在未煅烧的TS-1上浸渍光稳定金前驱体以促进丙烷的催化加氢氧化

IF 10.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Zhihua Zhang, Erchuan Yang, Fan Liu, Kesheng Xu, Yuxia Zhong, Jinwei Sun, Shudong Shi, Xuezhi Duan, Xinggui Zhou
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引用次数: 0

摘要

用简单的浸渍法在硅酸钛-1 (TS-1)上固定高度分散的金纳米粒子仍然是一项具有挑战性的任务。本文首次合成了具有巯基配体保护的高光稳定性金前驱体,制备的金前驱体在光照下具有30天以上的优异稳定性,而没有巯基配体的金前驱体在光照下仅2小时就形成了沉淀。随后,采用初湿浸渍法(IWI法)将硫醇配体保护的Au前驱体固定在未煅烧的TS-1(即TS-1- b)表面,制备Au/TS-1- b催化剂。制备的Au/TS-1-B催化剂在丙烷加氢氧化制丙酮中的活性比沉积-沉淀尿素法(DPU法)制备的催化剂高1.4倍。采用多种表征方法对Au/TS-1-B催化剂的结构进行了分析。与DPU法制备的Au/TS-1-B催化剂相比,IWI法制备的Au/TS-1-B催化剂具有更窄的Au纳米颗粒尺寸分布和更多的小Au颗粒(<2 nm),这是其活性优越的主要原因。此外,还考察了含金量、反应温度和Si/Ti摩尔比对IWI法制备的Au/TS-1-B催化剂催化性能的影响。此外,IWI法制备的Au/TS-1-B催化剂在140 h以上也表现出优异的稳定性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Impregnating photo-stable gold precursor onto uncalcined TS-1 to boost catalytic hydro-oxidation of propane

Immobilizing highly dispersed Au nanoparticles onto titanium silicalite-1 (TS-1) by a simple impregnation method under light is still a challenging task. In this work, a high photostable Au precursor protected by thiol ligands was firstly synthesized, and the as-prepared Au precursor displayed excellent stability under light for over 30 days, while the Au precursor without thiol ligands formed precipitates after just 2 h under light. Subsequently, the Au precursor protected by thiol ligands was immobilized on the external surface of uncalcined TS-1 (i.e., TS-1-B) by the incipient wetness impregnation method (IWI method) to prepare Au/TS-1-B catalyst. The activity of as-prepared Au/TS-1-B catalyst in the hydro-oxidation of propane to acetone was 1.4 times higher than that of the catalyst prepared by the deposition-precipitation urea method (DPU method). The structures of the Au/TS-1-B catalysts prepared by different methods were analyzed by multiple characterizations. Compared to the Au/TS-1-B catalyst prepared by the DPU method, the Au/TS-1-B catalyst synthesized by the IWI method exhibited a narrower size distribution of Au nanoparticles and had more small Au particles (<2 nm), which is the main reason for its superior activity. Additionally, the effects of gold loadings, reaction temperature and Si/Ti molar ratio on the catalytic performance of the Au/TS-1-B catalyst prepared by the IWI method were also investigated. In addition, the Au/TS-1-B catalyst prepared by the IWI method also exhibited excellent stability for over 140 h.

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来源期刊
Science China Chemistry
Science China Chemistry CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
14.40
自引率
7.30%
发文量
3787
审稿时长
2.2 months
期刊介绍: Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field. Categories of articles include: Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry. Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies. Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.
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