Optimization of thermally impregnated Ni–olivine catalysts for tar removal

Optimization of thermally impregnated Ni–olivine catalysts for tar removal
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DOI:
10.1016/j.apcata.2009.04.042
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发表时间:
2009-07
影响因子:
5.5
通讯作者:
Zhongkui Zhao;N. Lakshminarayanan;J. Kuhn;Allyson Senefeld-Naber;L. Felix;R. B. Slimane;Chun-Whan Choi-Chun-Whan
Zhongkui Zhao;N. Lakshminarayanan;J. Kuhn;Allyson Senefeld-Naber;L. Felix;R. B. Slimane;Chun-Whan Choi-Chun-Whan
中科院分区:
化学2区
文献类型:
--
作者:
Zhongkui Zhao;N. Lakshminarayanan;J. Kuhn;Allyson Senefeld-Naber;L. Felix;R. B. Slimane;Chun-Whan Choi-Chun-Whan

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热浸渍镍橄榄石是潜在的催化剂,用于热清除流化床生物质气化炉中产生的焦油。本研究探讨了合成参数的影响,即镍前体,制备温度,和橄榄石载体上的物理化学和催化性能的镍-橄榄石催化剂制备的热浸渍。催化活性和稳定性监测重整萘,模型焦油化合物在模拟生物质衍生的合成气和重整甲烷。物理化学性质,其中包括结构(XRD,TPR,和拉曼光谱)和表面测量(BET表面积和XPS),评价新鲜和废催化剂。镍前体(NiO或Ni)的选择表现出最小的影响,对萘和甲烷水蒸气重整的物理化学性质和催化活性和稳定性。然而,合成温度(1100和1400°C)和橄榄石载体确实有影响。当使用较低的合成温度时,观察到大的结构变化和失活,这表明该制剂是不期望的。使用华盛顿橄榄石作为载体证明了与两种其他橄榄石载体相比改进的催化性能和稳定性,并且进一步表征表明处理在确定最终结构特征中是重要的。
Thermally impregnated Ni–olivines are potential catalysts for hot cleanup of tars generated in fluidized bed biomass gasifiers. The present study examined the influence of synthesis parameters, namely Ni precursor, preparation temperature, and olivine support upon the physiochemical and catalytic properties of Ni–olivine catalysts prepared by thermal impregnation. Catalytic activity and stability was monitored by reforming naphthalene, a model tar compound in simulated biomass-derived syngas and by reforming methane. Physiochemical properties, which include both structural (XRD, TPR, and Raman spectroscopy) and surface measurements (BET surface area and XPS), were evaluated for both fresh and spent catalysts. Choice of Ni precursor (NiO or Ni) demonstrated minimal influence upon physiochemical properties and catalytic activity and stability for naphthalene- and methane-steam reforming. The synthesis temperature (1100 and 1400°C) and olivine support, however, did have an impact. Large structural changes and deactivation were observed when lower synthesis temperatures were used, which indicated that this formulation was not desirable. The use of the Washington olivine as the support demonstrated improved catalytic performance and stability compared to two other olivine supports and further characterization showed that treatments are important in determining the final structural features.