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通过扩孔和钯锌合金化促进铃木耦合反应。

Boosting Suzuki coupling reaction via pore expanding and palladium-zinc alloying.

作者信息

He Hongwei, Ma Zhoulin, Zhang Shuya, Cai An, Ye Huan, Fan Xiaobin, Peng Wenchao, Li Yang

机构信息

School of Chemical Engineering and Technology, Tianjin University, Tianjin 300354, PR China.

School of Chemical Engineering and Technology, Tianjin University, Tianjin 300354, PR China; Institute of Shaoxing, Tianjin University, Zhejiang 312300, PR China.

出版信息

J Colloid Interface Sci. 2025 Feb;679(Pt A):152-160. doi: 10.1016/j.jcis.2024.09.232. Epub 2024 Sep 29.

DOI:10.1016/j.jcis.2024.09.232
PMID:39362140
Abstract

A palladium-zinc alloy nanoparticles decorated nitrogen-doped porous carbon catalyst (PdZn-NC) was synthesized and utilized for Suzuki coupling reaction. The alloying palladium (Pd) with zinc (Zn) and pore expanding are realized simultaneously. Density functional theory (DFT) calculations and experimental studies reveal that the alloying Pd with Zn can lower the energy barrier in Suzuki coupling reaction. Nitrogen adsorption-desorption measurements uncover that pore expansion caused by the zinc nitrate hexahydrate assisted calcination gives rise to the multiplication of mesopore with a pore diameter of 6 nm, which facilitates mass transfer during the reaction. As a result, the alloying Pd with Zn and pore expanding together endow PdZn-NC with excellent catalytic activity. PdZn-NC demonstrates exceptional catalytic activity and stability in Suzuki coupling reaction. A high biphenyl yield of 97.7 % within 40 min and stable reusability of 93.3 % yield after five reuse cycles can be achieved. This work not only offers a viable method for Suzuki coupling reaction, but also provides insights for designing new catalysts toward Suzuki coupling reaction.

摘要

合成了一种钯锌合金纳米颗粒修饰的氮掺杂多孔碳催化剂(PdZn-NC)并将其用于铃木耦合反应。钯(Pd)与锌(Zn)合金化以及孔径扩大得以同时实现。密度泛函理论(DFT)计算和实验研究表明,钯与锌合金化可降低铃木耦合反应中的能垒。氮吸附-脱附测量结果表明,六水合硝酸锌辅助煅烧引起的孔径扩大导致了孔径为6纳米的中孔数量增加,这有利于反应过程中的传质。结果,钯与锌合金化以及孔径扩大共同赋予了PdZn-NC优异的催化活性。PdZn-NC在铃木耦合反应中表现出卓越的催化活性和稳定性。40分钟内联苯产率高达97.7%,五次重复使用循环后产率稳定在93.3%。这项工作不仅为铃木耦合反应提供了一种可行的方法,还为设计用于铃木耦合反应的新型催化剂提供了思路。

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