Ke Yi-Hu, Zhu Chun-Mei, Xu Huan-Huan, Wang Xue, Liu Hai, Yuan Hong
Key Laboratory for Chemical Engineering and Technology, State Ethnic Affairs Commission, North Minzu University Yinchuan 750021 P. R. China.
Ningxia Key Laboratory of Solar Chemical Conversion Technology, North Minzu University Yinchuan 750021 P. R. China.
RSC Adv. 2023 Sep 8;13(39):27054-27065. doi: 10.1039/d3ra04300b.
The catalytic conversion of biomass-derived glycerol into high-value-added products, such as glyceric acid (GLYA), using catalyst-supported Au nanoparticles (Au NPs) at room temperature presents a significant challenge. In this study, we constructed a series of supported Au catalysts, including Au/ZrO@C, Au/C, Au/ZrO, and Au/ZrO-C, and investigated their effectiveness in selectively catalytic oxidizing glycerol to GLYA at room temperature. Among these catalysts, the Au/ZrO@C catalyst exhibited the best catalytic performance, achieving a glycerol conversion rate of 73% and a GLYA selectivity of 79% under the optimized reaction conditions (reaction conditions: 30 mL 0.1 M glycerol, glycerol/Au = 750 mol mol, = 25 °C, (O) = 10 bar, stirring speed = 600 rpm, time = 6 h). Physical adsorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and other characterization methods were employed to analyze the texture properties of the catalyst. The findings indicated that the support structure, the strong metal-support interactions between Au NPs and the support, and the presence of small metallic Au NPs were the primary factors contributing to the catalyst's high activity and selectivity. Moreover, the reusability of the Au/ZrO@C catalyst was investigated, and a probable reaction mechanism for the oxidation of glycerol was proposed.
在室温下使用负载型金纳米颗粒(Au NPs)将生物质衍生的甘油催化转化为高附加值产品,如甘油酸(GLYA),是一项重大挑战。在本研究中,我们构建了一系列负载型金催化剂,包括Au/ZrO@C、Au/C、Au/ZrO和Au/ZrO-C,并研究了它们在室温下将甘油选择性催化氧化为GLYA的有效性。在这些催化剂中,Au/ZrO@C催化剂表现出最佳的催化性能,在优化的反应条件下(反应条件:30 mL 0.1 M甘油,甘油/Au = 750 mol/mol,温度 = 25 °C,氧气压力 = 10 bar,搅拌速度 = 600 rpm,时间 = 6 h),甘油转化率达到73%,GLYA选择性达到79%。采用物理吸附、X射线衍射(XRD)、X射线光电子能谱(XPS)、透射电子显微镜(TEM)等表征方法分析了催化剂的织构性质。研究结果表明,载体结构、Au NPs与载体之间强烈的金属-载体相互作用以及小尺寸金属Au NPs的存在是导致催化剂具有高活性和选择性的主要因素。此外,还研究了Au/ZrO@C催化剂的可重复使用性,并提出了甘油氧化的可能反应机理。