MOF衍生碳纳米片负载的Pt上甘油的催化氧化
Catalytic Oxidation of Glycerol over Pt Supported on MOF-Derived Carbon Nanosheets.
作者信息
Ke Yihu, Zhu Chunmei, Li Jingyun, Liu Hai, Yuan Hong
机构信息
Key Laboratory of Chemical Engineering and Technology, State Ethnic Affairs Commission, School of Chemistry and Chemical Engineering, North Minzu University, Yinchuan 750021, P. R. China.
Ningxia Key Laboratory of Solar Chemical Conversion Technology, North Minzu University, Yinchuan 750021, P. R. China.
出版信息
ACS Omega. 2022 Dec 9;7(50):46452-46465. doi: 10.1021/acsomega.2c05155. eCollection 2022 Dec 20.
A series of nitrogen-doped porous carbon nanosheets (NPCNs) doped with transition-metal-supported Pt catalysts were prepared by colloidal deposition and evaluated for the selective oxidation of glycerol to glyceric acid (GLYA) under nonalkaline conditions. The transition metal contained in the catalyst was found to affect its performance and selectivity for GLYA, with the Pt/Zr@NPCN catalyst showing the highest catalytic activity and selectivity. These materials were characterized using Brunauer-Emmett-Teller surface area analysis, transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and CO temperature-programmed desorption. The results showed that the small size of the Pt nanoparticles, the interaction between the Pt nanoparticles and the support, and the unique textural properties of the catalyst all promoted glycerol conversion and GLYA selectivity. A Zr concentration of 1.5 wt % and a support preparation temperature of 800 °C were found to provide a catalyst with the optimal performance that exhibited a glycerol conversion and selectivity for GLYA of 68.62 and 77.29%, respectively, at an initial O pressure of 10 bar and 60 °C after 6 h. Even after being recycled five times, this material provided a GLYA selectivity of approximately 75%, although the glycerol conversion decreased from 68 to 50%. The insights may provide new suggestions on the design of efficient support for the selective oxidation of polyols.
通过胶体沉积法制备了一系列负载过渡金属的Pt催化剂掺杂的氮掺杂多孔碳纳米片（NPCN），并对其在非碱性条件下将甘油选择性氧化为甘油酸（GLYA）的性能进行了评估。研究发现，催化剂中所含的过渡金属会影响其对GLYA的性能和选择性，其中Pt/Zr@NPCN催化剂表现出最高的催化活性和选择性。采用布鲁诺尔-埃米特-泰勒比表面积分析、透射电子显微镜、X射线衍射、X射线光电子能谱和CO程序升温脱附等方法对这些材料进行了表征。结果表明，Pt纳米颗粒的小尺寸、Pt纳米颗粒与载体之间的相互作用以及催化剂独特的织构性质均促进了甘油的转化和GLYA的选择性。研究发现，Zr浓度为1.5 wt%且载体制备温度为800℃时，可提供一种性能最佳的催化剂，在初始O压力为10 bar、60℃条件下反应6 h后，该催化剂对甘油的转化率和对GLYA的选择性分别为68.62%和77.29%。即使经过五次循环使用，该材料对GLYA的选择性仍约为75%，尽管甘油转化率从68%降至50%。这些见解可能为多元醇选择性氧化高效载体的设计提供新的建议。
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