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科学家研发水塑性非均相纳米粒子预催化剂
作者:小柯机器人 发布时间:2021/2/28 19:24:16

2021年2月25日,美国加州大学圣芭芭拉分校Bruce H. Lipshutz课题组在《美国化学会杂志》发表论文,宣布他们研究出水塑性非均相纳米粒子预催化剂,用于在水胶束催化条件下的Mizoroki-Heck偶联。

课题组研究出粉状球形纳米颗粒(NPs),含有ppm水平的钯,由t-Bu3P连接,由FeCl3衍生,简单暴露在水里,其形态会发生显著变化,导致纳米棒催化Mizoroki-Heck (MH)耦合反应。这种NP的改变是普遍的,表现在发生在三个不相关的含膦配体的NPs。

研究人员使用X射线光电子能谱(XPS)、能量色散X射线能谱(EDX)、透射电子显微镜(TEM)和低温透射电子显微镜(cryo-TEM)分析对每种催化剂进行了研究。在水性胶束催化条件下,室温至45°C之间发生的偶联特别依赖于含t-Bu3P连接的Pd的NP,并显示出较宽的底物范围。

与这项新技术相关的其他关键特性包括产品中的低残留Pd、水相反应介质的循环利用以及相关的低E因子。半胱氨酸碱(汉考克生物碱家族的成员)的前体的合成显示了该技术潜在的工业应用。

附:英文原文

Title: Water-Sculpting of a Heterogeneous Nanoparticle Precatalyst for Mizoroki–Heck Couplings under Aqueous Micellar Catalysis Conditions

Author: Haobo Pang, Yuting Hu, Julie Yu, Fabrice Gallou, Bruce H. Lipshutz

Issue&Volume: February 25, 2021

Abstract: Powdery, spherical nanoparticles (NPs) containing ppm levels of palladium ligated by t-Bu3P, derived from FeCl3, upon simple exposure to water undergo a remarkable alteration in their morphology leading to nanorods that catalyze Mizoroki–Heck (MH) couplings. Such NP alteration is general, shown to occur with three unrelated phosphine ligand-containing NPs. Each catalyst has been studied using X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM), and cryogenic transmission electron microscopy (cryo-TEM) analyses. Couplings that rely specifically on NPs containing t-Bu3P-ligated Pd occur under aqueous micellar catalysis conditions between room temperature and 45 °C, and show broad substrate scope. Other key features associated with this new technology include low residual Pd in the product, recycling of the aqueous reaction medium, and an associated low E Factor. Synthesis of the precursor to galipinine, a member of the Hancock family of alkaloids, is suggestive of potential industrial applications.

DOI: 10.1021/jacs.0c11484

Source: https://pubs.acs.org/doi/10.1021/jacs.0c11484

 

期刊信息

JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:14.612
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000