can be deposited intact on the SiO(2) support. The clusters remained weakly bonded to the SiO(2) surface and could be extracted with CH(2)Cl(2) without any significant changes in their structure. Subsequent heating in H(2) led to complete decarbonylation of the supported clusters at approximately 350 degrees C and the formation of Pt-Fe nanoparticles with sizes in the 1-2 nm range, as indicated by HRTEM imaging. A few larger nanoparticles enriched in Pt were also observed, indicating that a small fraction of the deposited clusters were segregated to the individual components following the hydrogen treatment. A higher degree of metal dispersion and more homogeneous mixing of the two metals were observed during HRTEM/XEDS analysis with the cluster-derived samples, as compared to a PtFe/SiO(2) catalyst prepared through a conventional impregnation route. Furthermore, the cluster-derived PtFe(2)/SiO(2) and Pt(5)Fe(2)/SiO(2) samples were more active than Pt/SiO(2) and the conventionally prepared PtFe/SiO(2) sample for the oxidation of CO in air. However, substantial deactivation was also observed, indicating that the properties of the Pt-Fe bimetallic sites in the cluster-derived samples were altered by exposure to the reactants. The Pt(5)Fe(2)/SiO(2) sample was also more active than Pt/SiO(2) for PROX with a selectivity of approximately 92% at 50 degrees C. In this case, the deactivation with time on stream was substantially slower, indicating that the highly reducing environment under the PROX conditions helps maintain the properties of the active Pt-Fe bimetallic sites.  相似文献   

15.
Surfaces of hexagonally packed silica spheres have been functionalized with silanes containing different hydrocarbon or fluorocarbon chains. The resulting chemical and physical structures were studied to establish the effect of surface hydrophobicity on the measured contact angles on the rough surfaces. The results were used to assess the effects of surface modifications on the parameters in the Cassie equation. To achieve superhydrophobicity via a biomimetic approach, we created two-scale structures by first forming hexagonally packed SiO2 spheres, followed by Au deposition on the spheres and heat treatment to form Au nanoparticles on sphere surfaces. Contact angles over 160 degrees were achieved. This work provides improved understanding of the effect of the surface roughness and solid surface fraction on superhydrophobicity.  相似文献   

16.
Chen YD  Zhang LY  Shi LX  Chen ZN 《Inorganic chemistry》2004,43(23):7493-7501
Reaction of Pt(diimine)(edt) (edt = 1,2-ethanedithiolate) with M(2)(dppm)(2)(MeCN)(2)(2+) (dppm = bis(diphenylphosphino)methane) gave heterotrinuclear complexes [PtCu(2)(edt)(mu-SH)(dppm)(3)](ClO(4)) (11) and [PtCu(2)(diimine)(2)(edt)(dppm)(2)](ClO(4))(2) (diimine = 2,2'-bpyridine (bpy), 12; 4,4'-dibutyl-2,2'-bipyridine (dbbpy), 13; phenanthroline (phen), 14; 5-bromophenanthroline (brphen), 15) when M = Cu(I). The reaction, however, afforded tetra- and trinuclear complexes [Pt(2)Ag(2)(edt)(2)(dppm)(2)](SbF(6))(2) (17) and [PtAu(2)(edt)(dppm)(2)](SbF(6))(2) (21) when M = Ag(I) and Au(I), respectively. The complexes were characterized by elemental analyses, electrospray mass spectroscopy, (1)H and (31)P NMR, IR, and UV-vis spectrometry, and X-ray crystallography for 14, 17, and 18. The Pt(II)Cu(I)(2) heterotrinuclear complexes 11-15 exhibit photoluminescence in the solid states at 298 K and in the frozen acetonitrile glasses at 77 K. It is likely that the emission originates from a ligand-to-metal charge transfer (dithiolate-to-Pt) (3)[p(S) --> d(Pt)] transition for 11 and from an admixture of (3)[d(Cu)/p(S)-pi(diimine)] transitions for 12-16. The Pt(II)(2)Ag(I)(2) heterotetranuclear complexes 17 and 18 are nonemissive in the solid states and in solutions at 298 K but show photoluminescence at 77 K. The Pt(II)Au(I)(2) heterotrinuclear complexes 19-21, however, are luminescent at room temperature in the solid state and in solution. Compounds 19 and 20 afford negative solvatochromism associated with a charge transfer from an orbital of a mixed metal/dithiolate character to a diimine pi orbital.  相似文献   

