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Electrocatalytic activity of ligand-protected gold particles: formaldehyde oxidation 配体保护金颗粒的电催化活性:甲醛氧化
IF 2.2 4区 工程技术 Q2 Chemistry Pub Date : 2013-10-07 DOI: 10.1007/s13404-013-0110-0
Kun Luo, Haiming Wang, Xiaogang Li

Tris(hydroxymethyl)phosphine oxide (THPO) and triphenyl phosphine oxide (PPh3O) were introduced onto the surface of colloidal gold nanoparticles (Au NPs), and the effect of capping ligands on the catalytic electrooxidation of formaldehyde was studied voltammetrically by using colloidal Au-NP-modified glassy carbon electrodes (GCEs). This was compared with polycrystalline Au and another Au-NP-modified GCE without a capping molecule. We found that PPh3O causes a larger decrease in the catalytic activity of the Au NPs in liquid than THPO does, indicating that the catalytic activity of the Au NPs is closely associated with the capping ligands. The effect of capping ligands is discussed based on the available surface ratio (ASR), which is defined as the ratio of the total surface area measured electrochemically to the calculated value based on the number and geometry of the Au NPs. These were determined to be 70.6?% for THPO and 0.23?% for PPh3O, respectively. The significant blocking of formaldehyde is probably due to the structure and hydrophobicity of the benzene rings in the PPh3O molecule, which is responsible for the decrease in catalytic activity of the Au NPs.

将三(羟甲基)氧化膦(THPO)和三苯基氧化膦(pph30)分别引入胶体金纳米粒子(Au NPs)表面,采用胶体金纳米粒子修饰的玻碳电极(gce)伏安法研究了盖层配体对甲醛催化电氧化的影响。这与多晶Au和另一种没有盖层分子的Au- np修饰的GCE进行了比较。我们发现,与THPO相比,pph30对液体中Au NPs的催化活性降低幅度更大,这表明Au NPs的催化活性与盖层配体密切相关。基于有效表面比(ASR)讨论了盖层配体的影响,有效表面比定义为电化学测量的总表面积与基于Au NPs数量和几何形状的计算值的比值。这些被确定为70.6?% THPO和0.23?%分别为pph30。甲醛的显著阻断可能是由于pph30分子中苯环的结构和疏水性,这是Au NPs催化活性降低的原因。
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引用次数: 6
Electron transfer processes on Au nanoclusters supported on graphite 石墨负载金纳米团簇的电子转移过程
IF 2.2 4区 工程技术 Q2 Chemistry Pub Date : 2013-10-05 DOI: 10.1007/s13404-013-0109-6
Jie Shen, Juanjuan Jia, Kirill Bobrov, Laurent Guillemot, Vladimir A. Esaulov

Electron transfer processes play an important role in surface chemistry. This paper presents results of a study of changes in resonant electron transfer processes, as a function of gold cluster sizes, on the example of electron transfer between Li+ ions scattered on Au clusters on highly oriented pyrolytic graphite (HOPG). The gold nanoclusters were grown on lightly sputtered HOPG surface in order to obtain a wide coverage distribution of clusters. The growth of clusters was monitored by scanning tunneling microscopy. We found that electron transfer is much more probable on small clusters, whose lateral size is of the order of 2 to 3?nm and height in the 1-nm range, than on bulk Au or thin Au films. A comparison with Au clusters grown on the semiconducting titania did not reveal significant differences with HOPG.

电子转移过程在表面化学中起着重要的作用。本文以高取向热解石墨(HOPG)上分散在Au团簇上的Li+离子之间的电子转移为例,研究了共振电子转移过程随金团簇大小的变化。在轻溅射的HOPG表面生长金纳米团簇,以获得团簇覆盖范围广的分布。用扫描隧道显微镜观察簇的生长情况。我们发现电子转移更可能发生在横向尺寸为2到3?厚度在1nm范围内,比在大块或薄Au薄膜上。与生长在半导体二氧化钛上的金簇的比较没有发现与HOPG的显著差异。
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引用次数: 10
Gold, and lots of it 金子,很多金子
IF 2.2 4区 工程技术 Q2 Chemistry Pub Date : 2013-09-12 DOI: 10.1007/s13404-013-0104-y
Trevor Keel
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引用次数: 0
Highlights from recent literature 近期文献亮点
IF 2.2 4区 工程技术 Q2 Chemistry Pub Date : 2013-08-29 DOI: 10.1007/s13404-013-0105-x
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引用次数: 0
On the selection and design of proteins and peptide derivatives for the production of photoluminescent, red-emitting gold quantum clusters 制备光致发光、发红金量子团簇所需蛋白质和肽衍生物的选择和设计
IF 2.2 4区 工程技术 Q2 Chemistry Pub Date : 2013-08-01 DOI: 10.1007/s13404-013-0100-2
Balázs Söptei, Lívia Naszályi Nagy, Péter Baranyai, Ildikó Szabó, Gábor Mező, Ferenc Hudecz, Attila Bóta

