物理化学学报Issue(8)：1527-1534,8.DOI:10.3866/PKU.WHXB201406121
不同载体对负载型氧化钨催化剂在己二酸合成反应中的结构及性能影响
Effect of Support on the Structural Evolution and Catalytic Performance of WO3-Supported Catalysts in the Synthesis of Adipic Acid
摘要
Abstract
A series of tungsten-based catalysts were synthesized via a traditional impregnation method using SBA-15, hexagonal mesoporous silica (HMS), and SnO2 as the support. The supported catalysts were characterized by X-ray powder diffraction (XRD), transmission electron microscopy/field-emission transmission electron microscopy (TEM/FETEM), UV-Vis diffuse reflection spectroscopy (UV-Vis DRS), Raman spectrometry, X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared (FTIR) spectroscopy. It was found that the support was crucial to the dispersion and nature of the tungsten species on the catalyst. In this study, the catalytic performances of catalysts with different supports were investigated for the synthesis of adipic acid (AA) from the selective oxidation of cyclohexene oxide. The excellent catalytic performance of the catalyst was obtained over WO3/SnO2, followed by WO3/HMS and WO3/SBA-15. The XRD results indicate that the degree of crystallinity of the tungsten species of WO3/SnO2 catalyst was low and the particle size of WO3 was small (~2 nm). TEM and XPS results imply a high dispersion of tungsten species on the SnO2 support. The UV-Vis DRS spectra demonstrate the existence of [WO4] and low-polymeric tungsten species. In addition, the W-based catalyst with SnO2 as the support could retain high activity, even after being reused six times, suggesting that there is strong interaction between tungsten species and the SnO2-support that enhanced the stability of the catalyst. This shows the potential of the WO3/SnO2 as a catalyst for the synthesis of adipic acid.关键词
三氧化钨/SBA-15/HMS/二氧化锡/己二酸/高分散性Key words
Tungsten oxide/SBA-15/HMS/Tin oxide/Adipic acid/High dispersion分类
化学化工引用本文复制引用
张召艳,祝全敬,丁靖,戴维林,宗保宁..不同载体对负载型氧化钨催化剂在己二酸合成反应中的结构及性能影响[J].物理化学学报,2014,(8):1527-1534,8.基金项目
The project was supported by the National Key Basic Research Program of China (973)(2012CB224804), National Natural Science Foundation of China (21173052,21373054), State Key Laboratory of Catalytic Materials and Reaction Engineering, China (RIPP, SINOPEC), and Science and Technology Commission of Shanghai Municipality, China (08DZ2270500).国家重点基础研究发展规划项目(973)(2012CB224804),国家自然科学基金(21173052,21373054),石油化工催化材料与反应工程国家重点实验室(中国石油化工股份有限公司石油化工科学研究院)开放基金课题及上海市科委科技基金(08DZ2270500)资助 （973）
