Comparative study on phenol and naphthalene steam reforming over Ni-Fe alloy catalysts supported on olivine synthesized by different methods
Comparative study on phenol and naphthalene steam reforming over Ni-Fe alloy catalysts supported on olivine synthesized by different methods
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不同方法合成的橄榄石负载Ni-Fe合金催化剂苯酚和萘水蒸气重整对比研究
DOI：
10.1016/j.enconman.2018.04.112
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发表时间：
2018-07
影响因子：
10.4
通讯作者：
Li Haibin
中科院分区：
文献类型：
--
作者：
Meng Junguang;Zhao Zengli;Wang Xiaobo;Zheng Anqing;Zhang Dongyan;Huang Zhen;Zhao Kun;Wei Guoqiang;Li Haibin
以橄榄石为载体，采用湿浸法和热熔法制备了Ni/Fe催化剂，并在固定床反应器上考察了不同焦油模型化合物（苯酚和萘）的催化裂解和水蒸气重整反应。考察了反应温度和时空对苯酚和萘催化裂解活性的影响，水蒸气对催化剂碳摩尔比（S/C）的影响以及不同合成方法对苯酚和萘水蒸气重整反应的影响。此外，使用程序升温氧化（TPO）、拉曼光谱和透射电子显微镜（TEM）方法分析了沉积在催化剂上的碳。采用X射线荧光（XRF）分析了催化剂的元素组成，采用X射线衍射（XRD）、BET比表面积、扫描电子显微镜（SEM）、透射电子显微镜（TEM）、拉曼光谱、程序升温还原（TPR）和X射线光电子能谱（XPS）对催化剂的物化性能进行了表征。结果表明，TF-Ni/Fe/橄榄石复合材料的结构与煅烧后的橄榄石（主要为Mg 2SiO 4相）相比发生了较大的变化，部分Fe融入橄榄石结构并重组为新的（Mg，Fe）Fe 2 O 4相。还原后，两种催化剂上均检测到Ni-Fe合金，TF-Ni/Fe/橄榄石上Ni-Fe合金的粒径小于WI-Ni/Fe/橄榄石。TF-Ni/Fe/橄榄石催化剂可将苯酚裂解为小分子气体（CO和H2）和少量烯烃。相比之下，苯酚在没有催化剂的情况下聚合成萘。WI-Ni/Fe/橄榄石催化剂上苯酚和萘水蒸气重整转化率均高于TF-Ni/Fe/橄榄石催化剂。对TF-Ni/Fe/橄榄石和WI-Ni/Fe/橄榄石催化剂进行了苯酚水蒸气重整反应100 h的稳定性测试，结果表明，TF-Ni/Fe/橄榄石催化剂在反应初期表现出较高的稳定性，这是由于活性中心与橄榄石载体之间的相互作用较强。萘水蒸气重整生成的沉积碳中含有较多的石墨化程度较高的Cβ和Cγ，因而较难脱除。
Ni/Fe bimetallic catalysts were synthesized on an olivine support using the wetness impregnation (WI) and thermal fusion (TF) methods, and catalytic cracking and steam reforming on different tar model compounds (phenol and naphthalene) were investigated in a fixed bed reactor. The effects of the reaction temperature and space-time on the catalytic cracking activity of phenol and naphthalene were tested, and the influences of steam on the carbon molar ratio (S/C) and different synthesized methods on the steam reforming of phenol and naphthalene were also studied. In addition, the carbon deposited on the catalyst was analysed using temperature program oxidation (TPO), Raman spectroscopy and transmission electron microscopy (TEM) methods. The elemental composition of the catalyst was analysed by X-ray fluorescence (XRF), and the physiochemical properties of the catalysts were characterized via X-ray diffraction (XRD), the BET surface area, scanning electron microscopy (SEM), TEM, Raman spectroscopy, temperature program reduction (TPR), and X-ray photoelectron spectroscopy (XPS). The results showed that the structure of TF-Ni/Fe/olivine changed considerably compared with that of calcined olivine (mainly the Mg2SiO4phase) and that a portion of Fe was fused into the olivine structure and reorganized into a new (Mg, Fe) Fe2O4phase. After reduction, the Ni-Fe alloy was detected on both catalysts, and the particle size of the Ni-Fe alloy on TF-Ni/Fe/olivine was smaller than that of WI-Ni/Fe/olivine. The TF-Ni/Fe/olivine cracked phenol into small-molecule gas (CO and H2) and a small quantity of olefin. By contrast, phenol was polymerized to naphthalene in the absence of a catalyst. The phenol and naphthalene steam reforming conversion on WI-Ni/Fe/olivine were both higher than that of TF-Ni/Fe/olivine. A 100-h stability test of phenol steam reforming on TF-Ni/Fe/olivine and WI-Ni/Fe/olivine was conducted, and TF-Ni/Fe/olivine showed higher stability in the early stages of the experiment due to stronger interactions between the active sites and olivine support. The deposited carbon from naphthalene steam reforming was more difficult to eliminate because it contained more Cβand Cγ, which had higher degrees of graphitization.
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