Novel pathways of the synthesis of photoluminescent gold quantum clusters (AuQCs) using biomolecules as reactants provide biocompatible products for biological imaging techniques. In order to rationalize the rules for the preparation of red-emitting AuQCs in aqueous phase using proteins or peptides, the role of different organic structural units was investigated. Three systems were studied: proteins, peptides, and amino acid mixtures, respectively. We have found that cysteine and tyrosine are indispensable residues. The SH/S-S ratio in a single molecule is not a critical factor in the synthesis, but on the other hand, the stoichiometry of cysteine residues and the gold precursor is crucial. These observations indicate the importance of proper chemical behavior of all species in a wide size range extending from the atomic distances (in the AuI-S semi ring) to nanometer distances covering the larger sizes of proteins assuring the hierarchical structure of the whole self-assembled system.

利用生物分子作为反应物合成光致发光金量子团簇(auqc)的新途径为生物成像技术提供了生物相容性产品。为了使在水相中使用蛋白质或多肽制备红色auqc的规律更加合理,研究了不同有机结构单元的作用。研究了三种体系:蛋白质、多肽和氨基酸混合物。我们发现半胱氨酸和酪氨酸是不可缺少的残基。单分子的SH/S-S比不是合成的关键因素,但另一方面,半胱氨酸残基和金前体的化学计量是至关重要的。这些观察结果表明,在从原子距离(在AuI-S半环中)到纳米距离(覆盖较大尺寸的蛋白质)的广泛尺寸范围内,所有物种的适当化学行为的重要性,确保了整个自组装系统的层次结构。
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引用次数: 22
Au as an efficient promoter for electrocatalytic oxidation of formic acid and carbon monoxide: a comparison between Pt-on-Au and PtAu alloy catalysts Au作为甲酸和一氧化碳电催化氧化的有效促进剂:Pt-on-Au和PtAu合金催化剂的比较
IF 2.2 4区 工程技术 Q2 Chemistry Pub Date : 2013-07-19 DOI: 10.1007/s13404-013-0098-5
Qiang Zhang, Ruirui Yue, Fengxing Jiang, Huiwen Wang, Chunyang Zhai, Ping Yang, Yukou Du

The absence of unpaired d-electrons of gold leads to its lack of reactivity and paucity of catalytic activity. Synergistic activity of bimetallic PtAu has been proved, and its structure greatly influences on the electrocatalytic activity toward formic acid and carbon monoxide oxidation. Here, a comparison between Pt-modified Au (designated as Pt-on-Au) and PtAu alloy catalysts has been studied. The Pt-on-Au catalyst was prepared by electrodeposition of Pt on the pre-prepared Au, while PtAu alloy was obtained by co-electrodeposition. As a whole, both types of PtAu catalysts were found to be more active toward formic acid electrooxidation compared to pure Pt, exhibiting maximum activity on Pt-on-Au catalyst with Pt to Au atomic ratio of 1:10.22. Moreover, the Pt/Au atomic ratio directly relates to the oxidation pathway of formic acid and carbon monoxide oxidation. The results may be ascribed to much less COads on the surface than single Pt catalyst due to the effect of Au nanoparticles. CO stripping voltammograms present the obvious variation between Pt-on-Au and PtAu alloy catalysts. Meanwhile, the electrocatalytic activities of bimetallic PtAu are evaluated by electrochemical impedance spectroscopy and Tafel analysis.

金中没有不成对的d电子导致其缺乏反应性和催化活性。双金属PtAu的协同作用已被证实,其结构对甲酸和一氧化碳氧化的电催化活性有很大影响。本文对pt改性Au(称为Pt-on-Au)和PtAu合金催化剂进行了比较研究。通过电沉积Pt在预制备的Au上制备Pt-on-Au催化剂,通过共电沉积得到PtAu合金。总的来说,两种类型的PtAu催化剂都比纯Pt具有更强的甲酸电氧化活性,当Pt与Au原子比为1:10.22时,Pt-on-Au催化剂的活性最大。此外,Pt/Au原子比直接关系到甲酸和一氧化碳氧化的氧化途径。这一结果可能是由于Au纳米粒子的作用,表面负载比单一Pt催化剂少得多。CO溶出伏安图在Pt-on-Au和PtAu合金催化剂之间表现出明显的差异。同时,通过电化学阻抗谱和Tafel分析对双金属PtAu的电催化活性进行了评价。
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引用次数: 28
Green biosynthesis of gold nanometre scale plates using the leaf extracts from an indigenous Australian plant Eucalyptus macrocarpa 利用澳大利亚本土植物巨桉叶提取物的绿色生物合成金纳米尺度板
IF 2.2 4区 工程技术 Q2 Chemistry Pub Date : 2013-07-02 DOI: 10.1007/s13404-013-0096-7
Gérrard Eddy Jai Poinern, Peter Chapman, Xuan Le, Derek Fawcett

