用于无溶剂氢化的聚合物支撑钯纳米粒子

IF 14.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2024-09-13 DOI:10.1021/jacs.4c09241

Qingsong Luo, Hai Wang, Qian Xiang, Yating Lv, Jiabao Yang, Lijuan Song, Xiaoming Cao, Liang Wang, Feng-Shou Xiao

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引用次数: 0

摘要

打破支撑金属催化剂活性与稳定性之间的权衡一直是催化领域长期面临的挑战，尤其是对于氢化活性高但稳定性差的金属纳米颗粒（NPs）而言。在此，我们报告了一种多孔聚（二乙烯基苯）聚合物支撑的 Pd NP 催化剂（Pd/PDVB），该催化剂在硝基苯的无溶剂加氢反应中具有高活性和出色的稳定性，即使在环境温度（25 °C）和 H2 压力（0.1 兆帕）下也是如此。在 70 °C 和 0.4 MPa 条件下，Pd/PDVB 的翻转频率高达 22,632 h-1，超过了同等条件下传统 Pd/C 催化剂的 5556 h-1。机理研究表明，聚合物载体有利于苯胺产物从钯表面解吸，这对于在无溶剂条件下快速加氢至关重要。此外，Pd/PDVB 中的聚合物支撑还能有效阻止钯的浸出，从而获得良好的稳定性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Polymer-Supported Pd Nanoparticles for Solvent-Free Hydrogenation

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Polymer-Supported Pd Nanoparticles for Solvent-Free Hydrogenation

Breaking the trade-off between activity and stability of supported metal catalysts has been a long-standing challenge in catalysis, especially for metal nanoparticles (NPs) with high hydrogenation activity but poor stability. Herein, we report a porous poly(divinylbenzene) polymer-supported Pd NP catalyst (Pd/PDVB) with both high activity and excellent stability for the solvent-free hydrogenation of nitrobenzene, even at ambient temperature (25 °C) and H₂ pressure (0.1 MPa). Pd/PDVB gave a turnover frequency as high as 22,632 h^–1 at 70 °C and 0.4 MPa, exceeding 5556 h^–1 of the classical Pd/C catalyst under equivalent conditions. Mechanistic studies reveal that the polymer support benefits the desorption of the aniline product from the Pd surface, which is crucial for rapid hydrogenation under solvent-free conditions. In addition, the polymer support in Pd/PDVB efficiently hindered Pd leaching, resulting in good stability.

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来源期刊

Journal of the American Chemical Society 化学-化学综合

CiteScore

24.40

自引率

6.00%

发文量

2398

审稿时长

1.6 months

期刊介绍： The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.