甲烷部分氧化制合成气La-Ni-O系催化剂性能的研究
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摘要
甲烷催化部分氧化具有能耗低、反应速率比水蒸气重整快几个数量级、生成的合成气中H2/CO比适合作甲醇及F-T合成等优点,因此近几十年一直为众多研究者所关注。镍基催化剂由于活性高和成本低而被认为是最有应用前景的催化剂之一,但由于其反应的稳定性差仍不能满足实际要求,因此探索如何提高催化剂稳定性是目前研究工作的重要内容。
本文以BET、XRD、TPR、TG/DTA、SEM、XPS、反应活性评价等多种研究方法,重点考察了NiO/La_2O_3、LaNiO_3、La_2NiO_4催化剂的制备条件对其物化性质和甲烷部分氧化性能的影响,对LaNiO_3、La_2NiO_4物化性质和甲烷部分氧化性能进行了较为系统的比较,探讨了影响催化剂积碳和稳定性的因素。
NiO/La_2O_3的研究结果表明,采用浸渍法制备的NiO/La_2O_3催化剂在经过高温焙烧后会形成LaNiO_3和La_2NiO_4;Ni含量为20～30%的催化剂具有相对较好的结构特征和催化活性;反应过程中生成的La_2O_2CO_3是有利于反应进行的物种,它能消除以金属碳化物形式存在的积碳,表现出良好的抗积碳性能。
采用溶胶-凝胶法制备了钙钛矿型复合氧化物LaNiO_3。结果表明:制备过程中柠檬酸用量对催化剂的形貌及其甲烷部分氧化催化活性有很大的影响。当柠檬酸用量为La:Ni:CA=1:1:3时所制备的催化剂具有良好的结构形貌和催化活性。
对于类钙钛矿复合氧化物La_2NiO_4,同样采用了溶胶-凝胶法制备。结果表明:当焙烧温度为850℃,柠檬酸用量为La:Ni:CA=2:1:3时,可以形成完整的、颗粒均匀的类钙钛矿型La_2NiO_4,而且甲烷部分氧化活性也良好。在500℃下用H2预还原处理后的催化剂活性明显高于未进行还原处理的催化剂。
在甲烷部分氧化反应中,还原态Ni0是该催化反应的活性中心,La_2NiO_4上活性组分Ni0晶粒比LaNiO_3上的Ni0晶粒小,而且分散度要高,这也是La_2NiO_4甲烷部分氧化活性和稳定性比LaNiO_3好的主要原因。
在甲烷部分氧化反应过程中,La_2NiO_4和LaNiO_3上都有积碳产生;La_2NiO_4产生的积碳主要以金属碳化物形式存在,而LaNiO_3产生的积碳以石墨碳为主;金属碳化物可以被反应过程中形成的La_2O2CO_3消除掉,而石墨碳活性低,不易被除去,这也是La_2NiO_4稳定性好而LaNiO_3稳定性差的原因。
Partial oxidation of methane (POM) to syngas has attracted both academic and industrial interest. Compared with steam reforming, POM is more energy efficient and can be carried out with a much lower investment of capital. POM produces syngas with a H_2/CO ratio of ca. 2, which is suitable for use in the production of methanol and Fisher-Tropsch synthesis. Nickel-based catalysts are promising for its industrialization because of their high activity and relatively low cost. However, their application is limited due to their easy deactivation under reaction condition. Thus, it is important to develop the useful POM catalysts with ideal stability.
In this work, the effects of different preparation condition on the structure and POM reactivity of NiO/La_2O_3, LaNiO_3 and La_2NiO_4 were examined. The structure and POM reactivity of LaNiO_3 and La_2NiO_4 were compared systemtically.
NiO/La_2O_3 was prepared by wet impregnation method. The research on NiO/La_2O_3 showed that the provskite structure of LaNiO_3 can be formed after calcinations at high temperature, the NiO/La_2O_3 contained 20～30wt.% nickel exhibited good activity for partial oxidation of methane, La_2O_2CO_3 formed during reaction is probably species, which may favor removal of carbon deposition existed in MxC.
LaNiO_3 and La_2NiO_4 were successfully prepared by a sol-gel method and used in partial oxidation of methane. The results showed that the amount of citric acid and calcination temperature have significant influence on the characteristics of the catalysts and their catalytic activity. The catalyst reduced in H2 at 500℃showed better POM performance.
Ni0 is active site of the POM reaction, perovskite-like oxide La_2NiO_4 presents smaller nickel particle NiO after reduction treatment. Consequently the catalytic activity is higher than perovskite oxide LaNiO_3.
The carbon deposition had formed on catalysts LaNiO_3 and La_2NiO_4 in POM reaction. Most of the carbon deposited on La_2NiO_4 was MxC, which can be removed by La_2O_2CO_3, while one on LaNiO_3 was graphite which is low active. So the stability of perovskite-like oxide La_2NiO_4 is better than perovskite oxide LaNiO_3.
