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通过柠檬酸改性获得的表面原纤化纤维素负载金纳米颗粒的尺寸控制制备

Size-Controlled Preparation of Gold Nanoparticles Deposited on Surface-Fibrillated Cellulose Obtained by Citric Acid Modification.

作者信息

Chutimasakul Threeraphat, Uetake Yuta, Tantirungrotechai Jonggol, Asoh Taka-Aki, Uyama Hiroshi, Sakurai Hidehiro

机构信息

Department of Chemistry and Center of Excellence for Innovation in Chemistry, Faculty of Science, Mahidol University, Bangkok 10400, Thailand.

Division of Applied Chemistry, Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan.

出版信息

ACS Omega. 2020 Dec 17;5(51):33206-33213. doi: 10.1021/acsomega.0c04894. eCollection 2020 Dec 29.

Abstract

Cellulose-based functional materials have gained immense interest due to their low density, hydrophilicity, chirality, and degradability. So far, a facile and scalable preparation of fibrillated cellulose by treating the hydroxy groups of cellulose with citric acid (F-CAC) has been developed and applied as a reinforcing filler for polypropylene composite. Herein, a size-selective preparation of Au nanoparticles (NPs) stabilized by F-CAC is described. By modifying the conditions of transdeposition method, established in our group previously, a transfer of Au NPs from poly(-vinyl-2-pyrrolidone) (PVP) to F-CAC proceeded up to 96% transfer efficiency with retaining its cluster sizes in EtOH. Meanwhile, the deposition efficiency drastically decreased in the case of nonmodified cellulose, showing the significance of citric acid modification. A shift of binding energy at Au 4f core level X-ray photoelectron spectroscopy from 82.0 to 83.3 eV indicated that the NPs were stabilized on an F-CAC surface rather than by PVP matrix. The reproducible particle size growth was observed when 2-propanol was used as a solvent instead of EtOH, expanding the range of the available particle size with simple manipulation. The thus-obtained Au:F-CAC nanocatalysts exhibited a catalytic activity toward an aerobic oxidation of 1-indonol in toluene to yield 1-indanone quantitatively and were recyclable at least six times, illustrating high tolerance against organic solvents.

摘要

基于纤维素的功能材料因其低密度、亲水性、手性和可降解性而备受关注。到目前为止,已经开发出一种通过用柠檬酸处理纤维素的羟基来制备原纤化纤维素的简便且可扩展的方法(F-CAC),并将其用作聚丙烯复合材料的增强填料。在此,描述了一种由F-CAC稳定的金纳米颗粒(NPs)的尺寸选择性制备方法。通过改变我们小组之前建立的转沉积方法的条件,金纳米颗粒从聚(乙烯基-2-吡咯烷酮)(PVP)转移到F-CAC上,转移效率高达96%,且在乙醇中保持其团簇尺寸。同时,在未改性纤维素的情况下,沉积效率急剧下降,这表明柠檬酸改性的重要性。金4f核心能级X射线光电子能谱中结合能从82.0 eV 变为83.3 eV,表明纳米颗粒稳定在F-CAC表面而不是由PVP基质稳定。当使用2-丙醇代替乙醇作为溶剂时,观察到可重复的粒径增长,通过简单操作扩大了可用粒径范围。如此获得的Au:F-CAC纳米催化剂对甲苯中1-茚醇的需氧氧化表现出催化活性,定量生成1-茚酮,并且至少可循环使用六次,说明对有机溶剂具有高耐受性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/809f/7774275/9206236c21e9/ao0c04894_0006.jpg

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