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利用设计良好的钯纳米结构实现太阳能到催化氢化的高效耦合。

Efficient coupling of solar energy to catalytic hydrogenation by using well-designed palladium nanostructures.

机构信息

Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, School of Chemistry and Materials Science and CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/

出版信息

Angew Chem Int Ed Engl. 2015 Feb 16;54(8):2425-30. doi: 10.1002/anie.201407785. Epub 2014 Oct 19.

Abstract

A Ru(3+)-mediated synthesis for the unique Pd concave nanostructures, which can directly harvest UV-to-visible light for styrene hydrogenation, is described. The catalytic efficiency under 100 mW cm(-2) full-spectrum irradiation at room temperature turns out to be comparable to that of thermally (70 °C) driven reactions. The yields obtained with other Pd nanocrystals, such as nanocubes and octahedrons, are lower. The nanostructures reported here have sufficient plasmonic cross-sections for light harvesting in a broad spectral range owing to the reduced shape symmetry, which increases the solution temperature for the reaction by the photothermal effect. They possess a large quantity of atoms at corners and edges where local heat is more efficiently generated, thus providing active sites for the reaction. Taken together, these factors drastically enhance the hydrogenation reaction by light illumination.

摘要

一种 Ru(3+)介导的独特 Pd 凹面纳米结构的合成方法被描述,这种方法可以直接收集从紫外线到可见光的光,用于苯乙烯氢化。在室温下,在 100mW/cm(2)全光谱辐照下的催化效率可与热(70°C)驱动反应相媲美。用其他 Pd 纳米晶体,如纳米立方体和八面体,得到的产率较低。由于形状对称性降低,这里报道的纳米结构在较宽的光谱范围内具有足够的等离子体横截面用于光捕获,这通过光热效应增加了反应的溶液温度。它们在角和边缘处具有大量的原子,局部热量更有效地产生,从而为反应提供了活性位点。总的来说,这些因素通过光照极大地增强了氢化反应。

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