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Tetraalkylammonium Functionalized Hydrochars as Efficient Supports for Palladium Nanocatalysts
ChemCatChem ( IF 3.8 ) Pub Date : 2020-03-09 , DOI: 10.1002/cctc.201902305
Tiago A. G. Duarte 1, 2 , Isabelle Favier 3 , Christian Pradel 3 , Luísa M. D. R. S. Martins 1 , Ana P. Carvalho 2 , Daniel Pla 3 , Montserrat Gómez 3
Affiliation  

With the aim of preparing bio‐sourced supports with enhanced properties in catalysis, we devised an original strategy allowing the immobilization of metal nanoparticles. Thus, size‐controlled hydrochars with a high degree of hydroxyl functionalities, from both neat sucrose or modified with acrylic acid (10 wt.%), were derivatized with ether linkers containing ammonium groups. These non‐porous carbon‐based materials were used as suitable supports for the immobilization of palladium nanoparticles. The catalytic materials were synthesized by reduction of Pd(OAc)2 to Pd(0) under H2 atmosphere in the presence of the corresponding hydrochar, and fully characterized by standard methods. Among the different hydrochar‐supported palladium materials, those functionalized with tetraalkylammonium groups afforded heterogeneous catalysts, exhibiting high activity in hydrogenations of different types of substrates (alkynes, alkenes, and carbonyl and nitro derivatives). The most efficient catalyst was recycled up to ten runs without loss of catalytic behavior, in agreement with the unchanged composite materials after catalysis (Transmission Electron Microscopy (TEM) analyses) and the lack of metal leaching in the extracted organic products (no palladium detected by Inductively Coupled Plasma‐Atomic Emission Spectrometry (ICP‐AES)); these systems exhibited enhanced recyclability properties as compared to commercial Pd/C catalyst.

中文翻译:

四烷基铵官能化烃类作为钯纳米催化剂的有效载体

为了制备具有增强的催化性能的生物来源载体,我们设计了一种独创的策略来固定金属纳米颗粒。因此,无论是纯蔗糖还是丙烯酸改性(10 wt。%)的,具有高度羟基官能度的大小受控的烃类都可以通过含有铵基的醚连接基衍生化。这些无孔碳基材料被用作固定钯纳米颗粒的合适载体。通过在H 2下将Pd(OAc)2还原为Pd(0)来合成催化材料相应的水焦炭存在下,通过标准方法充分表征。在不同的以烃为载体的钯材料中,用四烷基铵基团官能化的材料提供了多相催化剂,在不同类型的底物(炔烃,烯烃,羰基和硝基衍生物)的氢化中表现出很高的活性。与催化后不变的复合材料(透射电子显微镜(TEM)分析)和萃取的有机产物中没有金属浸出(通过检测未发现钯)相一致,最有效的催化剂可循环使用十次而不会失去催化性能。电感耦合等离子体原子发射光谱法(ICP-AES)); 与市售Pd / C催化剂相比,这些系统具有增强的可回收性。
更新日期:2020-04-22
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