本文以BET、XRD、TPR、TG/DTA、SEM、XPS、反应活性评价等多种研究方法,重点考察了NiO/La_2O_3、LaNiO_3、La_2NiO_4催化剂的制备条件对其物化性质和甲烷部分氧化性能的影响,对LaNiO_3、La_2NiO_4物化性质和甲烷部分氧化性能进行了较为系统的比较,探讨了影响催化剂积碳和稳定性的因素。
NiO/La_2O_3的研究结果表明,采用浸渍法制备的NiO/La_2O_3催化剂在经过高温焙烧后会形成LaNiO_3和La_2NiO_4;Ni含量为20～30%的催化剂具有相对较好的结构特征和催化活性;反应过程中生成的La_2O_2CO_3是有利于反应进行的物种,它能消除以金属碳化物形式存在的积碳,表现出良好的抗积碳性能。
采用溶胶-凝胶法制备了钙钛矿型复合氧化物LaNiO_3。结果表明:制备过程中柠檬酸用量对催化剂的形貌及其甲烷部分氧化催化活性有很大的影响。当柠檬酸用量为La:Ni:CA=1:1:3时所制备的催化剂具有良好的结构形貌和催化活性。
对于类钙钛矿复合氧化物La_2NiO_4,同样采用了溶胶-凝胶法制备。结果表明:当焙烧温度为850℃,柠檬酸用量为La:Ni:CA=2:1:3时,可以形成完整的、颗粒均匀的类钙钛矿型La_2NiO_4,而且甲烷部分氧化活性也良好。在500℃下用H2预还原处理后的催化剂活性明显高于未进行还原处理的催化剂。
在甲烷部分氧化反应中,还原态Ni0是该催化反应的活性中心,La_2NiO_4上活性组分Ni0晶粒比LaNiO_3上的Ni0晶粒小,而且分散度要高,这也是La_2NiO_4甲烷部分氧化活性和稳定性比LaNiO_3好的主要原因。
在甲烷部分氧化反应过程中,La_2NiO_4和LaNiO_3上都有积碳产生;La_2NiO_4产生的积碳主要以金属碳化物形式存在,而LaNiO_3产生的积碳以石墨碳为主;金属碳化物可以被反应过程中形成的La_2O2CO_3消除掉,而石墨碳活性低,不易被除去,这也是La_2NiO_4稳定性好而LaNiO_3稳定性差的原因。
Partial oxidation of methane (POM) to syngas has attracted both academic and industrial interest. Compared with steam reforming, POM is more energy efficient and can be carried out with a much lower investment of capital. POM produces syngas with a H_2/CO ratio of ca. 2, which is suitable for use in the production of methanol and Fisher-Tropsch synthesis. Nickel-based catalysts are promising for its industrialization because of their high activity and relatively low cost. However, their application is limited due to their easy deactivation under reaction condition. Thus, it is important to develop the useful POM catalysts with ideal stability.
In this work, the effects of different preparation condition on the structure and POM reactivity of NiO/La_2O_3, LaNiO_3 and La_2NiO_4 were examined. The structure and POM reactivity of LaNiO_3 and La_2NiO_4 were compared systemtically.
NiO/La_2O_3 was prepared by wet impregnation method. The research on NiO/La_2O_3 showed that the provskite structure of LaNiO_3 can be formed after calcinations at high temperature, the NiO/La_2O_3 contained 20～30wt.% nickel exhibited good activity for partial oxidation of methane, La_2O_2CO_3 formed during reaction is probably species, which may favor removal of carbon deposition existed in MxC.
LaNiO_3 and La_2NiO_4 were successfully prepared by a sol-gel method and used in partial oxidation of methane. The results showed that the amount of citric acid and calcination temperature have significant influence on the characteristics of the catalysts and their catalytic activity. The catalyst reduced in H2 at 500℃showed better POM performance.
Ni0 is active site of the POM reaction, perovskite-like oxide La_2NiO_4 presents smaller nickel particle NiO after reduction treatment. Consequently the catalytic activity is higher than perovskite oxide LaNiO_3.
The carbon deposition had formed on catalysts LaNiO_3 and La_2NiO_4 in POM reaction. Most of the carbon deposited on La_2NiO_4 was MxC, which can be removed by La_2O_2CO_3, while one on LaNiO_3 was graphite which is low active. So the stability of perovskite-like oxide La_2NiO_4 is better than perovskite oxide LaNiO_3.
引文
[1] Ohno Y, Shikada T, Ogawa T, et al. 213# ACS Meeting, San Francisco,USA, 1997, 705
[2] Tindall B M, King D. Hydrocarbon Processing, July, 1994
[3] 陆世雄译,C1化学-创造未来的化学,日本化学会编,1990
[4] Bharadwaj S S, Schmidt L D. Catalytic partial oxidation of natural gas to syngas. Fuel Processing Technology, 1995, 42: 109~127
[5] Tsang S C, Claridge J B, Green M L H. Recent advances in the conversion syngas. Fuel Processing Technology, 1995, 42: 109~127
[6] Farina G L, Supp E. Produce syngas for methanol. Hydrogen Processing, Mar. 1992, 71(3): 77
[7] Prettre M, Ichner C E. Trans. Faraday Soc., 1946, 43:335
[8] Dissanayake D, Rosynek M P. Partial oxidation of methane to carbon monoxide and hygrogen over a Ni/Al2O3. J. Catal.,1991, 132:117～127
[9] Choudhary V R, Rane V H, Rajput A M. Selective oxidation of methane to CO and H2 over unreduced NiO-rare earth oxide catalysts. Catal. Lett.,1993, 22( 4): 289~297
