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利用记忆效应重构负载钌的钴镁铝水滑石用于无碱条件下5-羟甲基糠醛的选择性氧化

Reconstruction of cobalt magnesium aluminum hydrotalcite loaded ruthenium using the memory effect for selective oxidation of 5-hydroxymethylfurfural under alkali-free conditions.

作者信息

Zhang Shuang, Wang Sai, Ma Ji, Cao Suzhen

机构信息

Institute of Petrochemical Technology, Jilin Institute of Chemical Technology 45 Chengde Street Jilin 132022 PR China

出版信息

RSC Adv. 2025 Jul 18;15(31):25413-25424. doi: 10.1039/d5ra02352a. eCollection 2025 Jul 15.

Abstract

The hydrotalcite CoMgAl-LDH was prepared using a hydrothermal method. The calcined hydrotalcite was rehydrated utilizing its "memory effect", and the catalyst Ru/CoMgAl-RLDH was prepared by loading ruthenium nanoparticles through the impregnation reduction method. The pristine hydrotalcite CoMgAl-LDH exhibited a specific surface area of 9.2 m g, while the Ru-loaded reconstructed hydrotalcite Ru/CoMgAl-RLDH demonstrated a significant increase in specific surface area to 130.0 m g. The total basicity of the original hydrotalcite CoMgAl-LDH catalyst surface was 0.25 mmol g, and all these basic sites were weak basic sites. By contrast, the total basicity of the reconstructed hydrotalcite Ru/CoMgAl-RLDH catalyst surface was 0.37 mmol g, consisting of weak and moderate basic sites. The reconstructed hydrotalcite not only showed higher thermal stability than the original one but also enabled the systematic adjustment of its basic sites by changing the molar ratio of elements in the hydrotalcite and the calcination temperature. The Ru/CoMgAl-RLDH catalyst prepared with the Co : Mg : Al molar ratio of 1 : 2 : 1, calcination temperature of 400 °C, and Ru loading of 4 wt% demonstrated optimal catalytic activity, achieving complete 5-hydroxymethylfurfural (HMF) conversion and 87.6% 2,5-furandicarboxylic acid (FDCA) yield under alkali-free conditions.

摘要

采用水热法制备了水滑石CoMgAl-LDH。利用其“记忆效应”对煅烧水滑石进行再水化,并通过浸渍还原法负载钌纳米颗粒制备了催化剂Ru/CoMgAl-RLDH。原始水滑石CoMgAl-LDH的比表面积为9.2 m²/g,而负载钌的重构水滑石Ru/CoMgAl-RLDH的比表面积显著增加至130.0 m²/g。原始水滑石CoMgAl-LDH催化剂表面的总碱度为0.25 mmol/g,所有这些碱性位点均为弱碱性位点。相比之下,重构水滑石Ru/CoMgAl-RLDH催化剂表面的总碱度为0.37 mmol/g,由弱碱性和中等碱性位点组成。重构水滑石不仅比原始水滑石具有更高的热稳定性,还能通过改变水滑石中元素的摩尔比和煅烧温度来系统地调节其碱性位点。以Co : Mg : Al摩尔比为1 : 2 : 1、煅烧温度为400 °C、Ru负载量为4 wt%制备的Ru/CoMgAl-RLDH催化剂表现出最佳催化活性,在无碱条件下实现了5-羟甲基糠醛(HMF)的完全转化和2,5-呋喃二甲酸(FDCA)87.6%的产率。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3584/12272569/46e1038c7089/d5ra02352a-f1.jpg

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