Highly dispersed Ni/SBA-15 catalysts prepared with different nickel salts as nickel precursors:Effects of activation atmospheres
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摘要: 以硝酸镍和乙酸镍为镍前体,用浸渍法分别在空气和氢气氛围活化制得系列Ni/SBA-15催化剂,通过XRD、H2-TPD、N2物理吸附和在线质谱等物理化学手段对催化剂进行了表征,并结合微型高压反应釜萘加氢反应,评价了催化剂的加氢性能。结果表明,氢气氛围活化对硝酸镍为镍前体所制Ni/SBA-15催化剂的镍分散度和活性有显著促进作用,而空气氛围活化对乙酸镍为镍前体所制催化剂有明显促进作用。根据催化剂前体在不同氛围活化时的热分解产物,提出了活化氛围对不同镍前体制得Ni/SBA-15催化剂所产生的作用机理。Abstract: With nickel nitrate and nickel acetate as nickel precursors, a series of Ni/SBA-15 catalysts were prepared by using the impregnation method and activating in air or hydrogen atmosphere. The Ni/SBA-15 catalysts were characterized with XRD, H2-TPD, N2 physisorption and online mass spectroscopy. Their catalytic properties were evaluated with hydrogenation of naphthalene as a model reaction. It was shown that activation in hydrogen greatly increased the Ni dispersion and catalytic activity of Ni/SBA-15 prepared with nickel nitrate, while activation in air significantly improved the sample prepared with nickel acetate. In terms of the thermal decomposition products of the catalyst precursors activated in different atmospheres, the affecting mechanism of the activation atmosphere on the Ni/SBA-15 catalysts prepared with different nickel precursors was proposed.
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Key words:
- Ni/SBA-15 /
- nickel nitrate /
- nickel acetate /
- activation atmosphere /
- dispersion /
- hydrogenation of naphthalene
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STANISLAUS A, COOPER B H. Aromatic hydrogenation catalysis: A review[J]. Catal Rev Sci Eng, 1994, 36(1): 75-123.
WEISSERMEL K, ARPLE H J. Industrial organic chemistry[M]. 4th ed. Weinheim: Wiley-VCH, 2003.
DILLEN A J, TERÖRDE R M, LENSVELD D J. Synthesis of supported catalysts by impregnation and drying using aqueous chelated metal complexes[J]. J Catal, 2003, 216(1): 257-264.
LI F, YI X D, FANG W P. Effect of organic nickel precursor on the reduction performance and hydrogenation activity of Ni/Al2O3 catalysts[J]. Catal Lett, 2009, 130(3/4): 335-340.
LIU H C, WANG H, SHEN J H, SUN Y, LIU Z M. Preparation, characterization and activities of the nano-sized Ni/SBA-15 catalyst for producing COx-free hydrogen from ammonia[J]. Appl Catal A: Gen, 2008, 337(2): 138-147.
REN S B, ZHANG P, SHUI H F, LEI Z P, WANG Z C, KANG S G. Promotion of Ni/SBA-15 catalyst for hydrogenation of naphthalene by pretreatment with ammonia/water vapour[J]. Catal Commun, 2010, 12(2): 132-136.
LI X K, JI W J, ZHAO J, WANG S J, AU C T. Ammonia decomposition over Ru and Ni catalysts supported on fumed SiO2, MCM-41, and SBA-15[J]. J Catal, 2005, 236(2): 181-189.
POELS E K, DEKKER J G, LEEUWEN W A V. Hydrothermal sintering of the active phase in alumina supported fixed bed nickel catalysts during reduction[J]. Stud Surf Sci Catal, 1991, 63: 205-214.
VOS B, POELS E K, BLIEK A. Impact of calcination conditions on the structure of alumina-supported nickel particles[J]. J Catal, 2001, 198(1): 77-88.
DE LOOSDRECHT J V, BARRADAS S, CARICATO E A, NGWENYA N G, NKWANYANA P S, RAWAT M A S, SIGWEBELA B H, VAN BERGE P J, VISAGIE J L. Calcination of Co-based Fischer-Tropsch synthesis catalysts[J]. Top Catal, 2003, 26(1/4): 121-127.
SIETSMA J R A, MEELDIJK J D, BREEJEN J P, VERSLUIJS-HELDER M, JOS VAN DILLEN A, DE JONGH P E, DE JONG K P. The preparation of supported NiO and Co3O4 nanoparticles by the nitric oxide controlled thermal decomposition of nitrates[J]. Angew Chem Int Ed, 2007, 46(24): 4547-4549.
SIETSMA J R A, FRIEDRICH H, BROERSMA A, VERSLUIJS-HELDER M, JOS VAN DILLEN A, DE JONGH P E, DE JONG K P. How nitric oxide affects the decomposition of supported nickel nitrate to arrive at highly dispersed catalysts[J]. J Catal, 2008, 260(2): 227-235.
SIETSMA J R A, MEELDIJK J D, VERSLUIJS-HELDER M, BROERSMA A, JOS VAN DILLEN A, DE JONGH P E, DE JONG K P. Ordered mesoporous silica to study the preparation of Ni/SiO2 ex nitrate catalysts: Impregnation, drying, and thermal treatments[J]. Chem Mater, 2008, 20(9): 2921-2931.
REN S B, ZHAO R, ZHANG P, LEI Z P, WANG Z C, KANG S G, PAN C X, SHUI H F. Effect of activation atmosphere on reduction behaviors, dispersion and activities of nickel catalysts for hydrogenation of naphthalene[J]. React Kinet Mech Cat, 2014, 111(1): 247-257.
KIRUMAKKI S R, SHPEIZER B G, SAGAR G V, CLEARFIELD A. Hydrogenation of Naphthalene over NiO/SiO2-Al2O3 catalysts: Structure-activity correlation[J]. J Catal, 2006, 242(2): 319-331.
VELU S, GANGWAL S K. Synthesis of alumina supported nickel nanoparticle catalysts and evaluation of nickel metal dispersions by temperature programmed desorption[J]. Solid State Ionics, 2006, 177(7): 803-811.
DE JESUS J C, GONZ'ALEZ I, QUEVEDO A, PUERTA T. Thermal decomposition of nickel acetate tetrahydrate: An integrated study by TGA, QMS and XPS techniques[J]. J Mol Catal A, 2005, 228(1): 283-291.
HELVEG S, LÓPEZ-CARTES C, SEHESTED J, HANSEN P L, CLAUSEN B S, ROSTRUP-NIELSEN J R, ABILD-PEDERSEN F, NØRSKOV J K. Atomic-scale imaging of carbon nanofibre growth[J]. Nature, 2004, 427(6973): 426-429.
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