浸渍溶液对Ni/Al_2O_3催化剂CO甲烷化性能的影响
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摘要
通过浸渍法制备Ni/Al_2O_3催化剂,研究不同浸渍溶液(水、无水乙醇、N,N-二甲基甲酰胺)对催化剂的结构和甲烷化反应性能的影响。采用X射线衍射、氮气吸附脱附、紫外-可见光漫反射光谱、氢气程序升温还原、扫描电子显微镜等分析方法对催化剂的结构和形貌进行表征。结果表明,以DMF作为浸渍溶剂制备的催化剂(Ni/Al_2O_3-D)具有较小的镍颗粒尺寸和强的金属-载体作用力,在CO甲烷化反应中表现出更好的低温活性、高甲烷选择性和高温稳定性。
Ni/Al_2O_3 Catalyst was prepared by impregnation method with different solutions(water,ethanol,N,N-dimethylformamide),aiming at clarifying the effect of impregnation solution on the catalytic performances of Ni/Al_2O_3 for CO methanation.The catalysts were characterized by using X-ray diffraction,N_2-adsorption,UV visible diffuse reflectance spectra,hydrogen temperature programmed reduction and scanning electron.The results for methanation reaction indicated that the DMF impregnated NiO/Al_2O_3 possesses a better low temperature activity,high selectivity,and good stability,which is ascribed to the larger surface area,small nickel nanoparticle and strong interaction between Ni and Al_2O_3 in comparison with the catalysts impregnated with water and ethanol.
Ni/Al_2O_3 Catalyst was prepared by impregnation method with different solutions(water,ethanol,N,N-dimethylformamide),aiming at clarifying the effect of impregnation solution on the catalytic performances of Ni/Al_2O_3 for CO methanation.The catalysts were characterized by using X-ray diffraction,N_2-adsorption,UV visible diffuse reflectance spectra,hydrogen temperature programmed reduction and scanning electron.The results for methanation reaction indicated that the DMF impregnated NiO/Al_2O_3 possesses a better low temperature activity,high selectivity,and good stability,which is ascribed to the larger surface area,small nickel nanoparticle and strong interaction between Ni and Al_2O_3 in comparison with the catalysts impregnated with water and ethanol.
引文
[1] 李民瀚,孟凡会,李忠.溶胶凝胶法镍基催化剂的制备及其应用研究进展[J].天然气化工:C1化学与化工,2015,40(6):88-94.
[2] 林志峰,胡日茗,周晓龙.镍基催化剂的研究进展[J].化工学报,2017,68(s1):26-36.
[3] 路霞,陈世恒,王万丽,等.CO甲烷化Ni基催化剂的研究进展[J].石油化工,2010,39(3):340-345.
[4] 朱秋军.镍基催化剂上一氧化碳甲烷化反应性能研究[D].天津:天津大学化工学院,2012.
[5] 胡大成,高加俭,贾春苗,等.甲烷化催化剂及反应机理的研究进展[J].过程工程学报,2011,11(5):880-893.
[6] 刘超雷,李晨佳,史立杰,等.Ni基催化剂在CO-H2合成气反应体系中积炭研究进展[J].工业催化,2016,24(9):12-17.
[7] Zhen W L,Gao F,Tian B,et al.Enhancing activity for carbon dioxide methanation by encapsulating (111) facet Ni particle in metal-organic frameworks at low temperature[J].Journal of Catalysis,2017,348:200-211.
[8] Wang W X,Li X K,Zhang Y,et al.Strong metal-support interactions between Ni and ZnO particles and their effect on the methanation performance of Ni/ZnO[J].Catalysis Science & Technology,2017,7(19):4413-4421.
[9] 李翠平,赵瑞红,郭奋,等.不同负载方法制备镍金属有序介孔氧化铝催化剂的结构及性能[J].北京化工大学学报:自然科学版,2007,34(4):358-362.
[10] 祝新利.等离子体处理对甲烷转化催化剂的影响[D].天津:天津大学化工学院,2007.
[11] L P-F R,Jim N-G C,Rivas B D,et al.Partial oxidation of methane to syngas on bulk NiAl2O4 catalyst.Comparison with alumina supported nickel,platinum and rhodium catalysts[J].Applied Catalysis A General,2012,s 437/438(18):53-62.
[12] Kim P,Kim Y H,Kim H,et al.Synthesis and characterization of mesoporous alumina with nickel incorporated for use in the partial oxidation of methane into synthesis gas[J].Applied Catalysis A General,2004,272(1):157-166.
[13] Zhao A M,Ying W Y,Zhang H T,et al.Ni/Al2O3 catalysts prepared by solution combustion method for syngas methanation[J].Catalysis Communications,2012,17(1):34-38.
[14] 杨霞,郑文涛,汪国高,等.MgO对Ni/Al2O3催化剂CO甲烷化性能的影响[J].现代化工,2014,34(1):90-94.
