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二维超薄表面活性剂包裹的多金属氧酸盐组装体作为载体,用于单分散高催化活性和稳定性的贵金属纳米粒子。

Two-dimensional ultrathin surfactant-encapsulating polyoxometalate assemblies as carriers for monodispersing noble-metal nanoparticles with high catalytic activity and stability.

机构信息

Key Laboratory of Polyoxometalate Science of Ministry of Education, Faculty of Chemistry, Northeast Normal University, Changchun, 130024, P. R. China.

出版信息

Dalton Trans. 2021 Feb 9;50(5):1666-1671. doi: 10.1039/d0dt03976d.

Abstract

Noble metal nanoparticles (NMNPs) with excellent catalytic activity and stability play an important role in the field of environmental governance. A uniform distribution and a strong binding force with the carriers of the noble metal nanoparticles are important, but avoidance of the use of additional reducing agents is a promising direction of research. Herein, 2D ultrathin surfactant-encapsulating polyoxometalate (SEP) nanosheets constructed by the self-assembly of dodecyldimethylammonium bromide (DODA) and molybdophosphate (H3PMo12O40, PMo12) are designed to be versatile carriers for Ag nanoparticles. Under the synergistic effect of the well-arranged PMo12 units, encapsulating hydrophobic oleic acid (OA) and reductive molybdophosphate under Xe lamp irradiation, the silver oleate (AgOA)-derived Ag nanoparticles (5 ± 2 nm) are monodispersed on the DODA-PMo12 assemblies and form the Agx/DODA-PMo12 composite. The optimized Ag4.89/DODA-PMo12 composite exhibits high catalytic activity and stability in the degradation of 4-nitrophenol (4-NP), which reaches a superior rate constant of 6.49 × 10-3 s-1 and without significant deterioration after three recycles. This technique can be facilely promoted to other noble metal nanoparticles with excellent catalytic activity and stability.

摘要

贵金属纳米粒子(NMNPs)具有优异的催化活性和稳定性,在环境治理领域发挥着重要作用。贵金属纳米粒子与载体之间具有均匀的分布和较强的结合力非常重要,但避免使用额外的还原剂是一个有前途的研究方向。本文设计了由十二烷基二甲基溴化铵(DODA)和磷钼酸盐(H3PMo12O40,PMo12)自组装而成的二维超薄表面活性剂包裹的多金属氧酸盐(SEP)纳米片,作为 Ag 纳米粒子的多功能载体。在排列整齐的 PMo12 单元的协同作用下,在 Xe 灯照射下,疏水性油酸钠(OA)和还原态磷钼酸盐被包裹,AgOA 衍生的 Ag 纳米粒子(5±2nm)均匀分散在 DODA-PMo12 组装体上,并形成 Agx/DODA-PMo12 复合材料。优化后的 Ag4.89/DODA-PMo12 复合材料在 4-硝基苯酚(4-NP)的降解中表现出高催化活性和稳定性,其速率常数高达 6.49×10-3 s-1,经过三次循环后没有明显的性能下降。该技术可以方便地推广到其他具有优异催化活性和稳定性的贵金属纳米粒子。

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