[10] Slagtern A, Swaan H M, Olsbye U. Catalytic partial oxidation of methane over Ni-, Co- and Fe- based catalysts. Catal. Today, 1998, 46:107～115
[11] Takeguchi T, Furukawa S N. Autothermal reforming of methane over Ni catalysts supported over CaO-CeO2-ZrO2 solid solution. Appl. Catal. A: General, 2003, 240: 223~233
[12] Nishimoto H, Nakagawa K, Suzuki T, et al. Partial oxidation of methane to synthesis gas over oxidized diamond catalysts. Appl. Catal. A: General, 2004, 264: 65～72
[13] Barbero J, Pen M A, Campos-Martin J M, et al. Support effect in supported Ni catalysts on their performance for methane partial oxidation. Catal. Lett. 2003, 87 (3~4): 211~218
[14] Sittiphong, Pengpanich, Vissanu, et al. Methane partial oxidation over Ni/CeO2-ZrO2 mixed oxide solid solution catalysts. Catal. Today, 2004, 93: 95~105
[15] 曹立新,李燕馨,李文钊,Ni 系列催化剂上甲烷直接氧化制合成气,分子催化,1994,8(5):375～382
[16] Hayakawa T, Anderson A G, Shimizu M, et al. Partial oxidation of methane to synthesis gas over some titanates based perovskite oxides. Catal. Lett. 1993, 22: 307~317
[17] Provendier H, Petita C, Stabilization of active nickel catalyts in partial oxidation of methane to synthesis gas by iron addition. Appl. Catal. A: General, 1999, 180: 163~173
[18] Alptekin G O, Herring A M, Williamson D L, et al. Methane partial oxidation by unsupported and silica supported iron phosphate catalysts: influence of reaction conditions and Co-feeding of water on activity and selectivity. J. Catal., 1999, 181: 104~112
[19] Vermeiren W J M, Blomsma E, Jacobs P A. Catalytic and thermodynamic approach of the oxyreforming reaction of methane. Catal. Today, 1992, 13: 427～436
[20] Utaka T, Abdulaziz A D S. Partial oxidation of methane over Ni catalysts based on hexaaluminate or perovskite type oxides. Appl. Catal., A: General, 2003, 247(1): 125~131
[21] 张兆斌,余长春,甲烷部分氧化制合成气的 La2O3 助 Ni/MgA12O4 催化剂,催化学报,2000,21(1):14-18
[22] Ruckenstein E, Hu Y H. Methane partial oxidation over NiO/MgO solid solution catalysts. Appl. Catal. A: Gen, 1999, 183: 85~92
[23] Vernon P D F, Green M L H, Cheetham A K. Partial oxidation of methane to synthesis gas. Catal. Lett., 1990, 6: 181~186
[24] Torniainen P M, Chu X, Schmidt L D. Comparison of monolith-supported metals for the direct oxidation of methane to syngas. J. Catal., 1994, 146: 1~10
[25] Kunimori K, Umeda S. Partial oxidation to synthesis gas over rhodium vanadate RhVO4: redispersion of Rh metal during the reaction. Chem. Soc. Jpn., 1992, 65: 2526~2564
[26] Bhattacharya A K, Breach J A, Chand S, et al. Selective oxidation of methane to carbon monoxide on supported palladium catalyst. Appl. Catal. A: General, 1992, 80(1): 1~5
[27] Mataumura Y, Moffat J B. Partial oxidation of methane to carbon-monoxide and hydrogen with molecular-oxygen and nitrous-oxide over hydroxyapatite catalysts. J. catal. 1994, 148:323～333
[28] Claridge J B, York A P E, Brungs A J, et al. New catalysts for the conversion of methane to synthesis gas:molybdenum and tungsten carbide. J. Catal., 1998, 180: 85～100
[29] Hickman D A, Schmidt L D. Synthesis gas formation by direct oxidation of methane over Pt monoliths. J. Catal., 1992, 138: 267~282
[30] 沈师孔,李春义,余长春,Ni/Al2O3 催化剂上甲烷部分氧化制合成气反应机理,催化学报,1998,19(4):309～314
[31] Au C T, Wang Y H, Wan H L. Mechanistic Studies of CH4/O2 Conversion over SiO2-Supported Nickel and Copper Catalysts. J. Catal., 1996, 158: 343~348
[32] Lu Y, Xue J Z, Yu C C, et al. Mechanistic investigations on the partial oxidation of methane to synthesis gas over a nickel-on-alumina catalyst. Appl. Catal. A: Gen., 1998, 174: 121~128
[33] Ji Y Y, Li W Z, Xu H Y, et al. Partial oxidation of methane to syngas in fluidized bed reactor. Chinese J. Catal., 2000, 21(2): 97～98
[34] Claridge J B, Green M H L, Tsang S C, et al. A study of carbon deposition on catalysts during the partial oxidation of methane to synthesis gas. Catal. Lett., 1993, 22: 299~305
[35] Rostrup-Nielsen J R. Coking on nickel catalysts for steam reforming of hydrogen. J. Catal., 1974, 33:184～201
