水滑石基Ni/Al_(2)O_(3)催化剂催化玉米秸秆加氢裂解制二元醇和芳香族单体性能研究  

Study on performance of hydrotalcite-derived Ni/Al_(2)O_(3) catalyst in hydrocracking of corn stover into diols and aromatic monomers

作　　者：马泽暐 温哲 MA Zewei;WEN Zhe(SINOPEC Research Institute of Petroleum Processing Co.,Ltd.,Beijing 100083,China;School of Petrochemical Engineering,Changzhou University,Changzhou 213164,Jiangsu,China)

机构地区：[1]中石化石油化工科学研究院有限公司,北京100083 [2]常州大学石油化工学院,江苏常州213164

出　　处：《低碳化学与化工》2024年第6期63-72,共10页Low-Carbon Chemistry and Chemical Engineering

基　　金：国家自然科学基金(U20B6002);江苏省高等学校基础科学(自然科学)研究面上项目(23KJD530001)。

摘　　要：生物质是化石能源最有前景的可再生替代品之一,由生物质制备高附加值化学品是实现生物质多元化应用的有效途径。采用尿素沉淀法和程序升温还原法制备了水滑石基Ni/Al_(2)O_(3)催化剂,通过X射线衍射(XRD)分析了催化剂及其前驱体的物相组成,并考察了Ni/Al_(2)O_(3)催化剂对玉米秸秆在水-甲醇混合溶剂中加氢裂解反应的催化性能。结果表明,Ni/Al_(2)O_(3)催化剂表现出较好的催化活性,在最优反应条件(V(H_(2)O):V(CH_(3)OH)=7:3、240℃和3.0 MPa H_(2))下,玉米秸秆转化率接近100%,二元醇产率为38.8%,芳香族单体产率为13.6%。V(H_(2)O):V(CH_(3)OH)和反应温度显著影响了玉米秸秆转化率和小分子产物产率,Ni/Al_(2)O_(3)催化剂和反应气氛主要影响了小分子产物产率和分布。对经过一次循环后的催化剂进行循环性测试发现,二元醇产率和芳香族单体产率分别下降至10.8%和5.4%。根据拉曼光谱分析结果推测,催化剂活性下降可能是因为催化剂表面形成了积炭。分析二元醇和芳香族单体的生成路径发现,Ni/Al_(2)O_(3)催化剂对活性中间体的稳定起到了重要作用。Biomass is one of the most potential alternatives of fossil fuel.The production of high value-added chemicals from biomass is an effective way to realize the diversified application of biomass.A hydrotalcite-derived Ni/Al_(2)O_(3) catalyst was prepared via urea precipitation and temperature-programmed reduction,which was analyzed with X-ray diffraction(XRD).The catalytic performance of Ni/Al_(2)O_(3) catalysts hydrocracking of corn stover was investigated in water-methanol mixed solvent.The results show that Ni/Al_(2)O_(3) catalyst exhibits good catalytic performance,and the corn stover conversion rate is up to 100%,and the diols yield is 38.8%,and the phenolic monomers yield is 13.6% under the optimum conditions(V(H_(2)O):V(CH_(3)OH)=7:3,240℃ and 3.0 MPa H_(2)).V(H_(2)O):V(CH_(3)OH)and temperature show notable impacts on corn stover conversion rate and small yields of molecule products.Ni/Al_(2)O_(3) catalyst and atmosphere influence small molecule products as well as products distribution.Cyclic test of the catalyst after one cycle reveals that the yields of diols and aromatic monomers decrease to 10.8% and 5.4%,respectively.Based on the results of Raman spectroscopy,it is speculated that the decrease in catalyst activity may be due to the formation of carbon deposits on the catalyst surface.Furthermore,it can be inferred that Ni/Al_(2)O_(3) catalyst shows crucial role in the stabilization of active intermediates by analyzing the generation pathways of diols and aromatic monomers.

关 键 词：玉米秸秆 加氢裂解 Ni/Al_(2)O_(3)催化剂 二元醇 芳香族单体 

分 类 号：TQ7[化学工程]