摘要
采用浸渍法制备了有机硅烷改性的UiO-66铜基催化剂(CuO/Si-UiO-66),并对其进行了有关CO_(2)加氢制甲醇的实验研究。通过X射线衍射(XRD)、傅里叶变换红外光谱(FTIR)、X射线光电子能谱(XPS)、热重(TG)等表征方法考察了有机硅烷改性对催化剂的性能与结构的影响。实验结果显示,有机硅烷改性后的催化剂相较于UiO-66的CO_(2)转换率、甲醇选择性有了明显的提高,并且稳定性方面有了显著的增强。这可能是因为有机硅烷中硅的进入到UiO-66骨架中使其结构稳定性得以保持,从而可以更好的限制分布较均匀的CuO纳米粒子。此外,还对催化剂进行CO_(2)加氢合成甲醇的催化性能测试。在180℃、3 MPa的反应条件下CH3OH的时空产率最高,达到了72.4 mmol/(gMeoH·h)。
In this paper,organosilane-modified UiO-66 copper-based catalysts(CuO/Si-UiO-66)were prepared by the impregnation method and experimentally investigated with respect to CO_(2) hydrogenation to methanol.The effect of organosilane modification on the performance and structure of the catalysts was investigated by using characterization methods such as X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR),X-ray photoelectron spectroscopy(XPS),and thermogravimetry(TG).The experimental results showed that the organosilane-modified catalysts showed a significant improvement in CO_(2) conversion,methanol selectivity,and a significant enhancement in stability compared to UiO-66.This may be attributed to the fact that the entry of silicon in the organosilanes into the UiO-66 skeleton allowed its structural stability to be maintained,which could better confine the more uniformly distributed CuO nanoparticles.In addition,the catalysts were tested for their catalytic performance in the synthesis of methanol by CO_(2) hydrogenation.The highest spatiotemporal yield of CH 3OH was achieved at 180℃and 3 MPa under the reaction conditions,reaching 72.4 mmol/(g MeoH·h).
作者
彭一帆
纳薇
高文桂
黄浩
PENG Yifan;NA Wei;GAO Wengui;HUANG Hao(State Key Laboratory for Clean Utilization of Complex Nonferrous Metal Resources,Kunming University of Science and Technology,Kunming 650093,China;Faculty of Metallurgical and Energy Engineering,Kunming University of Science and Technology,Kunming 650093,China)
出处
《功能材料》
北大核心
2025年第1期1133-1138,共6页
Journal of Functional Materials
基金
云南省科技重大专项(202302AG050005)
云南省万人计划项目(YNWR-QNBJ-2020-016)。