In this preliminary study, we demonstrate an environmentally friendly process for the green synthesis of gold nanometre scale particles using the leaf extract from an indigenous Australian plant Eucalyptus macrocarpa as both the stabilising agent and the reducing agent. The synthesis process is straightforward, clean and non-toxic. It also has the advantages of being performed at room temperature and does not need complex processing equipment. Formation of the gold nanometre sized particles was confirmed and characterised by UV-visible spectroscopy, X-ray diffraction, transmission electron microscopy and field emission scanning electron microscopy. The antibacterial activity of the synthesised gold particles was also quantified using the sensitivity method of Kirby–Bauer.

在这项初步研究中,我们展示了一种绿色合成纳米级金颗粒的环保工艺,该工艺使用澳大利亚本土植物巨桉(Eucalyptus macrocarpa)的叶子提取物作为稳定剂和还原剂。合成过程简单、清洁、无毒。它还具有在室温下进行,不需要复杂的加工设备的优点。通过紫外可见光谱、x射线衍射、透射电子显微镜和场发射扫描电子显微镜对纳米级金颗粒的形成进行了证实和表征。利用Kirby-Bauer灵敏度法对合成金颗粒的抗菌活性进行了定量测定。
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引用次数: 42
Highlights from recent literature 近期文献亮点
IF 2.2 4区 工程技术 Q2 Chemistry Pub Date : 2013-06-18 DOI: 10.1007/s13404-013-0095-8
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引用次数: 3
Gold and diagnostics—some staggering numbers 黄金和诊断学——一些惊人的数字
IF 2.2 4区 工程技术 Q2 Chemistry Pub Date : 2013-06-14 DOI: 10.1007/s13404-013-0097-6
Trevor Keel
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引用次数: 1
Simultaneous determination of uric acid and dopamine using a carbon fiber electrode modified by layer-by-layer assembly of graphene and gold nanoparticles 使用石墨烯和金纳米颗粒逐层组装修饰的碳纤维电极同时测定尿酸和多巴胺
IF 2.2 4区 工程技术 Q2 Chemistry Pub Date : 2013-05-19 DOI: 10.1007/s13404-013-0090-0
Jiao Du, Ruirui Yue, Fangfang Ren, Zhangquan Yao, Fengxing Jiang, Ping Yang, Yukou Du

A novel layer-by-layer assembly of graphene sheets and gold nanoparticles modified carbon fiber electrode (GE/Au/GE/CFE) was successfully fabricated and applied to simultaneous determination of dopamine (DA) and uric acid (UA). The structure of GE/Au/GE/CFE was characterized by scanning electron microscopy (SEM). It was observed that the gold nanoparticles were homogeneously assembled between the two layers of GE sheets. Cyclic voltammetry (CV) measurements elucidate that GE/Au/GE/CFE has higher electrocatalytic activity for the oxidation of DA and UA when compared with graphene modified carbon fiber electrode (GE/CFE), and graphene and gold nanoparticles modified carbon fiber electrode (Au/GE/CFE). Simultaneous determination of UA and DA on GE/Au/GE/CFE was conducted with a differential pulse voltammetry technique, and two well-defined and fully resolved anodic oxidation peaks were observed. Anodic oxidation currents of DA and UA are linear with their concentration in the range of 0.59–43.96?μM and 12.6–413.62?μM, respectively. Moreover, the composite electrode displays high reproducibility and selectivity for the determination of UA and DA.

成功制备了一种新型的石墨烯片与金纳米颗粒修饰的碳纤维电极(GE/Au/GE/CFE),并将其应用于同时测定多巴胺(DA)和尿酸(UA)。用扫描电镜(SEM)对GE/Au/GE/CFE的结构进行了表征。结果表明,金纳米粒子在两层GE片之间均匀组装。循环伏安法(CV)测试表明,与石墨烯修饰碳纤维电极(GE/CFE)和石墨烯与金纳米粒子修饰碳纤维电极(Au/GE/CFE)相比,GE/Au/GE/CFE对DA和UA的氧化具有更高的电催化活性。采用差分脉冲伏安法同时测定了GE/Au/GE/CFE上的UA和DA,观察到两个清晰且完全分解的阳极氧化峰。DA和UA的阳极氧化电流在0.59 ~ 43.96?m和12.6-413.62 ?μM,分别。此外,复合电极对UA和DA的测定具有较高的重复性和选择性。
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引用次数: 67
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Gold Bulletin
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