[36] 徐恒泳,孙希贤,范业梅等,甲烷、二氧化碳转化制合成气的研究,石油化工,1992,21(3):147~153
[37] 李春义,余长春,沈师孔,Ni /Al2O3 催化剂上 CH4 部分氧化制合成气反应积碳的原因,催化学报,2001,22(4):377~382
[38] 曹立新,陈燕馨,李文钊,载体对甲烷直接氧化制合成气的影响,天然气化工,1996,21(3):3~15
[39] Tsipouriari V A, Verykios X E. Catalytic partial oxidation of methane to synthesis gas over Ni-based catalysts: II. transient, FTIR, and XRD measurements. J. Catal., 1998, 179: 292～299
[40] 金荣超,陈燕馨,李文剑,甲烷催化部分氧化 Ni 催化剂及 Ce 的研究,物理化学学报,1998, 14(8):737~741
[41] 路勇,余长春,沈师孔等,负载型镍金属催化剂上甲烷与二氧化碳重整制合成气,催化学报,1996, 17(3):212~216
[42] Takashi Hayakawa, Hideaki Harihara, Ahdrew P E York, et al. A Sustainable catalyst for the partial oxidation of methane to syngas: Ni / Ca l-xSrxTiO3prepared in situ from perovskite precursors. Angew. Chem. Int. Ed. Engl., 1996, 35(2):192~
[43] Torniainen P, Chu X, Schmidt L D. Comparison of monolith- supported metal for the direct oxidation of methane to syngas, J. Catal., 1994, 146:1~10
[44] Honig R E, Kramer D A, RCA Rec., 1969,30:285
[45] Lu Y, Shen S K. Design of stable Ni catalysts for partial oxidation of methane to synthesis gas. J. Catal., 1998, 177:386~388
[46] Liu S L, Xiong G X. The effect of Li and La on NiO/Al2O3 catalyst for CH4/O2 to syngas reaction. React. Kinet. Catal. Lett., 1999, 68(2):243~247
[47] Rao C N R, Ganguly P. A comparative study of the magnetic and electrical properties of perovskite oxide and the corresponding two-dimensional oxides of K2NiF4 structure. Singh K K, Ram R A M. J. solid state chem. 1988, 72:14
[48] Odier P, Leblanc M, Choisnet J. Structural characterization of an orthorhombic form of La2NiO4. Mater. Res. Bull, 1986, 21(7):787~796
[49] 何俊,孙颖稼等,A2BO4 型催化活性材料结构与性能的研究,分子催化,1994,8(5):325~329
[50] Weng D, Zhao H S, Wu X D, et al. Influence of cerium on the performance of LaMO3(M=Mn or Mn-Cu) perovskite-type catalyst. Mater. Sci. Eng. A, 2003, 361:173~178
[51] Libby W R. Promising catalyst for auto exhaust. Science,1971,171:499~500
[52] Gunasekaran N, Rajadurai S, Carberry J. Catalytic decomposition of nitrous oxide over perovskite type solid oxide solutions and supported noble metal catalysts. Catal. Lett., 1995, 35(3,4):373
[53] Nakamura T, Misono M, Yoneda Y. Reduction-oxidation and catalytic properties of perovskite-type mixed oxide catalysts lanthanum strontium cobalt oxide ( La1-xSrxCoO3). Chem. Lett., 1981, (11):1589
[54] Gao L Z, Au C T. Studies on the decomposition of N2O over Nd2CuO4,Nd1.6Ba0.4CuO4 and Nd1.8Ce0.2CuO4. J. Mol. Catal. A, 2001, 168(2):173~186
[55] Arai H, Yamada T, Eguchi K, et al. Catalytic combustion of methane over various perovskite-type oxides. Appl. Catal., 1986, 26(1-2):265
[56] Pena M A, Fierro J L G. Chemical structures and performance of perovskite oxides. Chem. Rev., 2001, 101(7):1981~2018
[57] 杨秋华,傅希贤,纳米 LaMO3(M = Cr, Mn, Fe, Co)化合物的光催化氧化活性分析,硅酸盐学报,2003, 31(3):254~256
[58] 傅希贤,桑丽霞,钙钛矿型(ABO3)化合物的光催化活性及其影响因素,天津大学学报,2001,34(2):229~231
[59] Wang D F, Zhou Z G.A new spinel type photocatalysts BaCr2O4 for H2 evolution under UV and Visible Light irradiation.Chem.Phys.Lett., 2003, (373):191~196
[60] 冉锐,吴晓东,翁端,稀土钙钛矿催化剂制备方法研究进展,稀土,2004,25(5):46～50
[61] 徐科,严洁,钙钛矿型稀土纳米复合氧化物制备及应用研究进展,贵州大学学报(自然科学版),2003,20(4):421～425
[62] 刘源,钙钛矿型 LaCoO3 和 LaMnO3 超细粒子的制备,内蒙古工业大学学报,2000,19(3):192~196
[63] 翟永青,姚子华,EDTA 络合溶胶-凝胶法制备 La0.8Sr0.2FeO3 纳米粉体,稀有金属,2002,26(1):69~72
[64] Ciambelli P, Cimino S, Lisi L. La, Ca and Fe oxide perovskites: preparation, characterization and catalytic properties for methane combustion. Appl. Catal. B: environmental, 2001, 33: 193~203
[65] 张翔宇,李振花,甲烷部分氧化制合成气催化剂的研究进展,化工进展,2002,21(12):903~907
[66] 张恒,董新法,林维明,Ni 基催化剂上甲烷部分氧化制合成气,天然气化工,2004,19(3):36~42
[67] Zhang Z, Verykios X E. Carbon dioxide reforming of methane to synthesis gas over Ni/La2O3 catalysts. Appl. Catal. A: General, 1996, 138: 109~133
[68] Tsipouriari V A, Verykios X E. Carbon and oxygen reaction pathways of CO2 reforming of methane over Ni/La2O3 and Ni/Al2O3 catalysts studied by isotopic tracing Techniques. J. Catal., 1999, 187: 85~94
