【摘要】 采用水热法合成了金属有机骨架材料MIL-100（Cr）,通过双溶剂浸渍和氢气还原制备了双功能催化剂Pd/MIL-100（Cr）.以苯甲醇一步氧化制缩醛为模型反应,研究了载体表面酸性质对催化性能的影响.结果表明,串联反应可以有效提高苯甲醇氧化反应的速率,不同还原温度及活化温度均对MIL-100（Cr）的酸性质有影响,进而影响缩醛产物的选择性.吡啶吸附红外光谱（Py-FTIR）及氨程序升温脱附（NH₃-TPD）表征结果表明,升高催化剂处理温度,L酸中心增加,B酸中心减少,B酸中心对提高缩醛选择性有利.在最优条件下,70℃反应12 h,苯甲醇的转化率大于99.9%,缩醛的选择性为76.2%.采用X射线光电子能谱（XPS）表征了Pd物种及载体MIL-100（Cr）的电子性质,考察了催化剂的循环稳定性;通过X射线粉末衍射仪（XRD）、场发射扫描电子显微镜（SEM）、氮气吸附-脱附等温线及NH₃-TPD表征分析了催化剂失活的原因.更多还原

【Abstract】 MIL-100（Cr） was hydrothermally synthesized and used as a solid-acid catalyst support.Pd nanoparticles were impregnated on MIL-100（Cr） by a double-solvent approach followed by hydrogen reduction to obtain Pd/MIL-100（Cr）.One-step tandem conversion of benzyl alcohol to acetal was selected as a model reaction,and the influence of acid property of MIL-100 on the product distribution was investigated.The results showed that Pd/MIL-100（Cr） catalyzed tandem reaction could accelerate the benzyl alcohol oxidation,and different reduction and activation temperatures had an impact on the acid properties of MIL-100（Cr）,which in turn affected the selectivity of acetal.The acid properties were characterized by pyridine adsorption infrared spectroscopy（Py-FTIR） and temperature programmed desorption of ammonia（NH₃-TPD）,the result showed that increasing the catalyst treatment temperature,the L acid sites increased,the B acid sites decreased,and the B acid sites was beneficial to improve the selectivity of acetal.Under optimal conditions,a benzyl alcohol conversion of 99.9%and acetal selectivity of 76.2%can be achieved at 70℃in 12 h.X-ray photoelectron spectroscopy（XPS） analysis was used to characterize the electronic properties of the Pd species and the MIL-100（Cr）,the cycling stability of the catalyst was investigated,and the reasons for the deactivation of the catalyst were analyzed by powder X-ray diffraction（XRD）,scanning electron microscopy（SEM）,N₂ adsorption-desorption isotherms and NH₃-TPD.更多还原