摘要
由于能源危机和温室效应,生物燃料作为化石燃料的替代品已经引起了全世界的广泛关注。以硬脂酸甲酯为模型化合物和甲酸(FA)为氢供体,探索了活性炭(AC)负载的Pt-Mo双功能催化剂的煅烧条件及其在催化硬脂酸甲酯原位加氢反应中的应用。结果表明:N2煅烧气氛能够增强Pt和Mo的相互作用,从而促进低氢供体用量条件下的反应活性;煅烧温度主要影响Mo组分的晶相和Pt-Mo相互作用,在750℃煅烧的Pt-Mo/AC-750催化剂在低氢供体用量(n(FA)∶n(硬脂酸甲酯)=3.9)下目标产物总收率达到95.4%,TON达到59.96 h-1。MoOxCy的存在和强烈的Pt-Mo相互作用是Pt-Mo/AC-750催化剂高活性的原因。催化剂表面活性位掩盖是导致活性降低的主要原因,将重复4次的催化剂通过750℃煅烧4 h再生后,目标产物总收率从45.8%恢复到86.2%。
Biofuel as an alternative to fossil fuel has attracted worldwide attention due to energy crisis and greenhouse effect.The calcination conditions of activated carbon(AC)supported Pt-Mo bifunctional catalyst and its application in in-situ hydrogenation of methyl stearate were investigated by using methyl stearate as model compound and formic acid(FA)as hydrogen donor.The results show that N_(2)calcination atmosphere can enhance the interaction between Pt and Mo,thus promoting the reactivity under the condition of low hydrogen donor dosage.The calcination temperature mainly affects the crystal phase of Mo component and the Pt-Mo interaction.The total yield and TON of Pt-Mo/AC-750 catalyst calcined at 750℃reached 95.4%and 59.96 h^(-1)at low hydrogen donor dosage(n(FA)∶n(methyl stearate)=3.9),respectively.The presence of MoO_(x)C_(y)and the strong Pt-Mo interaction are the reasons for the high activity of Pt-Mo/AC-750 catalyst.The main reason for the decrease of activity was the covering of the active sites on the surface of the catalyst.The total yield of the target product recovers from 45.8%to 86.2%after the catalyst,which was repeated four times,was regenerated by calcining at 750℃for 4 h.
作者
杨微
郑雨欣
吴可荆
朱英明
刘颖颖
鲁厚芳
梁斌
YANG Wei;ZHENG Yu-xin;WU Ke-jing;ZHU Ying-ming;LIU Ying-ying;LU Hou-fang;LIANG Bin(School of Chemical Engineering,Sichuan University,Chengdu 610065,China;Institute of New Energy and Low-Carbon Technology,Sichuan University,Chengdu 610207,China)
出处
《化学试剂》
CAS
北大核心
2021年第11期1457-1465,共9页
Chemical Reagents
基金
国家自然科学基金资助项目(21808148)。