17.
SnO2-TiO2薄膜载体对Au-Pt纳米颗粒电化学性能的影响   总被引:1,自引:1,他引:0  
采用真空镀膜法在玻碳(GC)电极表面修饰SnO2-TiO2薄膜, 在SnO2-TiO2/GC复合电极表面组装Au-Pt双金属纳米颗粒, 制得Au-Pt/SnO2-TiO2/GC复合电极. 通过循环伏安法(CV)研究了SnO2-TiO2薄膜载体对Au-Pt双金属纳米颗粒电化学性能的影响; 采用扫描电镜(SEM)及X射线光电子能谱(XPS)对Au-Pt在SnO2-TiO2薄膜沉积的形貌及结构进行了表征. 研究结果表明, 10 nm的Au-Pt双金属纳米颗粒均匀地组装于SnO2-TiO2薄膜表面; SnO2-TiO2薄膜载体改善了复合电极抗CO中毒能力; Au-Pt双金属合金的形成提高了Pt 对甲醇氧化的电催化能力, SnO2-TiO2薄膜载体又使Pt纳米粒子d空轨道增多, 提高了Au-Pt双金属纳米颗粒的稳定性和催化性能.  相似文献   

18.
The tridentate dianionic ligand 2-[2'-(hydroxyisopropoxyphosphoryl)phenylsulfanyl]benzoate (L(2-)) reacts with cis-[Pt(NH(3))(2)(H(2)O)(2)](2+) to form an S,O-chelate in which the O-coordinated group is either carboxylate or phosphonate, depending on the degree of protonation of the complex. Carboxylate appears to be the stronger ligand, and the stoichiometric reaction between cis-[Pt(NH(3))(2)(H(2)O)(2)](2+) and L(2-) yields the neutral species [Pt(L)(NH(3))(2)], with L bound by sulfanyl and carboxylate groups, both in solution and in the solid state. Upon protonation of [Pt(L)(NH(3))(2)], the stronger basicity of the carboxylate causes the Pt coordination to switch from carboxylate to phosphonate, and the uncoordinated carboxylate group becomes protonated. In methanolic solution, the first-order kinetics of this rearrangement could be observed by (31)P NMR spectroscopy. Both complexes-the carboxylate-bound neutral complex [Pt(L)(NH(3))(2)].H(2)O (triclinic, P1 (no. 2), a=9.529(6), b=9.766(6), c=12.299(7) angstroms, alpha=106.91(2), beta=101.71(2), gamma=102.05(2) degrees, Z=2) and the perchlorate salt of the phosphonate-bound complex [Pt(LH)(NH(3))(2)]ClO(4).H(2)O (monoclinic, P2(1)/c (no. 14), a=12.095(2), b=14.046(2), c=14.448(2) angstroms, beta=95.55(2) degrees, Z=4)-were characterized by X-ray crystallography.  相似文献   

19.
This work describes the synthesis of cis-[Pt(C[triple bond]CPh)2(Hdmpz)2] (1) and its use as a precursor for the preparation of homo- and heteropolynuclear complexes. Double deprotonation of compound 1 with readily available M(I) (M = Cu, Ag, Au) or M(II) (M = Pd, Pt) species affords the discrete hexanuclear clusters [{PtM2(mu-C[triple bond]CPh)2(mu-dmpz)(2)}(2)] [M = Cu (2), Ag (3), Au (4)], in which both "Pt(C[triple bond]CPh)2(dmpz)(2)" fragments are connected by four d(10) metal centers, and are stabilized by alkynyl and dimethylpyrazolate bridging ligands, or the trinuclear complexes [Pt(mu-C[triple bond]CPh)2(mu-dmpz)(2){M(C/\P)}2] (M = Pd (5), Pt (6); C/\P = CH(2)-C(6)H(4)-P(o-tolyl)2-kappaC,P), respectively. The X-ray structures of complexes 1-4 and 6 are reported. The X-ray structure of the platinum-copper derivative 2 shows that all copper centers exhibit similar local geometry being linearly coordinated to a nitrogen atom and eta(2) to one alkynyl fragment. However in the related platinum-silver (3) and platinum-gold (4) derivatives the silver and gold atoms present three different coordination environments. The complexes have been studied by absorption and emission spectroscopy. The hexanuclear complexes exhibit bright luminescence in the solid state and in fluid solution (except 4 in the solid state at 298 K). Dual long-lived emission is observed, being clearly resolved in low-temperature rigid media. The low-energy emission is ascribed to MLM'CT Pt(d)/pi(C[triple bond]CPh)-->Pt(p(z))/M'(sp)/pi*(C[triple bond]CPh) modified by metal-metal interactions whereas the high-energy emission is tentatively attributed to an emissive state derived from dimethylpyrazolate-to-metal (d(10)) LM'CT transitions pi(dmpz)-->M'(d(10)).  相似文献   

20.
Au colloids were prepared by irradiation with a Nd:YAG laser. Au nanoparticles were characterized by absorption spectra, transmission electron microscopy (TEM) and X-ray diffraction (XRD) analysis. It is found that the wavelength of the laser has no effect on the size but the number of the Au nanoparticles. By irradiating a transparent silica gel doped with gold ions with the focused laser in the gel and subsequent exposing in air, a space-selective pattern of letter “P” consisting of Au nanoparticles was observed inside the silica gel.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号