Deng Xin, Zhu Lihua, Zhang Huan, Li Liqing, Zhao Ning, Wang Jiexiang, Osman Sameh M, Luque Rafael, Chen Bing Hui
Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, College of Chemistry and Chemical Engineering, Faculty of Materials Metallurgy and Chemistry, Jiangxi University of Science and Technology, Ganzhou, 341000, Jiang Xi, China.
Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, College of Chemistry and Chemical Engineering, Faculty of Materials Metallurgy and Chemistry, Jiangxi University of Science and Technology, Ganzhou, 341000, Jiang Xi, China; Guangdong Provincial Key Lab of Green Chemical Product Technology, Key Laboratory of Fuel Cell Technology of Guangdong Province, South China University of Technology, Guangzhou, 510640, China.
Environ Res. 2022 Nov;214(Pt 4):114027. doi: 10.1016/j.envres.2022.114027. Epub 2022 Aug 18.
A covalent organic framework (COF) was used as the support of the catalyst in this work in order to obtain an environmentally friendly catalyst with high catalytic performance, selectivity and stability for 4-nitrophenol hydrogenation. Pd tiny particles are fixed in the cavity of COF to obtain Pd/COF catalysts, which has a quite narrow particle size distribution (5.09 ± 1.30 nm). As-prepared Pd/COF catalysts (Pd loading-2.11 wt%) shows excellent catalytic performance (conversion - 99.3%, selectivity >99.0% and turnover frequency (TOF)-989.4 h) for 4-nitrophenol hydrogenation under relatively mild reaction conditions of reaction temperature-40 °C and reaction pressure-3.0 MPa H, and Pd/COF catalysts have high stability. Pd/COF catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscope energy-dispersive X-ray spectroscopy (SEM-EDS), transmission electron microscope (TEM), high resolution TEM (HRTEM), Brunauer-Emmett-Teller (BET), scanning TEM energy-dispersive X-ray spectroscopy (STEM-EDS) elemental analysis techniques to prove that the Pd nanoparticles are highly dispersed on the COF. Pd/COF catalysts have good stability and reusability hence with certain industrial application value.
在本工作中，共价有机框架（COF）被用作催化剂的载体，以获得一种对4-硝基苯酚加氢具有高催化性能、选择性和稳定性的环境友好型催化剂。钯微小颗粒固定在COF的空腔中以获得Pd/COF催化剂，其粒径分布相当窄（5.09±1.30纳米）。所制备的Pd/COF催化剂（钯负载量为2.11 wt%）在反应温度40℃和反应压力3.0 MPa H₂的相对温和反应条件下，对4-硝基苯酚加氢表现出优异的催化性能（转化率-99.3%，选择性>99.0%，周转频率（TOF）-989.4 h⁻¹），并且Pd/COF催化剂具有高稳定性。通过X射线衍射（XRD）、X射线光电子能谱（XPS）、扫描电子显微镜-能量色散X射线光谱（SEM-EDS）、透射电子显微镜（TEM）、高分辨率TEM（HRTEM）、布鲁诺尔-埃米特-泰勒（BET）、扫描TEM-能量色散X射线光谱（STEM-EDS）等元素分析技术对Pd/COF催化剂进行了表征，以证明钯纳米颗粒高度分散在COF上。Pd/COF催化剂具有良好的稳定性和可重复使用性，因此具有一定的工业应用价值。
