One-Step Hydropyrolysis and Hydrotreating Tandem Reactions of Miscanthus × giganteus Using Ni Impregnated ZSM-5/MCM-41 Composites
One-Step Hydropyrolysis and Hydrotreating Tandem Reactions of Miscanthus × giganteus Using Ni Impregnated ZSM-5/MCM-41 Composites
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DOI：
10.1021/acs.energyfuels.1c02453
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发表时间：
2021-11
期刊：
影响因子：
5.3
通讯作者：
Lei Yu;A. Farinmade;Oluwole Ajumobi;V. John;J. Valla
中科院分区：
文献类型：
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作者：
Lei Yu;A. Farinmade;Oluwole Ajumobi;V. John;J. Valla
在这项研究中，我们提出，利用包裹在球形Ni-MCM-41(Ni-ZSM-5/Ni-MCM-41)中的Ni-ZSM-5微晶的复合材料，可以一步完成生物质的多步、串联催化快速加氢裂解(CFHP)和加氢处理反应，以制备汽油和柴油级生物燃料。采用一步气溶胶法制备了该复合材料，并用氮气吸附-脱附、X-射线衍射、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、吡啶吸附、电感耦合等离子体发射光谱(ICPOES)和氢化学吸附等手段对其进行了表征。将该复合材料在600℃和500℃下进行了一段循环热压和芒果加氢处理的试验，并与一段Ni-ZSM-5和第二段加氢处理(加氢处理)的典型两段工艺的产物产率和分布进行了比较。使用Ni-ZSM-5、Ni-ZSM-5/MCM-41和ZSM-5/Ni-MCM-41复合材料以及Ni-ZSM-5和Ni-MCM-41的物理混合物进行了其他实验，以进一步了解复合材料各部分对一段CFHP和加氢处理反应产物产率和分布的影响。结果表明，Ni-ZSM-5/Ni-MCM-41复合材料在不牺牲单芳烃产率的情况下，提高了烷烃和甲烷的生成量。因此，本研究证明，这种独特的复合材料可以一步完成两步串联反应，导致一个自我持续和强化的过程。
In this study, we propose that the multistep, tandem catalytic fast hydropyrolysis (CFHP) and hydrotreatment reactions of biomass to produce gasoline and diesel grade biofuels can be conducted in a single step process using a composite of Ni-ZSM-5 microcrystals encapsulated in spherical particles of Ni-MCM-41 (Ni-ZSM-5/Ni-MCM-41). The composite has been successfully preparedviaa one-step aerosol method and characterized by N2adsorption–desorption, X-ray diffraction, scanning electron microscope (SEM), transmission electron microscope (TEM), pyridine adsorption, inductively coupled plasma-optical emission spectrometry (ICP-OES), and H2chemisorption. The composite has been tested for one-stage CFHP and hydrotreatment ofMiscanthus × giganteusat 600 and 500 °C. The product yields and distribution derived from the one-stage CFHP and hydrotreatment ofMiscanthus × giganteususing the Ni-ZSM-5/Ni-MCM-41 composite were compared to those of a typical two-stage process, with Ni-ZSM-5 in the first stage (CFHP) and Ni-MCM-41 in the second stage (hydrotreatment). Additional experiments were carried out using Ni-ZSM-5, Ni-ZSM-5/MCM-41, and ZSM-5/Ni-MCM-41 composites, as well as physical mixtures of Ni-ZSM-5 and Ni-MCM-41 to obtain further insights into the role of each part of the composites to the product yields and distribution derived from the one-stage CFHP and hydrotreatment reaction. The comparison of results showed that the Ni-ZSM-5/Ni-MCM-41 composite enhanced the production of alkanes and methane without sacrificing the yield to monoaromatic hydrocarbons. Therefore, this study proves that such a unique composite can complete the two-step tandem reactions in one single step, leading to a self-sustainable and intensified process.