Palladium Nanoparticles Anchored on COFs Prepared by Simple Calcination for Phenol Hydrogenation,Industrial & Engineering Chemistry Research

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Palladium Nanoparticles Anchored on COFs Prepared by Simple Calcination for Phenol Hydrogenation
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2021-09-09 , DOI: 10.1021/acs.iecr.1c02366
Hong Jiang ₁ , Xinhui Shen ₁ , Fengnan Wang ₁ , Jiuxuan Zhang ₁ , Yan Du ₂ , Rizhi Chen ₁

Affiliation

Covalent organic frameworks (COFs) used as supports for metal nanoparticles (MNPs) show high efficiency in heterogeneous catalysis. Developing a green and efficient way to synthesize COFs remains a great challenge. Herein, an imine COF (TpPa-1) was prepared via a green and convenient calcination method under low temperature, and then Pd nanoparticles (NPs) were loaded to prepare Pd@COFs catalysts for the selective phenol hydrogenation to cyclohexanone. XRD and FTIR results confirm the successful synthesis of TpPa-1 by a simple calcination method. A suitable calcination temperature (280 °C) is conducive to the synthesis of TpPa-1 (COF-280) with higher crystallinity, larger BET surface area, higher mesoporous proportion, and uniform spherical morphology. These characteristics of COF-280 increase the Pd loading, promote the formation of Pd with higher Pd⁰ proportion on the catalyst surface, and enhance the mass transfer, thereby improving the catalytic properties of Pd@COF-280 for the phenol hydrogenation, with a catalytic activity increased by 2 times compared to Pd@COF-220. The addition of p-toluenesulfonamide during the synthesis can affect the crystallinity and morphology of TpPa-1 and the corresponding catalytic performance. Furthermore, Pd@COF-280 shows good reusability during four reaction cycles. The work provides a green approach for preparing imine-COFs and their efficient applications in heterogeneous catalysis.

中文翻译：

通过简单煅烧制备苯酚氢化反应制备的 COFs 上的钯纳米颗粒

用作金属纳米粒子 (MNP) 载体的共价有机骨架 (COF) 在多相催化中表现出高效率。开发一种绿色高效的合成 COF 的方法仍然是一个巨大的挑战。在此，通过绿色便捷的低温煅烧方法制备了亚胺 COF (TpPa-1)，然后负载 Pd 纳米粒子 (NPs) 制备 Pd@COFs 催化剂，用于选择性苯酚加氢生成环己酮。XRD 和 FTIR 结果证实了通过简单的煅烧方法成功合成了 TpPa-1。合适的煅烧温度（280℃）有利于合成结晶度更高、BET表面积更大、介孔比例更高、球形形态均匀的TpPa-1（COF-280）。COF-280 的这些特性增加了 Pd 负载，⁰比例在催化剂表面，增强传质，从而提高 Pd@COF-280 对苯酚加氢的催化性能，催化活性比 Pd@COF-220 提高 2 倍。合成过程中对甲苯磺酰胺的加入会影响TpPa-1的结晶度和形貌以及相应的催化性能。此外，Pd@COF-280 在四个反应循环中显示出良好的可重复使用性。该工作为制备亚胺-COFs 及其在多相催化中的有效应用提供了一种绿色方法。

更新日期：2021-09-22

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