机械驱动选择性有机氧化利用mof涂层的压电SnSe纳米片

IF 17.1 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Hong Liu , Shun Li , Maosong Liu , Pengting Sun , Xinyue Zhang , Long Zhang , Yuqiao Zhang , Gastón Contreras-Jiménez , Jonathan Potier , Zhongti Sun , Xiaohong Yan , Yangyang Wan , Li-Dong Zhao , Jianming Zhang
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引用次数: 0

摘要

通过环境友好的催化方法实现有机转化的高选择性和高活性是绿色化学的关键。在这项研究中,我们报道了一种由非晶UiO-66-NH2金属有机框架(MOF)负载的二维(2D)压电SnSe纳米片组成的混合压电催化剂。该SnSe/MOF纳米复合催化剂具有优异的机械驱动选择性有机氧化效率,在超声振动(90 W, 45 kHz)下,苯甲醇氧化成苯甲醛的反应速率为604.3 μmol g−1 h−1,转化率为~95.3%,选择性超过99%。结合实验结果和理论模拟表明,SnSe与MOF之间形成的界面化学键为机械激发的自由载流子建立了电荷流“高速公路”,而MOF涂层作为助催化剂,降低了H2O2/•OH生成的反应势垒,促进了选择性有机转化反应。此外,MOF层显著提高了2D SnSe压电催化剂在反应溶剂中的亲水性和稳定性。本研究展示了一种简单、绿色、高效的压电介导机械化学方法,用于选择性合成高附加值有机化学品。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Mechanically driven selective organic oxidation using MOF-coated piezoelectric SnSe nanosheets

Mechanically driven selective organic oxidation using MOF-coated piezoelectric SnSe nanosheets
Achieving high selectivity and activity in organic conversions through environmental-friendly catalytic approaches is crucial in green chemistry. In this study, we report a hybrid piezocatalyst composed of two-dimensional (2D) piezoelectric SnSe nanosheets loaded by amorphous UiO-66-NH2 metal-organic frameworks (MOF). This SnSe/MOF nanocomposite catalyst exhibits exceptional efficiency for mechanically-driven selective organic oxidation, achieving a remarkable reaction rate of 604.3 μmol g−1 h−1 for oxidizing benzyl alcohol to benzaldehyde under ultrasonication vibration (90 W, 45 kHz), with a conversion ratio of ∼95.3 % in only 1.5 h and selectivity over 99 %. Combined experimental results and theoretical simulations elucidate that the interfacial chemical bonds formed between SnSe and MOF establish a charge flow “highway” for mechanically excited free carriers, while the MOF coating layer acts as a co-catalyst that lowers the reaction barrier for H2O2/•OH production, facilitating selective organic conversion reactions. Additionally, the MOF layer significantly enhances the hydrophilicity and stability of the 2D SnSe piezocatalysts in reaction solvents. This study demonstrates a simple, green, and efficient piezoelectrically-mediated mechanochemical method for selective synthesis of high-value-added organic chemicals.
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来源期刊
Nano Energy
Nano Energy CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
30.30
自引率
7.40%
发文量
1207
审稿时长
23 days
期刊介绍: Nano Energy is a multidisciplinary, rapid-publication forum of original peer-reviewed contributions on the science and engineering of nanomaterials and nanodevices used in all forms of energy harvesting, conversion, storage, utilization and policy. Through its mixture of articles, reviews, communications, research news, and information on key developments, Nano Energy provides a comprehensive coverage of this exciting and dynamic field which joins nanoscience and nanotechnology with energy science. The journal is relevant to all those who are interested in nanomaterials solutions to the energy problem. Nano Energy publishes original experimental and theoretical research on all aspects of energy-related research which utilizes nanomaterials and nanotechnology. Manuscripts of four types are considered: review articles which inform readers of the latest research and advances in energy science; rapid communications which feature exciting research breakthroughs in the field; full-length articles which report comprehensive research developments; and news and opinions which comment on topical issues or express views on the developments in related fields.
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