载体制备方法对Ni/ZrO_2催化剂顺酐液相加氢性能的影响
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摘要
分别以水和甲醇为溶剂制备晶粒尺寸基本一致的四方相ZrO_2,通过浸渍法制备Ni质量分数10%的Ni/ZrO_2-W(水为溶剂)与Ni/ZrO_2-M(甲醇为溶剂)催化剂,考察其催化顺酐液相加氢性能。采用BET、XRD、H_2-TPR、H_2-TPD和in situ FT-IR对催化剂进行表征。结果表明,以甲醇为溶剂制备的ZrO_2比表面积明显小于以水为溶剂制备的ZrO_2,但Ni/ZrO_2-M催化剂存在强的金属-载体相互作用,其活性金属分散度以及C=O加氢活性明显高于Ni/ZrO_2-W催化剂。在反应温度210℃和氢压5 MPa条件下反应3 h,Ni/ZrO_2-M催化剂上顺酐转化率几乎100%,γ-丁内酯选择性为22.8%,Ni/ZrO_2-W催化剂上γ-丁内酯选择性仅为2.5%。
Two kinds of ZrO_2 with tetragonal phase and the same crystalline size were prepared by using water and methanol as the solvents respectively. Ni/ZrO_2 catalysts with Ni mass fraction of 10% were prepared by impregnation method and applied in the liquid phase hydrogenation of maleic anhydride. The asprepared catalysts were characterized by BET,XRD,H_2-TPR,H_2-TPD and in situ FT-IR. The results showed that although the specific surface area of ZrO_2 prepared by using methanol as the solvent was obviously smaller than that prepared by using water as the solvent,Ni/ZrO_2-M catalyst prepared by using methanol as the solvent had stronger metal-support interaction,higher active metal dispersion and higher CO hydrogenation activity than Ni/ZrO_2-W catalyst prepared by using water as the solvent. Under the condition of reaction temperature 210 ℃,hydrogen pressure 5 MPa and reaction time 3 h,the conversion of maleic anhydride on Ni/ZrO_2-M catalyst was 100% and the selectivity to γ-butyrolactone was 22. 8%,while the selectivity to γ-butyrolactone on Ni/ZrO_2-W catalyst was only 2. 5% under the same reaction condition.
Two kinds of ZrO_2 with tetragonal phase and the same crystalline size were prepared by using water and methanol as the solvents respectively. Ni/ZrO_2 catalysts with Ni mass fraction of 10% were prepared by impregnation method and applied in the liquid phase hydrogenation of maleic anhydride. The asprepared catalysts were characterized by BET,XRD,H_2-TPR,H_2-TPD and in situ FT-IR. The results showed that although the specific surface area of ZrO_2 prepared by using methanol as the solvent was obviously smaller than that prepared by using water as the solvent,Ni/ZrO_2-M catalyst prepared by using methanol as the solvent had stronger metal-support interaction,higher active metal dispersion and higher CO hydrogenation activity than Ni/ZrO_2-W catalyst prepared by using water as the solvent. Under the condition of reaction temperature 210 ℃,hydrogen pressure 5 MPa and reaction time 3 h,the conversion of maleic anhydride on Ni/ZrO_2-M catalyst was 100% and the selectivity to γ-butyrolactone was 22. 8%,while the selectivity to γ-butyrolactone on Ni/ZrO_2-W catalyst was only 2. 5% under the same reaction condition.
引文
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[26]杨秋芸,朱渊,田莉,等.Au/Ti O2催化剂制备条件对巴豆醛选择加氢的影响[J].物理化学学报,2009,25(9):1853-1860.Yang Qiuyun,Zhu Yuan,Tian Li,et al.Influence of Au/Ti O2catalyst preparation parameters on the selective hydrogenation of crotonaldehyde[J].Acta Physico-Chimica Sinica,2009,25(9):1853-1860.
[27]Hao Cai-Hong,Guo Xiao-Ning,Pan Yung-Tin,et al.Visible-Light-Driven selective photocatalytic hydrogenation of cinnamaldehyde over Au/Si C catalysts[J].Journal of the American Chemical Society,2016,138(30):9361-9364.
[28]Regenhardt S A,Meyer C I,Garetto T F,et al.Selective gas phase hydrogenation of maleic anhydride over Ni-supported catalysts:effect of support on the catalytic performance[J].Applied Catalysis A:General,2012,449(1):81-87.
[29]Gao C,Zhao Y,Zhang,et al.Synthesis characterization and catalytic evaluation of Ni/Zr O2-Si O2aerogels catalysts[J].Journal of Sol-Gel Science and Technology,2007,44(2):145-151.
