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沉积在表面改性碳干凝胶上的金纳米颗粒作为在一氧化碳和水存在下用于环己烷C-H活化的可重复使用催化剂。

Gold Nanoparticles Deposited on Surface Modified Carbon Xerogels as Reusable Catalysts for Cyclohexane C-H Activation in the Presence of CO and Water.

作者信息

Ribeiro Ana Paula da Costa, Martins Luísa Margarida Dias Ribeiro de Sousa, Carabineiro Sónia Alexandra Correia, Figueiredo José Luís, Pombeiro Armando José Latourrette

机构信息

Centro de Química Estrutural, Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais, 1049-001 Lisboa, Portugal.

Chemical Engineering Department, Instituto Superior de Engenharia de Lisboa, Instituto Politécnico de Lisboa, R. Conselheiro Emídio Navarro, 1959-007 Lisboa, Portugal.

出版信息

Molecules. 2017 Apr 9;22(4):603. doi: 10.3390/molecules22040603.

Abstract

The use of gold as a promotor of alkane hydrocarboxylation is reported for the first time. Cyclohexane hydrocarboxylation to cyclohexanecarboxylic acid (up to 55% yield) with CO, water, and peroxodisulfate in a water/acetonitrile medium at circa 50 °C has been achieved in the presence of gold nanoparticles deposited by a colloidal method on a carbon xerogel in its original form (CX), after oxidation with HNO₃ (-ox), or after oxidation with HNO₃ and subsequent treatment with NaOH (-ox-Na). Au/CX-ox-Na behaves as re-usable catalyst maintaining its initial activity and selectivity for at least seven consecutive cycles. Green metric values of atom economy or carbon efficiency also attest to the improvement brought by this novel catalytic system to the hydrocarboxylation of cyclohexane.

摘要

首次报道了金作为烷烃氢羧基化促进剂的应用。在水/乙腈介质中,于约50℃下,以胶体法将金纳米颗粒沉积在原始形式的碳干凝胶(CX)上、用HNO₃氧化后(-ox)或用HNO₃氧化并随后用NaOH处理后(-ox-Na),实现了环己烷与CO、水和过二硫酸盐氢羧基化为环己烷羧酸(产率高达55%)。Au/CX-ox-Na表现为可重复使用的催化剂,至少连续七个循环保持其初始活性和选择性。原子经济性或碳效率的绿色指标值也证明了这种新型催化体系给环己烷氢羧基化带来的改进。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/18b3/6154559/6cc51cf30abb/molecules-22-00603-sch001.jpg

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