[69] Tsipouriari V A, Verykios X E. Kinetic study of the catalytic reforming of methane with carbon dioxide to synthesis gas over Ni/La2O3 catalyst. Catal. Today, 2001, 64: 83~90
[70] Tsipouriari V A, Zhang Z, Verykios X E. Catalytic partial oxidation of methane to synthesis gas over Ni-based catalysts. J. Catal., 1998, 179: 283~291
[71] 刘盛林,熊国兴,缪清等,锂和镧的添加对 NiO/Al2O3 甲烷部分氧化积碳的影响,天然气化工,1998,23(5):5~7
[72] 王爱菊,CH4 部分氧化制氢复合氧化物负载 Ni-Cu 催化剂制备及反应性能研究,[博士学位论文],天津,天津大学,2003
[73] Ruckenstein E, Hu Y H. Interactions between Ni and La2O3 in Ni/La2O3 catalystsprepared using different Ni precursors. J. Catal., 1996, 161: 55~61
[74] Barbero J, Pena M A, Campos-Martin J M, et al. Support effect in supported Ni catalysts on their performance for methane partial oxidation. Catal. Lett., 2003, 87: 211~218
[75] Slagtern A, Schuurman Y, Leclercq C, et al., Specific features concerning the mechanism of methane reforming by carbon dioxide over Ni/La2O3 catalysts. J. Catal. 1997, 172: 118~126
[76] 李文英,冯杰,谢克昌等,CH4-CO2 重整反应镍基催化剂的积碳性能的研究.燃料化学学报,1997,25(5):460~464
[77] 陈吉祥,王日杰,李玉敏等,镍基气凝胶催化 CH4-CO2 重整制取合成气反应的研究,燃料化学学报,2002,30(5):445~453
[78] 田辉平,钙钛矿型稀土复合氧化物的深度氧化性能研究,[博士学位论文],天津,天津大学,1992
[79] 陈铜,于作龙,远松月等,Bi-Mo-Nb 复合氧化物的结构与对丙烯氧化的催化活性,化学学报,1994(6):521～528
[80] Garin F, Simonot L, Maire G. A comparative study of LaCoO3, Co3O4 and a mix of LaCoO3-Co3O4 Ⅱ Catalytic properties for the CO + NO reaction. Appl. Catal. B: Environment, 1997, 11: 181~191
[81] Provendier H, Petit C, Estournes C, et al. Stabilisation of active nickel catalysts in partial oxidation of methane to synthesis gas by iron addition, Appl. Catal. A: General, 1999, 180: 163~173
[82] Takehira K, Shishido T, Kondo M. Partial oxidation of CH4 over Ni/SrTiO3 catalysts prepared by a solid-phase crystallization method. J. Catal. 2002, 207:307~316
[83] Guo C L, Zhang J L, Li W, et al. Partial oxidation of methane to syngas over BaTi1-xNixO3 catalysts. Catal. Today, 2004, 98:583~587
[84] Liu S, Tan X Y, Li K. Synthesis of strontium cerates-based perovskite ceramics via water-soluble complex precursor routes. Ceramics international, 2002, 28:327~335
[85] 侯峰,La-Ni-O 系薄膜复合材料氧敏性能的研究,[博士学位论文],天津,天津大学,2001
[86] Wang H, Zhu Y, Liu Y. Preparation of nanosized perovskite LaNiO3 powder via amorphous heteronuclear complex precursor. J. Mater. Sci., 2003, 38: 1939-1943
[87] 高利珍,于作龙,吴越,在镍系钙钛矿(ABO3)型催化剂上的氨氧化 Ⅲ.焙烧温度对催化剂结构和活性的影响,1992,9(2):21~25
[88] Fernandes J D G, Melo D M A, Zinner L B, et al. Low-temperature synthesis of single phase crystallize LaNiO3 perovskite via Pechini method. Mater. Lett., 2002, 53: 122~125
[89] Handbook of X-ray Photoelectron Spectroscopy, Moulder J F, Stickle W F, Sobol P E, Bomben K D. Published by Perkin-Elmer Corperation, United States of America
[90] Liu B S, Au C T. Sol-gel generated La2NiO4 for CH4/CO2 reforming. Catal. lett., 2003, 85(3-4):165~170
[91] Liu B S, Au C T. Carbon deposition and catalyst stability over La2NiO4/ γ ?Al2O3 during CO2 reforming of methane to syngas. Appl. Catal. A: General, 2003, 244: 181~195
[92] Zhang W D, Liu B S, Zhu C, et al. Preparation of La2NiO4 /ZSM-5 catalyst and catalytic performance in CO2/CH4 reforming to syngas. Appl. Catal. A: General, 2005, 292: 138~143
[93] 池玉娟,于海涛,李环宇,钙钛矿型复合氧化物 La1-xSrxFeO3 纳米晶制备研究,黑龙江大学自然科学学报,2000,17(1):73~78
[94] 娄向东,田圣军,姜聚慧,含镧钙钛矿型复合氧化物的制备方法评价,郑州轻工业学院学报,2000,15(4),84~86
[95] 李贺,梁奇,唐水花等,预还原催化剂 LaNiO3,La4Ni3O10,La3Ni2O7和 La2NiO4催化分解 CH4制碳纳米管的研究,化学学报,2001,59(8):1236～1240
[96] Rostrup-Nielsen J R. Sulfur-passivated nickel catalysts for carbon-free steam reforming of methane. J. Catal., 1984, 85:31～43
[2] Tindall B M, King D. Hydrocarbon Processing, July, 1994
[3] 陆世雄译,C1化学-创造未来的化学,日本化学会编,1990
[4] Bharadwaj S S, Schmidt L D. Catalytic partial oxidation of natural gas to syngas. Fuel Processing Technology, 1995, 42: 109~127
[5] Tsang S C, Claridge J B, Green M L H. Recent advances in the conversion syngas. Fuel Processing Technology, 1995, 42: 109~127
[6] Farina G L, Supp E. Produce syngas for methanol. Hydrogen Processing, Mar. 1992, 71(3): 77