[30]Mercy C I,Regenhardt S A,Marchi A J.Gas phase hydrogenation of maleic anhydride at low pressure over silicasupported cobalt and nickel catalysts[J].Applied Catalysis A:General,2012,417-418(6):59-65.
[2]Liu Yachun,Fang Kegong,Chena Jiangang,et al.Effect of pore size on the performance of mesoporous zirconia-supported cobalt Fischer-Tropsch catalysts[J].Green Chemistry,2007,9(6):611-615.
[3]Li Shuirong,Zhang Chengxi,Zhang Peng,et al.On the origin of reactivity of steam reforming of ethylene glycol on supported Ni catalysts[J].The Journal of Physical Chemistry,2012,14(12):4066-4069.
[4]Sharma,Anil Kumar.Zirconia-supported copper oxide——A catalyst for removal of vehicular exhaust gas pollutants[J].Environmental Engineering Science,2006,132(8):956-959.
[5]张鑫,徐柏庆.Au/Zr O2催化CO氧化反应中Zr O2纳米粒子的尺寸效应化学学报[J].化学学报,2005,63(1):86-90.Zhang Xin,Xu Boqing.Nano-size effect of zirconia in Au/Zr O2catalyst for CO oxidation[J].Acta Chimica Sinica,2005,63(1):86-90.
[6]孙翠枝,周仁贤.乙醇/水溶剂体系中Pt-Co/Zr O2催化剂上肉桂醛的选择性加氢性能[J].高等学校化学学报,2011,32(7):1551-1555.Sun Cuizhi,Zhou Renxian.Selective hydrogenation of cinnamaldehyde over Pt-Co/Zr O2catalyst in the solvent system of ethanol/water[J].Chemical Journal of Chinese Universities,2011,32(7):1551-1555.
[7]Grabosaki R,Sloczyński J,Sliwa M,et al.Influence of polymorphic Zr O2phases and the silver electronic state on the activity of Ag/Zr O2catalyst in the hydrogenation of CO2to methanol[J].ACS Catalysis,2011,1(4):266-278.
[8]Michiaki Yamasaki,Hiroki Habazaki,Katsuhiko Asami,et al.Effect of tetragonal Zr O2on the catalytic activity of Ni/Zr O2catalyst prepared from amorphous Ni-Zr alloys[J].Catalysis Communications,2006,7(1):24-28.
[9]张颜鑫.Zr O2晶型对Ni/Zr O2催化剂顺酐液相加氢性能[D].太原:山西大学,2013.Zhang Yanxin.Effect of Zr O2polymorphs on catalytic performance of Ni/Zr O2catalyst for liquid phase hydrogenation of maleic anhydride[D].Taiyuan:Shanxi University,2013.
[10]Zhang Xin,Wang Hai,Xu Boqing.Remarkable nanosize effect of zirconia in Au/Zr O2catalyst for CO oxidation[J].The Journal of Physical Chemistry B,2005,109(19):9678-9683.
[11]Li Shuirong,Zhang Chengxi,Huang Zhiqi,et al.A Ni@Zr O2nanocomposite for ethanol steam reforming:enhanced stability via strong etal-oxide interaction[J].Chemical Communications,2013,49(39):4226-4228.
[12]张胜红,张鸿鹏,李为臻,等.Zr O2晶相对Mo Ox/Zr O2催化剂结构及其甲醇选择性氧化性能的影响[J].物理化学学报,2010,26(7):1879-1886.Zhang Shenghong,Zhang Hongpeng,Li Weizhen,et al.Effects of zirconia crystallite phases on the structures of Mo Ox/Zr O2catalysts and their properties in the selective oxidation of methanol[J].Acta Physico-Chimica Sinica,2010,26(7):1879-1886.
[13]Min Chen,Zhang Long-guo,Jian Zheng,et al.CO2selective hydrogenation to syntheic natural gas(SNG)over pour nano-sized Ni/Zr O2samples:Zr O2crystalline phase&treatment impact[J].Journal of Energy Chemistry,2016,25(6):1070-1077.
[14]李为臻,刘海超.溶剂热法合成纯单斜和四方晶相氧化锆中的溶剂效应[J].物理化学学报,2008,24(12):2172-2178.Li Weizhen,Liu Haichao.Solvent effects on the solvothermal of pure monoclinic and tetragonal zirconia nanoparticles[J].Acta Physico-Chimica Sinica,2008,24(12):2172-2178.
[15]Zhang X P,Zhang Q,Tsubaki N S.Carbon dioxide reforming of methane over Ni nanoparticles incorporated into mesoporous amorphous Zr O2matrix[J].Fuel,2015,147:243-252.