[15] Leofanti G,Padovan M,Tozzola G,et al.Surface area and pore texture of catalysts[J].Catalysis Today,1998,90(4):207-219.
[16] Lakshmanan P,Min S K,Park E D.A highly loaded Ni@SiO2 core-shell catalyst for CO methanation[J].Applied Catalysis A General,2016,513:98-105.
[17] Li S,Tang H,Gong D,et al.Loading Ni/La2O3 on SiO2 for CO methanation from syngas[J].Catalysis Today,2017,297:298-307.
[18] Rostrup-Nielsen J R,Pedersen K.Sulfur poisoning of Boudouard and methanation reactions on nickel catalysts[J].Journal of Catalysis,1979,59(3):395-404.
[19] Chen D,Christensen K O,Ochoa-Fernández E,et al.Synthesis of carbon nanofibers:effects of Ni crystal size during methane decomposition[J].Journal of Catalysis,2005,229(1):82-96.
[20] Wang T,Ma H,Zeng L,et al.Highly loaded Ni-based catalysts for low temperature ethanol steam reforming[J].Nanoscale,2016,8(19):10177-10187.
[2] 林志峰,胡日茗,周晓龙.镍基催化剂的研究进展[J].化工学报,2017,68(s1):26-36.
[3] 路霞,陈世恒,王万丽,等.CO甲烷化Ni基催化剂的研究进展[J].石油化工,2010,39(3):340-345.
[4] 朱秋军.镍基催化剂上一氧化碳甲烷化反应性能研究[D].天津:天津大学化工学院,2012.
[5] 胡大成,高加俭,贾春苗,等.甲烷化催化剂及反应机理的研究进展[J].过程工程学报,2011,11(5):880-893.
[6] 刘超雷,李晨佳,史立杰,等.Ni基催化剂在CO-H2合成气反应体系中积炭研究进展[J].工业催化,2016,24(9):12-17.
[7] Zhen W L,Gao F,Tian B,et al.Enhancing activity for carbon dioxide methanation by encapsulating (111) facet Ni particle in metal-organic frameworks at low temperature[J].Journal of Catalysis,2017,348:200-211.
[8] Wang W X,Li X K,Zhang Y,et al.Strong metal-support interactions between Ni and ZnO particles and their effect on the methanation performance of Ni/ZnO[J].Catalysis Science & Technology,2017,7(19):4413-4421.
[9] 李翠平,赵瑞红,郭奋,等.不同负载方法制备镍金属有序介孔氧化铝催化剂的结构及性能[J].北京化工大学学报:自然科学版,2007,34(4):358-362.
[10] 祝新利.等离子体处理对甲烷转化催化剂的影响[D].天津:天津大学化工学院,2007.
[11] L P-F R,Jim N-G C,Rivas B D,et al.Partial oxidation of methane to syngas on bulk NiAl2O4 catalyst.Comparison with alumina supported nickel,platinum and rhodium catalysts[J].Applied Catalysis A General,2012,s 437/438(18):53-62.
[12] Kim P,Kim Y H,Kim H,et al.Synthesis and characterization of mesoporous alumina with nickel incorporated for use in the partial oxidation of methane into synthesis gas[J].Applied Catalysis A General,2004,272(1):157-166.
[13] Zhao A M,Ying W Y,Zhang H T,et al.Ni/Al2O3 catalysts prepared by solution combustion method for syngas methanation[J].Catalysis Communications,2012,17(1):34-38.
[14] 杨霞,郑文涛,汪国高,等.MgO对Ni/Al2O3催化剂CO甲烷化性能的影响[J].现代化工,2014,34(1):90-94.
[15] Leofanti G,Padovan M,Tozzola G,et al.Surface area and pore texture of catalysts[J].Catalysis Today,1998,90(4):207-219.
[16] Lakshmanan P,Min S K,Park E D.A highly loaded Ni@SiO2 core-shell catalyst for CO methanation[J].Applied Catalysis A General,2016,513:98-105.
[17] Li S,Tang H,Gong D,et al.Loading Ni/La2O3 on SiO2 for CO methanation from syngas[J].Catalysis Today,2017,297:298-307.
[18] Rostrup-Nielsen J R,Pedersen K.Sulfur poisoning of Boudouard and methanation reactions on nickel catalysts[J].Journal of Catalysis,1979,59(3):395-404.
[19] Chen D,Christensen K O,Ochoa-Fernández E,et al.Synthesis of carbon nanofibers:effects of Ni crystal size during methane decomposition[J].Journal of Catalysis,2005,229(1):82-96.
[20] Wang T,Ma H,Zeng L,et al.Highly loaded Ni-based catalysts for low temperature ethanol steam reforming[J].Nanoscale,2016,8(19):10177-10187.