[7] Prettre M, Ichner C E. Trans. Faraday Soc., 1946, 43:335
[8] Dissanayake D, Rosynek M P. Partial oxidation of methane to carbon monoxide and hygrogen over a Ni/Al2O3. J. Catal.,1991, 132:117～127
[9] Choudhary V R, Rane V H, Rajput A M. Selective oxidation of methane to CO and H2 over unreduced NiO-rare earth oxide catalysts. Catal. Lett.,1993, 22( 4): 289~297
[10] Slagtern A, Swaan H M, Olsbye U. Catalytic partial oxidation of methane over Ni-, Co- and Fe- based catalysts. Catal. Today, 1998, 46:107～115
[11] Takeguchi T, Furukawa S N. Autothermal reforming of methane over Ni catalysts supported over CaO-CeO2-ZrO2 solid solution. Appl. Catal. A: General, 2003, 240: 223~233
[12] Nishimoto H, Nakagawa K, Suzuki T, et al. Partial oxidation of methane to synthesis gas over oxidized diamond catalysts. Appl. Catal. A: General, 2004, 264: 65～72
[13] Barbero J, Pen M A, Campos-Martin J M, et al. Support effect in supported Ni catalysts on their performance for methane partial oxidation. Catal. Lett. 2003, 87 (3~4): 211~218
[14] Sittiphong, Pengpanich, Vissanu, et al. Methane partial oxidation over Ni/CeO2-ZrO2 mixed oxide solid solution catalysts. Catal. Today, 2004, 93: 95~105
[15] 曹立新,李燕馨,李文钊,Ni 系列催化剂上甲烷直接氧化制合成气,分子催化,1994,8(5):375～382
[16] Hayakawa T, Anderson A G, Shimizu M, et al. Partial oxidation of methane to synthesis gas over some titanates based perovskite oxides. Catal. Lett. 1993, 22: 307~317
[17] Provendier H, Petita C, Stabilization of active nickel catalyts in partial oxidation of methane to synthesis gas by iron addition. Appl. Catal. A: General, 1999, 180: 163~173
[18] Alptekin G O, Herring A M, Williamson D L, et al. Methane partial oxidation by unsupported and silica supported iron phosphate catalysts: influence of reaction conditions and Co-feeding of water on activity and selectivity. J. Catal., 1999, 181: 104~112
[19] Vermeiren W J M, Blomsma E, Jacobs P A. Catalytic and thermodynamic approach of the oxyreforming reaction of methane. Catal. Today, 1992, 13: 427～436
[20] Utaka T, Abdulaziz A D S. Partial oxidation of methane over Ni catalysts based on hexaaluminate or perovskite type oxides. Appl. Catal., A: General, 2003, 247(1): 125~131
[21] 张兆斌,余长春,甲烷部分氧化制合成气的 La2O3 助 Ni/MgA12O4 催化剂,催化学报,2000,21(1):14-18
[22] Ruckenstein E, Hu Y H. Methane partial oxidation over NiO/MgO solid solution catalysts. Appl. Catal. A: Gen, 1999, 183: 85~92
[23] Vernon P D F, Green M L H, Cheetham A K. Partial oxidation of methane to synthesis gas. Catal. Lett., 1990, 6: 181~186
[24] Torniainen P M, Chu X, Schmidt L D. Comparison of monolith-supported metals for the direct oxidation of methane to syngas. J. Catal., 1994, 146: 1~10
[25] Kunimori K, Umeda S. Partial oxidation to synthesis gas over rhodium vanadate RhVO4: redispersion of Rh metal during the reaction. Chem. Soc. Jpn., 1992, 65: 2526~2564
[26] Bhattacharya A K, Breach J A, Chand S, et al. Selective oxidation of methane to carbon monoxide on supported palladium catalyst. Appl. Catal. A: General, 1992, 80(1): 1~5
[27] Mataumura Y, Moffat J B. Partial oxidation of methane to carbon-monoxide and hydrogen with molecular-oxygen and nitrous-oxide over hydroxyapatite catalysts. J. catal. 1994, 148:323～333
[28] Claridge J B, York A P E, Brungs A J, et al. New catalysts for the conversion of methane to synthesis gas:molybdenum and tungsten carbide. J. Catal., 1998, 180: 85～100
[29] Hickman D A, Schmidt L D. Synthesis gas formation by direct oxidation of methane over Pt monoliths. J. Catal., 1992, 138: 267~282
[30] 沈师孔,李春义,余长春,Ni/Al2O3 催化剂上甲烷部分氧化制合成气反应机理,催化学报,1998,19(4):309～314
[31] Au C T, Wang Y H, Wan H L. Mechanistic Studies of CH4/O2 Conversion over SiO2-Supported Nickel and Copper Catalysts. J. Catal., 1996, 158: 343~348
[32] Lu Y, Xue J Z, Yu C C, et al. Mechanistic investigations on the partial oxidation of methane to synthesis gas over a nickel-on-alumina catalyst. Appl. Catal. A: Gen., 1998, 174: 121~128
