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N-functionalized mesoporous carbon supported Pd nanoparticles as highly active nanocatalyst for Suzuki-Miyaura reaction, reduction of 4-nitrophenol and hydrodechlorination of chlorobenzene
Journal of Industrial and Engineering Chemistry ( IF 6.1 ) Pub Date : 2021-09-14 , DOI: 10.1016/j.jiec.2021.09.005
Juti Rani Deka , Diganta Saikia , Po-Hung Chen , Ke-Ting Chen , Hsien-Ming Kao , Yung-Chin Yang

A series of nanocatalysts derived from immobilization of palladium nanoparticles (Pd NPs) into three dimensional (3D) tube-type architecture of nitrogen (N) functionalized and without functionalized mesoporous carbon CMK-9 is developed by dual agents chemical reduction approach. Herein, for the first time N-functionalized CMK-9 is explored as supports to immobilize Pd NPs and use as multifunctional catalysts for Suzuki-Miyaura cross-coupling reaction, reduction of 4-nitrophenol and hydrodechlorination of chlorobenzene. The Pd@N-CMK-9 catalysts show excellent activities with 100% conversion for Suzuki-Miyaura reaction between iodobenzene and phenylboronic acid and turnover frequency up to 1992 h−1. When use as catalyst for reduction of 4-nitrophenol to 4-aminophenol, it delivers an outstanding rate constant of 4.22 × 10-2 s−1 with activity parameter of 51719 s-1g−1 with respect to only Pd content. The nanocatalysts also demonstrate 100% conversion of chlorobenzene to benzene within 1 h. In addition, the catalyst exhibits remarkable catalytic stability for several cycles without any significant loss of products. The excellent catalytic activities can be attributed to synergistic effect of uniformly dispersed Pd NPs, favorable interaction between metal and support, and tubular interconnected mesoporous framework of N-functionalized CMK-9 that accelerate mass transportation. The present work signifies the versatility of Pd@N-CMK-9 nanocatalysts for various catalytic reactions.



中文翻译:

N-官能化介孔碳负载钯纳米粒子作为铃木-宫浦反应、4-硝基苯酚还原和氯苯加氢脱氯的高活性纳米催化剂

通过双试剂化学还原方法开发了一系列纳米催化剂,这些催化剂来源于将钯纳米粒子 (Pd NPs) 固定在氮 (N) 功能化和无功能化介孔碳 CMK-9 的三维 (3D) 管型结构中。在此,首次探索了 N 功能化的 CMK-9 作为固定 Pd NPs 的载体,并用作 Suzuki-Miyaura 交叉偶联反应、4-硝基苯酚的还原和氯苯加氢脱氯的多功能催化剂。Pd@N-CMK-9 催化剂表现出优异的活性,碘苯和苯基硼酸之间的 Suzuki-Miyaura 反应转化率为 100%,转换频率高达 1992 h -1. 当用作将 4-硝基苯酚还原为 4-氨基苯酚的催化剂时,它提供了 4.22 × 10 -2 s -1的出色速率常数,活性参数为 51719 s -1 g -1仅关于 Pd 含量。纳米催化剂还证明了氯苯在 1 小时内 100% 转化为苯。此外,该催化剂在几个循环中表现出显着的催化稳定性,而没有任何显着的产物损失。优异的催化活性可归因于均匀分散的 Pd NPs 的协同作用、金属与载体之间的良好相互作用以及 N 官能化 CMK-9 的管状互连介孔框架加速物质传输。目前的工作表明 Pd@N-CMK-9 纳米催化剂在各种催化反应中的多功能性。

更新日期:2021-10-11
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