Ren Zhijie, Li Huanhuan, Li Jin, Cai Jun, Zhong Lian, Ma Yingqi, Pang Yajie
Key Laboratory of Marine Environment and Ecology, Ministry of Education, Ocean University of China, Qingdao 266100, China.
Key Laboratory of Marine Environment and Ecology, Ministry of Education, Ocean University of China, Qingdao 266100, China.
Int J Biol Macromol. 2023 Feb 28;229:732-745. doi: 10.1016/j.ijbiomac.2022.12.282. Epub 2022 Dec 29.
Gold nanoparticles (AuNPs) have attracted extensive attention in the past few years due to their unique properties and great potential application in catalysis. However, the application of AuNPs remains a significant challenge due to the lack of high efficiency and stability caused by aggregation. Immobilization of AuNPs on appropriate support shows promising results in avoiding aggregation and improving catalytic activity. In this work, reduced graphene oxide/chitosan/gold nanoparticles (rGO/CHS/AuNPs) composites were prepared using chitosan with different molecular weights (MW) as a reducing agent and stabilizer, and characterized by FT-IR, XRD, XPS, SEM, FESEM, EDS, TEM, HRTEM, and TGA. The preparation conditions of rGO/CHS/AuNPs composites, including chitosan MW, CHS/GO mass ratio, reaction temperature and time, and HAuCl concentration were investigated in detail. The results indicated that reduction activity of chitosan for GO increased with the decrease of chitosan MW. The C/O ratio of rGO reduced by low molecular weight chitosan (LMWC) with viscosity-average molecular weight (Mv) of 21 kDa was 6.34. Small spherical AuNPs were uniformly immobilized on the rGO surface. The particle size of AuNPs increased from 9.29 to 13.03 nm as chitosan MW decreased from 465 to 21 kDa. The rGO/CHS/AuNPs showed good catalytic activity for the reduction of 4-NP in the presence of NaBH. The catalytic activity of rGO/CHS/AuNPs was closely related to chitosan MW. rGO/CHS/AuNPs synthesized by LMWC with Mv of 21 kDa showed the highest kinetic rate constant of 0.2067 min. The results of this experimental study could be useful in the development of effective catalysts for the reduction of aromatic nitro compounds.
在过去几年中,金纳米颗粒(AuNPs)因其独特的性质以及在催化领域的巨大潜在应用而备受广泛关注。然而,由于聚集导致缺乏高效性和稳定性,AuNPs的应用仍然是一个重大挑战。将AuNPs固定在合适的载体上在避免聚集和提高催化活性方面显示出有前景的结果。在这项工作中,使用不同分子量(MW)的壳聚糖作为还原剂和稳定剂制备了还原氧化石墨烯/壳聚糖/金纳米颗粒(rGO/CHS/AuNPs)复合材料,并通过傅里叶变换红外光谱(FT-IR)、X射线衍射(XRD)、X射线光电子能谱(XPS)、扫描电子显微镜(SEM)、场发射扫描电子显微镜(FESEM)、能谱仪(EDS)、透射电子显微镜(TEM)、高分辨率透射电子显微镜(HRTEM)和热重分析(TGA)对其进行了表征。详细研究了rGO/CHS/AuNPs复合材料的制备条件,包括壳聚糖MW、CHS/GO质量比、反应温度和时间以及HAuCl浓度。结果表明,壳聚糖对氧化石墨烯的还原活性随壳聚糖MW的降低而增加。由粘均分子量(Mv)为21 kDa的低分子量壳聚糖(LMWC)还原的rGO的C/O比为6.34。小的球形AuNPs均匀地固定在rGO表面。随着壳聚糖MW从465 kDa降至21 kDa,AuNPs的粒径从9.29 nm增加到13.03 nm。rGO/CHS/AuNPs在NaBH存在下对4-硝基苯酚的还原显示出良好的催化活性。rGO/CHS/AuNPs的催化活性与壳聚糖MW密切相关。由Mv为21 kDa的LMWC合成的rGO/CHS/AuNPs显示出最高的动力学速率常数,为0.2067 min⁻¹。该实验研究结果可能有助于开发用于还原芳香族硝基化合物的有效催化剂。