Construction of WOx@HTS-1 Nanoparticles for Efficient Catalysis of 1-Hexene Epoxidation

IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Xinpeng Li, , , Lingling Zou, , , Mei-hua Zhu*, , , Wenjun Yuan, , , Hongjie Peng, , , Qingshen Wu, , , Ziming Li, , , Rui Liu, , , Xiang-Shu Chen, , and , Hidetoshi Kita, 
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引用次数: 0

Abstract

1-Hexene epoxidation is difficult to achieve for the low electron cloud density of long-chain terminal olefin double bonds structure; the development of efficient and stable catalysts is the key to achieving the highly efficient epoxidation of 1-hexene. The titanosilicate/H2O2 system has been the most promising and environmentally friendly epoxidation route in recent research, and the WOx@HTS-1 nanoparticles were successfully prepared by an etching–impregnation–recrystallization strategy in this work. Unique structures of the WOx@HTS-1 nanoparticles could achieve the effects of “killing three birds with one stone” for 1-hexene epoxidation. I. Hierarchical structure and “hollow nests” could significantly enhance the accessibility of the active sites, shorten the transmission path, and improve the diffusion efficiency of the reactants and products. II. Titanium active centers and metal oxide active sites had significant and efficient synergistic catalytic effects on 1-hexene epoxidation. III. Fine WOx particles were highly dispersed on the hollow nests of WOx@HTS-1 nanoparticles, which prevented the sintering and poisoning of WOx clusters during the reaction process and ensured excellent stability of the catalysts by the restricted-domain effect. Attractively, 1-hexene conversion and 1,2-epoxyhexane selectivity were more than 90 and 96% with WOx@HTS-1 nanoparticles and H2O2, respectively, which provided many opportunities for the directional design of nanoparticles and their application in emerging catalytic fields.

Abstract Image

WOx@HTS-1纳米颗粒高效催化1-己烯环氧化反应的构建。
由于长链末端烯烃双键结构的电子云密度低,1-己烯难以实现环氧化;开发高效稳定的催化剂是实现1-己烯高效环氧化反应的关键。二氧化钛/H2O2体系是近年来研究中最有前途的环保环氧化途径,本研究成功地采用蚀刻-浸渍-再结晶策略制备了WOx@HTS-1纳米颗粒。WOx@HTS-1纳米颗粒的独特结构可以实现1-己烯环氧化“一石三鸟”的效果。1 .分层结构和“空心巢”能显著提高活性位点的可达性,缩短传递路径,提高反应物和产物的扩散效率。2。钛活性中心和金属氧化物活性位点对1-己烯环氧化反应具有显著而高效的协同催化作用。3。细小的WOx粒子高度分散在WOx@HTS-1纳米粒子的空心巢上,防止了反应过程中WOx团簇的烧结和中毒,并通过限制域效应保证了催化剂的优异稳定性。令人感兴趣的是,WOx@HTS-1纳米粒子和H2O2的1-己烯转化率和1,2-环氧己烷选择性分别超过90%和96%,这为纳米粒子的定向设计及其在新兴催化领域的应用提供了许多机会。
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来源期刊
Langmuir
Langmuir 化学-材料科学:综合
CiteScore
6.50
自引率
10.30%
发文量
1464
审稿时长
2.1 months
期刊介绍: Langmuir is an interdisciplinary journal publishing articles in the following subject categories: Colloids: surfactants and self-assembly, dispersions, emulsions, foams Interfaces: adsorption, reactions, films, forces Biological Interfaces: biocolloids, biomolecular and biomimetic materials Materials: nano- and mesostructured materials, polymers, gels, liquid crystals Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do? Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*. This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).
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