Effects of Yb2O3 promotor on the performance of Ni/SiC catalysts in CO2 reforming of CH4
-
摘要: 采用浸渍法制备了Ni/SiC和Ni-Ybx/SiC(x=2%、4%、6%、10%,质量分数)催化剂,在固定床反应装置中考察了催化剂在甲烷二氧化碳重整反应中的性能。利用BET、ICP-AES、XRD、H2-TPR、TG-DTA、XPS和TEM等技术对催化剂进行了表征。实验结果表明,Yb的适宜添加量为4%~6%。在800 ℃条件下Ni-Yb4/SiC和Ni-Yb6/SiC催化剂具有优异的催化活性和稳定性,在100 h的重整反应中,甲烷和二氧化碳的转化率始终保持在90%以上。Yb2O3助剂能够抑制镍颗粒的生长和减少碳沉积量,因此,Ni-Yb/SiC催化剂在连续反应中表现出稳定的活性。
-
关键词:
- 甲烷二氧化碳重整 /
- Ni-Yb/SiC催化剂 /
- 助剂 /
- 稳定性
Abstract: Ni/SiC and Ni-Ybx/SiC (x=2%, 4%, 6%,10%) catalysts were prepared by the impregnation method, and the performances of catalysts in the carbon dioxide reforming of methane were studied in a fixed-bed reactor.The catalysts were characterized by BET, ICP-AES, XRD, H2-TPR, TG-DTA, XPS and TEM techniques.The experimental results indicate that the appropriate addition amount of Yb is 4% to 6%.Ni-Yb4/SiC and Ni-Yb6/SiC catalysts exhibit excellent catalytic activity and stability at 800 ℃, and the conversion of CH4 and CO2 can be maintained over 90% during the 100 h testing. Yb2O3 promotor can inhibit the growth of nickel nanoparticles and reduce the amount of carbon deposition,therefore Ni-Yb/SiC catalysts show stable activity in the continuous reforming reaction.-
Key words:
- CO2 reforming of CH4 /
- Ni-Yb/SiC catalyst /
- promotor /
- stability
-
FAN M S, ABDULLAH A Z, BHATIA S. Catalytic technology for carbon dioxide reforming of methane to synthesis gas[J]. ChemCatChem, 2009, 1(2): 192-208. 王莉, 敖先权, 王诗翰. 甲烷与二氧化碳催化重整制取合成气催化剂[J]. 化学进展, 2012, 24(9): 1696-1706. (WANG Li, AO Xian-quan, WANG Shi-han. Catalysts for carbon dioxide catalytic reforming of methane to synthesis gas[J]. Progress in Chemistry, 2012, 24(9): 1696-1706.) FISCHER F, TROPSCH H. Conversion of methane into hydrogen and carbon monoxide[J]. BrennstChem, 1928, 9: 39-46. BRADFORD M C J, VANNICE M A. CO2 reforming of CH4 over supported Ru catalysts[J]. J Catal, 1999, 183(1): 69-75. WANG H Y, RUCKENSTEIN E. Carbon dioxide reforming of methane to synthesis gas over supported rhodium catalysts: The effect of support[J]. Appl Catal A: Gen, 2000, 204(1): 143-152. YAMAGUCHI A, IGLESIA E. Catalytic activation and reforming of methane on supported palladium clusters[J]. J Catal, 2010, 274(1): 52-63. WEI J M, GLESIA E. Structural and mechanistic requirements for methane activation and chemical conversion on supported iridium clusters[J]. Angew Chem Int Ed, 2004, 43(28): 3685-3688. PANT B, STAGG-WILLIAMS S M. Investigation of the stability of Pt/LaCoO3 during high temperature reforming reactions[J]. Catal Commun, 2004, 5(6): 305-309. ROSTRUPNIELSEN J R, HANSEN J H B. CO2-reforming of methane over transition metals[J]. J Catal, 1993, 144(1): 38-49. 徐军科, 任克威, 王晓蕾, 周伟, 潘相敏, 马建新. 甲烷干重整制氢研究进展[J]. 