[33] Ji Y Y, Li W Z, Xu H Y, et al. Partial oxidation of methane to syngas in fluidized bed reactor. Chinese J. Catal., 2000, 21(2): 97～98
[34] Claridge J B, Green M H L, Tsang S C, et al. A study of carbon deposition on catalysts during the partial oxidation of methane to synthesis gas. Catal. Lett., 1993, 22: 299~305
[35] Rostrup-Nielsen J R. Coking on nickel catalysts for steam reforming of hydrogen. J. Catal., 1974, 33:184～201
[36] 徐恒泳,孙希贤,范业梅等,甲烷、二氧化碳转化制合成气的研究,石油化工,1992,21(3):147~153
[37] 李春义,余长春,沈师孔,Ni /Al2O3 催化剂上 CH4 部分氧化制合成气反应积碳的原因,催化学报,2001,22(4):377~382
[38] 曹立新,陈燕馨,李文钊,载体对甲烷直接氧化制合成气的影响,天然气化工,1996,21(3):3~15
[39] Tsipouriari V A, Verykios X E. Catalytic partial oxidation of methane to synthesis gas over Ni-based catalysts: II. transient, FTIR, and XRD measurements. J. Catal., 1998, 179: 292～299
[40] 金荣超,陈燕馨,李文剑,甲烷催化部分氧化 Ni 催化剂及 Ce 的研究,物理化学学报,1998, 14(8):737~741
[41] 路勇,余长春,沈师孔等,负载型镍金属催化剂上甲烷与二氧化碳重整制合成气,催化学报,1996, 17(3):212~216
[42] Takashi Hayakawa, Hideaki Harihara, Ahdrew P E York, et al. A Sustainable catalyst for the partial oxidation of methane to syngas: Ni / Ca l-xSrxTiO3prepared in situ from perovskite precursors. Angew. Chem. Int. Ed. Engl., 1996, 35(2):192~
[43] Torniainen P, Chu X, Schmidt L D. Comparison of monolith- supported metal for the direct oxidation of methane to syngas, J. Catal., 1994, 146:1~10
[44] Honig R E, Kramer D A, RCA Rec., 1969,30:285
[45] Lu Y, Shen S K. Design of stable Ni catalysts for partial oxidation of methane to synthesis gas. J. Catal., 1998, 177:386~388
[46] Liu S L, Xiong G X. The effect of Li and La on NiO/Al2O3 catalyst for CH4/O2 to syngas reaction. React. Kinet. Catal. Lett., 1999, 68(2):243~247
[47] Rao C N R, Ganguly P. A comparative study of the magnetic and electrical properties of perovskite oxide and the corresponding two-dimensional oxides of K2NiF4 structure. Singh K K, Ram R A M. J. solid state chem. 1988, 72:14
[48] Odier P, Leblanc M, Choisnet J. Structural characterization of an orthorhombic form of La2NiO4. Mater. Res. Bull, 1986, 21(7):787~796
[49] 何俊,孙颖稼等,A2BO4 型催化活性材料结构与性能的研究,分子催化,1994,8(5):325~329
[50] Weng D, Zhao H S, Wu X D, et al. Influence of cerium on the performance of LaMO3(M=Mn or Mn-Cu) perovskite-type catalyst. Mater. Sci. Eng. A, 2003, 361:173~178
[51] Libby W R. Promising catalyst for auto exhaust. Science,1971,171:499~500
[52] Gunasekaran N, Rajadurai S, Carberry J. Catalytic decomposition of nitrous oxide over perovskite type solid oxide solutions and supported noble metal catalysts. Catal. Lett., 1995, 35(3,4):373
[53] Nakamura T, Misono M, Yoneda Y. Reduction-oxidation and catalytic properties of perovskite-type mixed oxide catalysts lanthanum strontium cobalt oxide ( La1-xSrxCoO3). Chem. Lett., 1981, (11):1589
[54] Gao L Z, Au C T. Studies on the decomposition of N2O over Nd2CuO4,Nd1.6Ba0.4CuO4 and Nd1.8Ce0.2CuO4. J. Mol. Catal. A, 2001, 168(2):173~186
[55] Arai H, Yamada T, Eguchi K, et al. Catalytic combustion of methane over various perovskite-type oxides. Appl. Catal., 1986, 26(1-2):265
[56] Pena M A, Fierro J L G. Chemical structures and performance of perovskite oxides. Chem. Rev., 2001, 101(7):1981~2018
[57] 杨秋华,傅希贤,纳米 LaMO3(M = Cr, Mn, Fe, Co)化合物的光催化氧化活性分析,硅酸盐学报,2003, 31(3):254~256
[58] 傅希贤,桑丽霞,钙钛矿型(ABO3)化合物的光催化活性及其影响因素,天津大学学报,2001,34(2):229~231
[59] Wang D F, Zhou Z G.A new spinel type photocatalysts BaCr2O4 for H2 evolution under UV and Visible Light irradiation.Chem.Phys.Lett., 2003, (373):191~196
[60] 冉锐,吴晓东,翁端,稀土钙钛矿催化剂制备方法研究进展,稀土,2004,25(5):46～50
[61] 徐科,严洁,钙钛矿型稀土纳米复合氧化物制备及应用研究进展,贵州大学学报(自然科学版),2003,20(4):421～425
[62] 刘源,钙钛矿型 LaCoO3 和 LaMnO3 超细粒子的制备,内蒙古工业大学学报,2000,19(3):192~196
[63] 翟永青,姚子华,EDTA 络合溶胶-凝胶法制备 La0.8Sr0.2FeO3 纳米粉体,稀有金属,2002,26(1):69~72
[64] Ciambelli P, Cimino S, Lisi L. La, Ca and Fe oxide perovskites: preparation, characterization and catalytic properties for methane combustion. Appl. Catal. B: environmental, 2001, 33: 193~203
[65] 张翔宇,李振花,甲烷部分氧化制合成气催化剂的研究进展,化工进展,2002,21(12):903~907
[66] 张恒,董新法,林维明,Ni 基催化剂上甲烷部分氧化制合成气,天然气化工,2004,19(3):36~42
