Polymer-Supported Pd Nanoparticles for Solvent-Free Hydrogenation,Journal of the American Chemical Society

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Polymer-Supported Pd Nanoparticles for Solvent-Free Hydrogenation
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-09-13 , DOI: 10.1021/jacs.4c09241
Qingsong Luo ₁ , Hai Wang ₁ , Qian Xiang ₂ , Yating Lv ₁ , Jiabao Yang ₃ , Lijuan Song ₃ , Xiaoming Cao _{2,

4} , Liang Wang ₁ , Feng-Shou Xiao ₁

Affiliation

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.

中文翻译：

用于无溶剂加氢的聚合物负载的钯纳米粒子

打破负载型金属催化剂的活性和稳定性之间的平衡一直是催化领域长期面临的挑战，特别是对于加氢活性高但稳定性差的金属纳米粒子（NP）。在此，我们报道了一种多孔聚（二乙烯基苯）聚合物负载的 Pd NP 催化剂（Pd/PDVB），即使在环境温度（25 °C）和 H ₂压力下，对于硝基苯的无溶剂加氢也具有高活性和优异的稳定性（0.1 兆帕）。 Pd/PDVB 在 70 °C 和 0.4 MPa 下的周转频率高达 22,632 h ^–1 ，超过同等条件下经典 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Pd表面解吸，这对于无溶剂条件下的快速氢化至关重要。此外，Pd/PDVB中的聚合物载体有效地阻碍了Pd的浸出，从而具有良好的稳定性。

更新日期：2024-09-13

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