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Catalytic activities of K-modified zeolite ZSM-5 supported rhodium catalysts in low-temperature steam reforming of bioethanol

机译:K改性沸石ZSM-5负载铑催化剂在生物乙醇低温蒸汽重整中的催化活性

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摘要

Recently, zeolite materials have attracted attention as efficient catalysts for low-temperature steam reforming of bioethanol (SRE). However, cost-effective zeolite ZSM-5 materials, one of the most popular industrial reforming catalysts, were rarely reported for SRE. In this study, low-load rhodium (Rh) catalysts are prepared using commercial high-silica zeolite ZSM-5 as the supports. The commercial zeolite ZSM-5 has strong acidic sites that lead to fairly extensive dehydration of bioethanol. To generate basic sites and mesoporous structure, zeolite supports are modified by K ion exchange and alkali treatment. The effect of the physicochemical properties of the modified supports on low-temperature SRE reaction is investigated by SEM, TEM, XRD, XRF, TPD, NMR and N-2 adsorption. The results indicate that strong acidic sites in zeolite ZSM-5 can be effectively neutralized by K ion exchange, while basic sites in zeolite ZSM-5 are noticeably altered only by alkali treatment. The hydrogen selectivity can be significantly promoted by the alkalinity of the zeolite KZSM-5, however, only the moderate alkali-treated Rh/S2 catalyst retains its high activity during reaction. Our results appear to demonstrate the positive effect of the special zeolitic structure of the Rh/52 catalyst with uniform mesopores, which can improve the Rh dispersion and avoid its sintering. Moreover, there seem to be a unique synergy between the Rh active component and the alkali-treated zeolite support, which might result in the lowest CO selectivity at 300-400 degrees C. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
机译:近来,沸石材料作为用于生物乙醇的低温蒸汽重整的有效催化剂已引起关注。然而,极少报道具有成本效益的沸石ZSM-5材料,其是最流行的工业重整催化剂之一。在这项研究中,低负载的铑(Rh)催化剂是使用商业化高硅沸石ZSM-5作为载体制备的。商业沸石ZSM-5具有强酸性部位,可导致生物乙醇相当广泛的脱水。为了产生碱性位点和中孔结构,通过K离子交换和碱处理来改性沸石载体。通过SEM,TEM,XRD,XRF,TPD,NMR和N-2吸附研究了改性载体的理化性质对低温SRE反应的影响。结果表明,通过钾离子交换可以有效地中和沸石ZSM-5中的强酸性位,而仅通过碱处理才能显着改变沸石ZSM-5中的碱性位。沸石KZSM-5的碱度可以大大提高氢的选择性,但是,只有中度碱处理的Rh / S2催化剂在反应过程中仍保持高活性。我们的结果似乎证明了具有均匀中孔的Rh / 52催化剂的特殊沸石结构的积极作用,可以改善Rh的分散性并避免其烧结。此外,Rh活性组分和碱处理的沸石载体之间似乎存在独特的协同作用,这可能导致在300-400摄氏度下最低的CO选择性。版权所有(C)2015,Hydrogen Energy Publications,LLC。由Elsevier Ltd.出版。保留所有权利。

著录项

  • 来源
    《International journal of hydrogen energy》 |2015年第32期|9924-9934|共11页
  • 作者单位

    Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangzhou 510640, Peoples R China;

    Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangzhou 510640, Peoples R China|Univ Chinese Acad Sci, Beijing 100049, Peoples R China;

    Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangzhou 510640, Peoples R China;

    Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangzhou 510640, Peoples R China;

    Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangzhou 510640, 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

    Hydrogen production; Stream reforming of bioethanol; Zeolite ZSM-5; Modification; Rh-based catalysts;

    机译:制氢;生物乙醇物流重整;沸石ZSM-5;改性;Rh基催化剂;

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