Synthesis of Atomically Ordered AuCu and AuCu3 Nanocrystals from Bimetallic Nanoparticle Precursors
摘要:
A new multistep approach was developed to synthesize atomically ordered intermetallic nanocrystals, using AuCu and AuCu3 as model systems. Bimetallic nanoparticle aggregates are used as precursors to atomically ordered nanocrystals, both to precisely define the stoichiometry of the final product and to ensure that atomic-scale diffusion distances lower the reaction temperatures to prevent sintering. In a typical synthesis, PVP-stabilized Au-Cu nanoparticle aggregates synthesized by borohydride reduction are collected by centrifugation and annealed in powder form. At temperatures below 175 degreesC, diffusion of Cu into Au occurs, and the atomically disordered solid solution CuxAu1-x exists. For AuCu, nucleation occurs by 200 degreesC, and atomically ordered AuCu exists between 200 and 400 degreesC. For AuCu3, an AuCu intermediate nucleates at 200 degreesC, and further diffusion of Cu into the AuCu intermediate at 300 degreesC nucleates AuCu3. Atomically ordered AuCu and AuCu3 nanocrystals can be redispersed as discrete colloids in solution after annealing between 200 and 300 degreesC.
一氧化碳(CO)的电催化还原是一个具有新催化剂结构的新兴方向,其中双金属组分催化剂具有功能多样性和高活性位点密度的特点。在这项工作中,我们证明了对相邻双金属位点的微调可以让我们在 CO 电还原过程中选择不同的反应途径生成 C 1或 C 2产物。制造并研究了具有不同原子比的 Cu 和 Cu-Au 合金催化剂适当的分子距离。发现纯铜催化剂对于将 CO 电还原为 C 2 H 4具有活性,因为相邻的 Cu 位点有利于吸附多个 CO 分子和随后的 C-C 耦合。另一方面,Cu与Au的合金引入了空间位阻和相邻吸附的*CO中间体之间更大的分子间距离,从而导致C 2 H 4选择性降低但CH 4途径增强。我们的工作揭示了 CO 电还原活性位点间距的重要性,这有利于催化剂设计,进一步提高电催化 CO 还原的活性和选择性。
Electrochemical Behavior of Evaporated Copper/Gold Alloys
作者:Robert Reining、Konrad G. Weil
DOI:10.1149/1.2069024
日期:1992.10.1
oxidation of copper from Cu 3 Au allows was studied recently by Parks et al. They found that that the critical oxidation potential for ordered alloys was about 250 mV more noble than for disordered ones. In contrast, Moffat et al. reported on experiments in which no such difference could be detected. Assuming that this discrepancy may be due to the preparation techniques, we investigated alloys prepared
Parks 等人最近研究了从 Cu 3 Au 中优先氧化铜。他们发现有序合金的临界氧化电位比无序合金高约 250 mV。相比之下,莫法特等人。报告了没有检测到这种差异的实验。假设这种差异可能是由于制备技术造成的,我们研究了通过蒸发制备的合金
Pressure dependence of the thermal and electrical conductivities of the intermetallic compounds AuCu and AuCu3
作者:P. Jacobsson、B. Sundqvist
DOI:10.1016/0022-3697(88)90105-9
日期:1988.1
The thermal diffusivity, a, electrical resistivity, ρ, and Seebeck coefficient, S, of ordered and disordered AuCu3 and AuCu have been measured as functions of T and P in the range 100–300 K and 0–2 ...
有序和无序 AuCu3 和 AuCu 的热扩散系数 a、电阻率 ρ 和塞贝克系数 S 已在 100-300 K 和 0-2 ...
Electrochemical and Scanning Tunneling Microscopic Study of Dealloying of Cu3Au
作者:Thomas P. Moffat、Fu‐Ren F. Fan、Allen J. Bard
DOI:10.1149/1.2085396
日期:1991.11.1
Dealloying of Cu~Au has been examined by in situ STM and several electrochemical methods. Three different regimes of behavior were noted. At low overpotentials, clustering of gold atoms occurs near sites of copper dissolution. This is es- sentially a two-dimensional process. The formation and smoothing of these clusters by capillary action, monitored in real time, demonstrated the highly mobile nature
A Seed-Based Diffusion Route to Monodisperse Intermetallic CuAu Nanocrystals
作者:Wei Chen、Rong Yu、Lingling Li、Annan Wang、Qing Peng、Yadong Li
DOI:10.1002/anie.200906835
日期:2010.4.6
A seedy route: MonodisperseCuAu and Cu3Au nanocrystals (NCs) were fabricated by a seed‐based diffusionroute using Au NCs as precursors. This method has advantages in controlling the size and monodispersity of the products. Moving a solid‐state reaction into solution may help to achieve homogeneous diffusion and require less time and thermal energy.
Gold-copper alloy catalysts were prepared by impregnation of TiO2 (anatase) support with mixed chloride precursors and tested in the gas-phase epoxidation of propene. The bimetallic systems contained different Au-Cu molar ratios and a total metal content of 4 wt.%. The corresponding monometallic AU/TiO2 and Cu/TiO2 catalysts were also prepared for comparison. X-ray diffraction, XPS and transmission electron microscopy studies indicated that alloying was achieved. The copper content in the catalyst seemed to have a strong influence on the dispersion and catalytic properties of the metal particles. In particular, the greater the Cu content in the alloy, the smaller the metal particle. These changes also contributed to an increase in activity and selectivity to propene oxide. The sample with a Cu/Au ratio of 3/1 showed the best catalytic behaviour. Moreover, the catalytic activity of the samples can be correlated with the results obtained by TPR. (C) 2007 Elsevier B.V. All rights reserved.