Ni/SiO2-Al2O3固体酸催化剂催化氢解碱木质素制备芳香类化合物  

Depolymerization of the Alkali Lignin for Aromatic Compounds over Ni/SiO_2-Al_2O_3 Solid Acid Catalysts

作　　者：周列 吴青云 徐莹[2] 王晨光[2] 马隆龙[2] 李文志[1] 陈佩丽[2] ZHOU Lie;WU Qingyun;XU Ying;WANG Chenguang;MA Longlong;LI Wenzhi;CHEN Peili(Nano Science and Technology Institute, University of Science and Technology of China, Suzhou 215123, China;Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, CAS Key Laboratory of Renewable Energy, Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development, Gnangzhou 510640, China)

机构地区：[1]中国科学技术大学纳米科学与技术学院,苏州215123 [2]中国科学院广州能源研究所,中国科学院可再生能源重点实验室,广东省新能源和可再生能源研究开发与应用重点实验,广州510640

出　　处：《高等学校化学学报》2018年第4期735-742,共8页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金(批准号：51676191); 广东省特支计划青年拔尖人才计划(批准号：2015TQ01W652); 广东省科技计划项目(批准号：2014A010106019); 中国科学院青年创新促进会项目(批准号：2016313)资助

摘　　要：以具有弱酸中心和中强酸中心的无定形硅铝为载体,负载Ni基催化剂,对碱木质素进行解聚制备了芳香类化合物.考察了Ni负载量、反应温度和反应时间对碱木质素氢解产物生成及分布的影响.对解聚产物进行气相色谱(GC)、气相色谱-质谱(GC-MS)及傅里叶变换红外光谱(FTIR)等分析,探讨了氢解反应过程.研究结果表明,催化剂的酸性是促进木质素解聚生成芳烃类产物的主要因素,且随着催化剂酸量的增加,芳烃类产物的收率呈上升趋势.以15%Ni/SiO_2-Al_2O_3为催化剂氢解木质素时,随着反应温度升高,芳香类化合物收率先增加后降低,在反应温度为300℃时最优,芳烃类产物收率为9.05%,芳香类化合物总收率为22.53%.随着反应时间的延长,芳香烃类产物收率先增加,后趋于稳定,酚类化合物收率逐渐提高,反应12 h时,芳香类化合物收率最高为26.54%.Optional discarded and unreasonable utilization of industrial alkali lignin leaded to water and air pollution. However,alkali lignin could be utilized as fine chemical resource for its specific phenyl propane structure. In this paper,we investigated efficient depolymerization methods on alkali lignin aiming for aromatic products over acidic SiO2-Al2O3 and Ni/SiO2-Al2O3 by one-step. The effects of Ni metal loading contents,reaction temperature and reaction time in this process were also discussed. Analysis of lignin depolymerized products were carried with gas chromatography（ GC）, gas chromatography-mass spectrometry（ GC-MS）,Fourier transform-infrared spectroscopy（ FTIR）. The results showed that Ni/SiO2-Al2O3 can promote the conversion of the alkali lignin. Yield（ mass fraction） of aromatic products increased and then decreased along with the rising of reaction temperature,which the yield of arenes was 9. 05% and the yield of aromatic products was 22. 53% over 15% Ni/SiO2-Al2O3 catalyst at 300 ℃ after depolymerization. Reaction time also showed significantly influence on depolymerized products,with the reaction times increasing. The arenes yield was increased and then stabilized,aromatic products yield reached 26. 54% after reacted 12 h.

关 键 词：镍催化剂 碱木质素 氢解 芳香化合物 

分 类 号：O643[理学—物理化学]