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Steam reforming of n-dodecane over mesoporous alumina supported nickel catalysts: Effects of metal-support interaction on nickel catalysts

机译:介孔氧化铝负载的镍催化剂上正十二烷的蒸汽重整:金属-载体相互作用对镍催化剂的影响

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摘要

Developing a highly active and stable Ni-based catalyst is still a challenge for the generation of on-site hydrogen through steam reforming of long-chained hydrocarbons, such as kerosene fuels. Ni nanoparticles (ca. 5 nm) on mesoporous alumina prepared by atomic layer deposition (ALD) were employed in steam reforming of n-dodecane, and exhibited a turnover frequency (TOF) of 477.6 h(-1), whereas Ni nanoparticles on commercial alumina support prepared by impregnation method exhibited a TOF of 100 h(-1). The high activity of ALD Ni catalysts was ascribed to high reduction degree, as confirmed by X-ray diffraction (XRD), transmission electron microscopy (TEM), and H-2-chemisorption. A deactivation was also observed on the ALD prepared catalysts, which was ascribed to the weak metal support interaction, as confirmed by H-2 temperature-programmed reduction (TPR). The ALD Ni/Al2O3 catalysts were further modified with CeO2 and they showed enhanced stability with 8% deactivation degree in steam reforming of n-dodecane. Further characterizations of spent catalysts showed that the presence of CeO2 was favorable for stabilizing Ni nanoparticles by enhancing moderate metal-support interaction, and reducing the formation of coke on the interfaces of Ni CeO2. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
机译:对于通过长链烃(例如煤油燃料)的蒸汽重整来产生现场氢气而言,开发高活性和稳定的Ni基催化剂仍然是一个挑战。通过原子层沉积(ALD)在介孔氧化铝上制备的Ni纳米颗粒(约5 nm)被用于正十二烷的蒸汽重整,其周转频率(TOF)为477.6 h(-1),而在工业应用中的Ni纳米颗粒浸渍法制备的氧化铝载体的TOF为100 h(-1)。通过X射线衍射(XRD),透射电子显微镜(TEM)和H-2-化学吸附证实了ALD Ni催化剂的高活性归因于高还原度。如H-2程序升温还原(TPR)所证实,在ALD制备的催化剂上也观察到失活,这归因于弱的金属载体相互作用。用CeO2对ALD Ni / Al2O3催化剂进行了进一步改性,在正十二烷的蒸汽重整中,失活度为8%,稳定性得到了提高。废催化剂的进一步表征表明,CeO2的存在有利于通过增强适度的金属-载体相互作用并减少Ni CeO2界面上焦炭的形成来稳定Ni纳米颗粒。 (C)2019氢能出版物有限公司。由Elsevier Ltd.出版。保留所有权利。

著录项

  • 来源
    《International journal of hydrogen energy》 |2019年第13期|6965-6977|共13页
  • 作者单位

    Tianjin Univ, Sch Chem Engn & Technol, Minist Educ, Key Lab Green Chem Technol, Tianjin 300072, Peoples R China;

    Missouri Univ Sci & Technol, Dept Chem & Biochem Engn, Rolla, MO 65409 USA;

    Tianjin Univ, Sch Chem Engn & Technol, Minist Educ, Key Lab Green Chem Technol, Tianjin 300072, Peoples R China;

    Tianjin Univ, Sch Chem Engn & Technol, Minist Educ, Key Lab Green Chem Technol, Tianjin 300072, Peoples R China;

    Missouri Univ Sci & Technol, Dept Chem & Biochem Engn, Rolla, MO 65409 USA;

    Tianjin Univ, Sch Chem Engn & Technol, Minist Educ, Key Lab Green Chem Technol, Tianjin 300072, Peoples R China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Ni/Al2O3 catalyst; Ceria; Metal-support interaction; Steam reforming; N-dodecane;

    机译:Ni / Al2O3催化剂;二氧化铈;金属-载体相互作用;蒸汽重整;N-十二烷;
  • 入库时间 2022-08-18 04:13:54

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