天然气化工, 2008, 33(3): 53-60. (XU Jun-ke, REN Ke-wei, WANG Xiao-lei, ZHOU Wei, PAN Xiang-min, Ma Jian-xin. Progress in studies on dry-reforming of methane to hydrogen[J]. Natural Gas Chemical Industry, 2008, 33(3): 53-60.) 孙楠楠, 闻霞, 王峰, 彭伟才, 肖福魁, 魏伟, 孙予罕, 李海. 反应条件对Ni-CaO-ZrO2催化剂上CH4-CO2重整反应及积炭的影响[J]. 燃料化学学报, 2012, 40(3): 345-349. (SUN Nan-nan, WEN Xia, WANG Feng, PENG Wei-cai, XIAO Fu-kui, WEI Wei, SUN Yu-han, LI Hai. Influences of reaction conditions on the CH4-CO2 reforming and coking properties of a Ni-CaO-ZrO2 catalyst[J]. Journal of Fuel Chemistry and Technology, 2012, 40(3): 345-349.) LIU H T, LI S Q, ZHANG S B, CHEN L, ZHOU G J, WANG J M, WANG X L. Catalytic performance of monolithic foam Ni/SiC catalyst in carbon dioxide reforming of methane to synthesis gas[J]. Catal Lett, 2008, 120(1/2): 111-115. SUNW Z, JIN G Q, GUO X Y. Partial oxidation of methane to syngas over Ni/SiC catalysts[J]. Catal Commun, 2005, 6(2): 135-139. 职国娟, 王英勇, 靳国强, 郭向云. 镍盐前驱体对CO2甲烷化Ni/SiC催化剂性能的影响[J]. 天然气化工, 2012, 37(5): 10-14. (ZHI Guo-juan, WANG Ying-yong, JIN Guo-qiang, GUO Xiang-yun. Effect of nickel precursors on catalytic performance of Ni/SiC catalysts for CO2 methanation[J]. Natural Gas Chemical Industry, 2012, 37(5): 10-14.) YANG R Q, XING C, LV C X, SHI L, TSUBAKI N. Promotional effect of La2O3 and CeO2 on Ni/gamma-Al2O3 catalysts for CO2 reforming of CH4[J]. Appl Catal A: Gen, 2010, 385(1/2): 92-100. LI X C, WU M, LAI Z H, HE F. Studies on nickel-based catalysts for carbon dioxide reforming of methane[J]. Appl Catal A: Gen, 2005, 290(1/2): 81-86. BARROSO-QUIROGA M M, CASTRO-LUNA A E. Catalytic activity and effect of modifiers on Ni-based catalysts for the dry reforming of methane[J]. Int J Hydrogen Energy, 2010, 35(11): 6052-6056. AMAIN M H, MANTRI K, NEWNHAM J, TARDIO J, BHARGAVA S K. Highly stable ytterbium promoted Ni/gamma-Al2O3 catalysts for carbon dioxide reforming of methane[J]. Appl Catal B: Environ, 2012, 119-120: 217-226. JIN G Q, GUO X Y. Synthesis and characterization of mesoporous silicon carbide[J]. Microporous Mesoporous Mater, 2003, 60(1/3): 207-212. GARCIA-VARGAS J M, VALVERDE J L, DE LUCAS-CONSUEGRA A, GOMEZ-MONEDERO B, SANCHEZ P, DORADO F. Precursor influence and catalytic behaviour of Ni/CeO2 and Ni/SiC catalysts for the tri-reforming process[J]. Appl Catal A: Gen, 2012, 431-432: 49-56. CONTARINI S, HOWLETT S P, RIZZO C, DE ANGELIS B A. XPS study on the dispersion of carbon additives in silicon carbide powders[J]. Appl Surf Sci, 1991, 51(3/4): 177-183. YAMAMOTO T, MATSUYAMA T, TANAKA T, FUNABIKI T, YOSHIDA S. Silica-supported ytterbium oxide characterized by spectroscopic methods and acid-catalyzed reactions[J]. J Mol Catal A: Chem, 2000, 155(1/2): 43-58.
点击查看大图
计量
- 文章访问数: 815
- HTML全文浏览量: 21
- PDF下载量: 670
- 被引次数: 0