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微晶纤维素负载金纳米催化剂用于苯硼酸的偶联反应。

Microcrystalline Cellulose-Supported Gold Nanoparticle Catalysts for Homocoupling of Phenylboronic Acids.

机构信息

Department of Inorganic Chemistry, University of Madras, Guindy Campus, Chennai 600025, India.

出版信息

Langmuir. 2022 Feb 22;38(7):2205-2212. doi: 10.1021/acs.langmuir.1c02264. Epub 2022 Feb 11.

Abstract

A solid-grinding strategy for the large-scale synthesis of solid microcrystalline cellulose (MCC)-supported gold nanoparticle (NP) catalysts without using solvents and a sophisticated purification technique is reported. In contrast to typical solution-based methods, the deposition of high loading of gold NPs with greater uniformity on native MCC polymers without chemical modifications was achieved rapidly by manual grinding. The Fourier transform infrared (FT-IR) study revealed that the abundant hydroxyl functional groups present on the MCC support could effectively hold tiny gold NPs through hydrogen bonding between the -OH groups of MCC and gold NPs, thereby making the MCC-supported gold NPs stable heterogeneous catalysts. Thus, the Au/MCC catalyst exhibits higher catalytic activity and selectivity toward homocoupling of phenylboronic acids into corresponding biphenyls in water under air. Compared to other solid-supported gold NP catalysts, the MCC-supported gold catalysts showed greater catalytic activity and selectivity in the homocoupling of phenylboronic acids. The kinetics study on the homocoupling reaction catalyzed by Au/MCC reveals that the catalysts possess much lower apparent activation energy than the reported gold catalysts. Thus, the present sustainable approach may inspire more studies on the design of renewable biopolymer matrix-supported gold NPs in a large scale for heterogeneous catalysis.

摘要

一种无需使用溶剂和复杂纯化技术的大规模合成固载金纳米颗粒(NP)催化剂的固态研磨策略被报道。与典型的基于溶液的方法相比,通过手动研磨可以快速将高负载量的金 NP 更均匀地沉积在天然 MCC 聚合物上,而无需进行化学修饰。傅里叶变换红外(FT-IR)研究表明,MCC 载体上丰富的羟基官能团可以通过 MCC 和金 NP 之间的-OH 基团之间的氢键有效地固定微小的金 NP,从而使 MCC 负载的金 NP 成为稳定的多相催化剂。因此,Au/MCC 催化剂在空气中的水中对苯硼酸的同偶联反应表现出更高的催化活性和选择性。与其他负载型金 NP 催化剂相比,MCC 负载的金催化剂在苯硼酸的同偶联反应中表现出更高的催化活性和选择性。Au/MCC 催化的同偶联反应的动力学研究表明,催化剂的表观活化能明显低于报道的金催化剂。因此,这种可持续的方法可能会激发更多关于可再生生物聚合物基质负载金 NP 的设计用于多相催化的研究。

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