[67] Zhang Z, Verykios X E. Carbon dioxide reforming of methane to synthesis gas over Ni/La2O3 catalysts. Appl. Catal. A: General, 1996, 138: 109~133
[68] Tsipouriari V A, Verykios X E. Carbon and oxygen reaction pathways of CO2 reforming of methane over Ni/La2O3 and Ni/Al2O3 catalysts studied by isotopic tracing Techniques. J. Catal., 1999, 187: 85~94
[69] Tsipouriari V A, Verykios X E. Kinetic study of the catalytic reforming of methane with carbon dioxide to synthesis gas over Ni/La2O3 catalyst. Catal. Today, 2001, 64: 83~90
[70] Tsipouriari V A, Zhang Z, Verykios X E. Catalytic partial oxidation of methane to synthesis gas over Ni-based catalysts. J. Catal., 1998, 179: 283~291
[71] 刘盛林,熊国兴,缪清等,锂和镧的添加对 NiO/Al2O3 甲烷部分氧化积碳的影响,天然气化工,1998,23(5):5~7
[72] 王爱菊,CH4 部分氧化制氢复合氧化物负载 Ni-Cu 催化剂制备及反应性能研究,[博士学位论文],天津,天津大学,2003
[73] Ruckenstein E, Hu Y H. Interactions between Ni and La2O3 in Ni/La2O3 catalystsprepared using different Ni precursors. J. Catal., 1996, 161: 55~61
[74] Barbero J, Pena M A, Campos-Martin J M, et al. Support effect in supported Ni catalysts on their performance for methane partial oxidation. Catal. Lett., 2003, 87: 211~218
[75] Slagtern A, Schuurman Y, Leclercq C, et al., Specific features concerning the mechanism of methane reforming by carbon dioxide over Ni/La2O3 catalysts. J. Catal. 1997, 172: 118~126
[76] 李文英,冯杰,谢克昌等,CH4-CO2 重整反应镍基催化剂的积碳性能的研究.燃料化学学报,1997,25(5):460~464
[77] 陈吉祥,王日杰,李玉敏等,镍基气凝胶催化 CH4-CO2 重整制取合成气反应的研究,燃料化学学报,2002,30(5):445~453
[78] 田辉平,钙钛矿型稀土复合氧化物的深度氧化性能研究,[博士学位论文],天津,天津大学,1992
[79] 陈铜,于作龙,远松月等,Bi-Mo-Nb 复合氧化物的结构与对丙烯氧化的催化活性,化学学报,1994(6):521～528
[80] Garin F, Simonot L, Maire G. A comparative study of LaCoO3, Co3O4 and a mix of LaCoO3-Co3O4 Ⅱ Catalytic properties for the CO + NO reaction. Appl. Catal. B: Environment, 1997, 11: 181~191
[81] Provendier H, Petit C, Estournes C, et al. Stabilisation of active nickel catalysts in partial oxidation of methane to synthesis gas by iron addition, Appl. Catal. A: General, 1999, 180: 163~173
[82] Takehira K, Shishido T, Kondo M. Partial oxidation of CH4 over Ni/SrTiO3 catalysts prepared by a solid-phase crystallization method. J. Catal. 2002, 207:307~316
[83] Guo C L, Zhang J L, Li W, et al. Partial oxidation of methane to syngas over BaTi1-xNixO3 catalysts. Catal. Today, 2004, 98:583~587
[84] Liu S, Tan X Y, Li K. Synthesis of strontium cerates-based perovskite ceramics via water-soluble complex precursor routes. Ceramics international, 2002, 28:327~335
[85] 侯峰,La-Ni-O 系薄膜复合材料氧敏性能的研究,[博士学位论文],天津,天津大学,2001
[86] Wang H, Zhu Y, Liu Y. Preparation of nanosized perovskite LaNiO3 powder via amorphous heteronuclear complex precursor. J. Mater. Sci., 2003, 38: 1939-1943
[87] 高利珍,于作龙,吴越,在镍系钙钛矿(ABO3)型催化剂上的氨氧化 Ⅲ.焙烧温度对催化剂结构和活性的影响,1992,9(2):21~25
[88] Fernandes J D G, Melo D M A, Zinner L B, et al. Low-temperature synthesis of single phase crystallize LaNiO3 perovskite via Pechini method. Mater. Lett., 2002, 53: 122~125
[89] Handbook of X-ray Photoelectron Spectroscopy, Moulder J F, Stickle W F, Sobol P E, Bomben K D. Published by Perkin-Elmer Corperation, United States of America
[90] Liu B S, Au C T. Sol-gel generated La2NiO4 for CH4/CO2 reforming. Catal. lett., 2003, 85(3-4):165~170
[91] Liu B S, Au C T. Carbon deposition and catalyst stability over La2NiO4/ γ ?Al2O3 during CO2 reforming of methane to syngas. Appl. Catal. A: General, 2003, 244: 181~195
[92] Zhang W D, Liu B S, Zhu C, et al. Preparation of La2NiO4 /ZSM-5 catalyst and catalytic performance in CO2/CH4 reforming to syngas. Appl. Catal. A: General, 2005, 292: 138~143
[93] 池玉娟,于海涛,李环宇,钙钛矿型复合氧化物 La1-xSrxFeO3 纳米晶制备研究,黑龙江大学自然科学学报,2000,17(1):73~78
[94] 娄向东,田圣军,姜聚慧,含镧钙钛矿型复合氧化物的制备方法评价,郑州轻工业学院学报,2000,15(4),84~86
[95] 李贺,梁奇,唐水花等,预还原催化剂 LaNiO3,La4Ni3O10,La3Ni2O7和 La2NiO4催化分解 CH4制碳纳米管的研究,化学学报,2001,59(8):1236～1240
[96] Rostrup-Nielsen J R. Sulfur-passivated nickel catalysts for carbon-free steam reforming of methane. J. Catal., 1984, 85:31～43
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