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利用基质组装团簇源将团簇束沉积放大至克级用于多相催化(水溶液中硝基苯酚的催化臭氧化)

Scale-Up of Cluster Beam Deposition to the Gram Scale with the Matrix Assembly Cluster Source for Heterogeneous Catalysis (Catalytic Ozonation of Nitrophenol in Aqueous Solution).

作者信息

Cai Rongsheng, Martelli Francesca, Vernieres Jerome, Albonetti Stefania, Dimitratos Nikolaos, Tizaoui Chedly, Palmer Richard E

机构信息

College of Engineering, Swansea University, Bay Campus, Fabian Way, SwanseaSA1 8EN, U.K.

Department of Industrial Chemistry "Toso Montanari", Alma Mater Studiorum-University of Bologna, Viale Risorgimento, 4, 40136 Bologna, Italy.

出版信息

ACS Appl Mater Interfaces. 2020 Jun 3;12(22):24877-24882. doi: 10.1021/acsami.0c05955. Epub 2020 May 22.

DOI:10.1021/acsami.0c05955
PMID:32391685
Abstract

The deposition of precisely controlled clusters from the beam onto suitable supports represents a novel method to prepare advanced cluster-based catalysts. In principle, cluster size, composition, and morphology can be tuned or selected prior to deposition. The newly invented matrix assembly cluster source (MACS) offers one solution to the long-standing problem of low cluster deposition rate. Demonstrations of the cluster activities under realistic reaction conditions are now needed. We deposited elemental silver (Ag) and gold (Au) clusters onto gram-scale powders of commercial titanium dioxide (TiO) to investigate the catalytic oxidation of nitrophenol (a representative pollutant in water) by ozone in aqueous solution, as relevant to the removal of waste drugs from the water supply. A range of techniques, including scanning transmission electron microscopy (STEM), Brunauer-Emmett-Teller (BET) surface area test, and X-ray photoelectron spectroscopy (XPS), were employed to reveal the catalyst size, morphology, surface area, and oxidation state. Both the Ag and Au cluster catalysts proved active for the nitrophenol ozonation. The cluster catalysts showed activities at least comparable to those of catalysts made by traditional chemical methods in the literature, demonstrating the potential applications of the cluster beam deposition method for practical heterogeneous catalysis in solution.

摘要

将精确控制的团簇从束流沉积到合适的载体上是制备先进的基于团簇的催化剂的一种新方法。原则上,团簇尺寸、组成和形态可以在沉积之前进行调整或选择。新发明的基质组装团簇源(MACS)为长期存在的团簇沉积速率低的问题提供了一种解决方案。现在需要在实际反应条件下证明团簇的活性。我们将元素银(Ag)和金(Au)团簇沉积到商用二氧化钛(TiO₂)的克级粉末上,以研究水溶液中臭氧对硝基苯酚(水中一种代表性污染物)的催化氧化,这与从供水系统中去除废弃药物相关。采用了一系列技术,包括扫描透射电子显微镜(STEM)、布鲁诺尔-埃米特-泰勒(BET)表面积测试和X射线光电子能谱(XPS),以揭示催化剂的尺寸、形态、表面积和氧化态。Ag和Au团簇催化剂都被证明对硝基苯酚臭氧化反应具有活性。团簇催化剂的活性至少与文献中传统化学方法制备的催化剂相当,这证明了团簇束沉积法在溶液中实际多相催化中的潜在应用。

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