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氧化石墨烯和还原氧化石墨烯负载的双金属Au-Sn催化剂催化苄醇高效氧化为苯甲醛

Efficient oxidation of benzyl alcohol into benzaldehyde catalyzed by graphene oxide and reduced graphene oxide supported bimetallic Au-Sn catalysts.

作者信息

Liu Lili, Zhou Xiaojing, Xin Chunling, Zhang Baoli, Zhang Guangman, Li Shanshan, Liu Li, Tai Xishi

机构信息

School of Chemistry & Chemical Engineering and Environmental Engineering, Weifang University Weifang 261061 China

出版信息

RSC Adv. 2023 Aug 7;13(34):23648-23658. doi: 10.1039/d3ra03496h. eCollection 2023 Aug 4.

Abstract

A series of bimetallic and monometallic catalysts comprising Au and Sn nanoparticles loaded on graphene oxide (GO) and reduced graphene oxide (rGO) were prepared using three distinct techniques: two-step immobilization, co-immobilization, and immobilization. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), energy dispersive X-ray (EDX), and Inductively-coupled plasma optical emission spectroscopy (ICP-OES) were used to characterize the chemical and physical properties of prepared Au-Sn bimetallic and Au or Sn monometallic nanocatalysts. The catalytic performance of the prepared nanocatalysts was evaluated in the selective oxidation of benzyl alcohol (BzOH) to benzaldehyde (BzH) using O as an oxidizing agent under moderate conditions. To obtain the optimal BzH yield, the experimental conditions and parameters, including the effects of the reaction time, temperature, pressure, and solvent type on BzOH oxidation, were optimized. Under optimal reaction conditions, bimetallic Au-Sn nanoparticles supported on GO (AuSn/GO-TS, 49.3%) produced a greater yield of BzH than the AuSn/rGO-TS catalysts (35.5%). The Au-Sn bimetallic catalysts were more active than the monometallic catalysts. AuSn/GO-TS and AuSn/rGO-TS prepared by the two-step immobilization method were more active than AuSn/GO-CoIM and AuSn/rGO-CoIM prepared by co-immobilization. In addition, the AuSn/GO-TS and AuSn/rGO-TS catalysts were easily separated from the mixture by centrifugation and reused at least four times without reducing the yield of BzH. These properties make Au-Sn bimetallic nanoparticles supported on GO and rGO particularly attractive for the environmentally friendly synthesis of benzaldehyde.

摘要

采用三种不同技术制备了一系列负载在氧化石墨烯(GO)和还原氧化石墨烯(rGO)上的包含金和锡纳米颗粒的双金属和单金属催化剂:两步固定法、共固定法和固定法。利用X射线衍射(XRD)、X射线光电子能谱(XPS)、透射电子显微镜(TEM)、能量色散X射线(EDX)和电感耦合等离子体发射光谱(ICP - OES)对制备的金 - 锡双金属和金或锡单金属纳米催化剂的化学和物理性质进行了表征。在温和条件下,以氧气作为氧化剂,在苯甲醇(BzOH)选择性氧化为苯甲醛(BzH)的反应中评估了所制备纳米催化剂的催化性能。为了获得最佳的BzH产率,对实验条件和参数进行了优化,包括反应时间、温度、压力和溶剂类型对BzOH氧化的影响。在最佳反应条件下,负载在GO上的双金属金 - 锡纳米颗粒(AuSn/GO - TS,49.3%)比负载在rGO上的AuSn/rGO - TS催化剂(35.5%)产生更高的BzH产率。金 - 锡双金属催化剂比单金属催化剂更具活性。通过两步固定法制备的AuSn/GO - TS和AuSn/rGO - TS比通过共固定法制备的AuSn/GO - CoIM和AuSn/rGO - CoIM更具活性。此外,AuSn/GO - TS和AuSn/rGO - TS催化剂通过离心可轻松从混合物中分离出来,并至少重复使用四次而不降低BzH的产率。这些特性使得负载在GO和rGO上的金 - 锡双金属纳米颗粒在苯甲醛的环境友好合成中特别具有吸引力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9563/10404934/ca7b9cd9706e/d3ra03496h-f1.jpg

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