[16]Parastoo Delir Kheyrollahi Nezhad,Mohammad Haghighi,Naimeh Jodeiri,et al.Sol-gel preparation of Ni O/Zr O2(x)-Mg O(100-x)nanocatalyst used in CO2/O2oxidative dehydrogenation of ethane to ethylene:influence of Mg/Zr ratio on catalytic performance[J].Journal of Sol-Gel Science and Technology,2016,80(2):436-450.
[17]Kresimir Anicl,Astrid Wolfbeisserl,Hao Li,et al.Surface spectroscopy on UHV-Grown and technological Ni-Zr O2reforming catalysts:from UHV to operando conditions[J].Topics in Catalysis,2016,59(17/18):1614-1627.
[18]张因,赵丽丽,张鸿喜,等.载体对镍基催化剂顺酐液相加氢性能的影响[J].化工学报,2015,66(7):2505-2513.Zhang Yin,Zhao Lili,Zhang Hongxi,et al.Effect of support on catalytic performance of nickel-based catalysts used for liquid phase hydrogenation of maleic anhydride[J].CIESC Journal,2015,66(7):2505-2513.
[19]Jasik A,Wojcieszak R.Study of nickel catalysts supported on Al2O3,Si O2or Nb2O5oxides[J].Journal of Molecular Catalysis A:Chemical,2005,242(1/2):81-90.
[20]Wu W H,Xu J,Ohnishi R.Complete hydrode chlorination of chlorobenzene and its derivatives over supported nickel catalysts under liquid phase conditions[J].Applied Catalysis B:Environmental,2005,60:129-137.
[21]Naeem M A,Al-Fatesh A S,Abasaeed A E,et al.Activities of Ni-based nano catalysts for CO2-CH4reforming prepared by polyol process[J].Fuel Process Technol,2014,122(6):141-152.
[22]杨燕萍,张因,高春光,等.Ti Ox(x<2)表面修饰Ni/Ti O2-Si O2催化顺酐液相选择加氢合成γ-丁内酯[J].催化学报,2011,32(11):1768-1774.Yang Yanping,Zhang Yin,Gao Chunguang,et al.Selective hydrogenation of maleic anhydridetoγ-butyrolactoneover Ti Ox(x<2)surface-modified Ni/Ti O2-Si O2in liquid phase[J].Chinese Journal of Catalysis,2011,32(11):1768-1774.
[23]Yao Na,Chen Jixiang,Zhang Jianxiang,et al.Influence of support calcination temperature on properties of Ni/Ti O2for catalytic hydrogenation of o-chloronitrobenzene to o-chloroaniline[J].Catalysis Communications,2008,9(6):1510-1516.
[24]Haruta M,Tsubota S.Low-temperature oxidation of carbon monoxide over gold supported on titanium dioxideα-ferricoxide and cobal ttetraoxide[J].Journal of Catalysis,1993,144(1):175-192.
[25]Kung H,Kung M C,Costello C K.Supported Au catalysts for low temperature CO oxidation[J].Journal of Catalysis,2003,216(1/2):425-443.
[26]杨秋芸,朱渊,田莉,等.Au/Ti O2催化剂制备条件对巴豆醛选择加氢的影响[J].物理化学学报,2009,25(9):1853-1860.Yang Qiuyun,Zhu Yuan,Tian Li,et al.Influence of Au/Ti O2catalyst preparation parameters on the selective hydrogenation of crotonaldehyde[J].Acta Physico-Chimica Sinica,2009,25(9):1853-1860.
[27]Hao Cai-Hong,Guo Xiao-Ning,Pan Yung-Tin,et al.Visible-Light-Driven selective photocatalytic hydrogenation of cinnamaldehyde over Au/Si C catalysts[J].Journal of the American Chemical Society,2016,138(30):9361-9364.
[28]Regenhardt S A,Meyer C I,Garetto T F,et al.Selective gas phase hydrogenation of maleic anhydride over Ni-supported catalysts:effect of support on the catalytic performance[J].Applied Catalysis A:General,2012,449(1):81-87.
[29]Gao C,Zhao Y,Zhang,et al.Synthesis characterization and catalytic evaluation of Ni/Zr O2-Si O2aerogels catalysts[J].Journal of Sol-Gel Science and Technology,2007,44(2):145-151.
[30]Mercy C I,Regenhardt S A,Marchi A J.Gas phase hydrogenation of maleic anhydride at low pressure over silicasupported cobalt and nickel catalysts[J].Applied Catalysis A:General,2012,417-418(6):59-65.