| 助剂对Ni/γ-Al2O3催化剂上多环烃JP-10重整制氢反应性能的影响 |
| Effects of Promoters on Polycyclic Hydrocarbon JP-10 Steam Reforming for Hydrogen Production over Ni/γ-Al2O3 Catalysts |
| 作者 | 单位 | E-mail | | 刘嘉辉 | 西安近代化学研究所, 氟氮化工资源高效开发与利用国家重点实验室, 西安 710065
陕西科技大学化学与化工学院, 西安 710021 | | | 孙道安 | 西安近代化学研究所, 氟氮化工资源高效开发与利用国家重点实验室, 西安 710065 | sundaoan2008@126.com;吕剑，lujian204@263.net | | 李春迎 | 西安近代化学研究所, 氟氮化工资源高效开发与利用国家重点实验室, 西安 710065 | | | 杜咏梅 | 西安近代化学研究所, 氟氮化工资源高效开发与利用国家重点实验室, 西安 710065 | | | 王志轩 | 西安近代化学研究所, 氟氮化工资源高效开发与利用国家重点实验室, 西安 710065 | | | 吕剑 | 西安近代化学研究所, 氟氮化工资源高效开发与利用国家重点实验室, 西安 710065 | lujian204@263.net |
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| 摘要: 采用等体积浸渍法制备了碱金属Na、碱土金属Mg以及稀土金属Ce改性的15% Ni-5% M/γ-Al2O3镍基负载型催化剂(标记为NMA，M=Na、Mg、Ce)。通过XRD (X射线衍射)、N2吸附-脱附、H2-TPR (H2-程序升温还原)、TEM (透射电镜)、NH3-TPD (NH3-程序升温脱附)、TG (热重)和拉曼光谱技术对催化剂的物相、织构、表面性质等进行了表征分析，并在微通道反应器内研究了多环烃挂式四氢双环戊二烯(JP-10)催化重整制氢性能。结果表明，不同助剂的加入均在一定程度上提高了Ni/γ-Al2O3(NA)催化剂的活性和抗积碳性能。其中，NNaA催化剂的表面活性镍物种的浓度最高，颗粒尺寸最小，且其表面总酸量较低，在高温重整反应中对活性组分镍的抑制聚集作用最为明显，从而使其获得最佳的改性效果。在常压、750℃、水碳比(S/C)为2.4、重时空速(WHSV)为472 h-1条件下，NNaA催化剂上JP-10的转化率和H2选择性分别可达82.9%和73.3%，而积碳量仅为0.53 mg·gfeed-1。反应后该催化剂的积碳多为丝状碳，而其他催化剂的积碳多为无定形碳。 |
| 关键词: 多环烃 催化重整 助剂 改性 制氢 |
| 基金项目: 国家自然科学基金(No.21905222)资助。 |
| Abstract: A series of 15%Ni-5%M/γ-Al2O3 catalysts (denoted as NMA, M=Na, Mg, Ce) modified by Alkali metal Na, alkaline-earth metal Mg, and rare earth metal Ce promoters were prepared by the incipient-wetness co-impregnation method. The texture and surface properties of the above catalysts were characterized and analyzed by XRD (X-ray diffraction), N2 adsorption-desorption, H2-TPR (H2-programmed temperature reduction), TEM (transmission electron microscope), NH3-TPD (NH3-programmed temperature desorption), TG (thermogravimetric), and Raman spectrum techniques. Effects of these promoters on the catalytic performance for steam reforming of JP-10 as a representative of polycyclic hydrocarbons were investigated in a micro-channel reactor (length: 300 mm, inner diameter: 4 mm, 304 stainless steel) wash-coated by catalyst slurry from 600 to 750 ℃ with the feeds of exo-tetrahydrodicyclopentadienew (JP-10) (0.5 mL·min-1) and deionized water (1.5 mL·min-1). The above catalyst slurry was prepared by fast ball-milling of catalyst powder, deionized water, 25% silica sol binder for 0.5 h, and the resulted catalyst loading was about 0.25 g. The results showed that all the promoters significantly improved the catalytic activity of Ni/γ-Al 2O3 catalysts (denoted as NA) and carbon deposition resistance. Among them, the alkali metal promoter Na exhibited the best modification effect overall. It not only reduced the size of nickel grains and total acid amount, improved the dispersibility of nickel active components, and reduced property, but also inhibited the accumulation of nickel in the high-temperature reforming reaction to the maximum extent. Specifically, conversion of JP-10 and H2 selectivity of NNaA catalyst could reach 82.9% and 73.3%, respectively, and the carbon formation was as low as 0.53 mg· gfeed-1 under the reaction conditions of normal pressure, 750 ℃ , steam/carbon (S/C) molar ratio of 2.4, and weight hourly space velocity (WHSV) of 472 h-1. After the reaction, most filamentous carbons were observed on catalysts NNaA, while carbon deposits on the other catalysts were mostly amorphous carbons. |
| Keywords: polycyclic hydrocarbon catalytic reforming promoter modification hydrogen production |
| 投稿时间：2022-06-04 修订日期：2022-08-29 |
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| 刘嘉辉,孙道安,李春迎,杜咏梅,王志轩,吕剑.助剂对Ni/γ-Al2O3催化剂上多环烃JP-10重整制氢反应性能的影响[J].无机化学学报,2022,38(12):2412-2422. |
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