La-Ni-Mo-B非晶态催化剂的制备及其苯酚加氢脱氧催化性能

doi:10.3866/PKU.WHXB201203081

摘要/Abstract

摘要： 以NaBH4为还原剂采用化学还原法制备出La-Ni-Mo-B 非晶态催化剂, 用扫描电子显微镜(SEM)、X射线衍射(XRD)、电感耦合等离子发射光谱(ICP-AES)、X射线光电子能谱(XPS)等手段对催化剂进行表征, 研究了助剂La 对Ni-Mo-B 催化剂催化性能的影响. 结果显示, 加入适量助剂La 能显著减小催化剂粒径, 增加Ni⁰含量, 促进Mo⁶⁺还原生成Mo⁴⁺, 但过量La 会覆盖Ni⁰和Mo⁴⁺的活性位点. 催化剂的高加氢活性主要归因于其非晶态结构和高Ni⁰含量, 高脱氧活性主要归因于其高Mo⁴⁺含量. 在苯酚的加氢脱氧(HDO)反应中, La-Ni-Mo-B非晶态催化剂催化苯酚HDO反应主要按照加氢-氢解的路径进行的, 显著降低了产物中芳烃含量. 通过优化反应条件, 催化苯酚的转化率和脱氧率都可达到99.0%. 高温下La-Ni-Mo-B 非晶态催化剂失活的主要原因是非晶态结构的破坏.

关键词: 非晶态催化剂, La-Ni-Mo-B, 加氢脱氧, 苯酚, 生物油

Abstract: Lanthanum-promoted Ni-Mo-B amorphous catalysts were prepared by chemical reduction of the corresponding metal salts with sodium borohydride aqueous solution. Scanning electron microscopy (SEM), X-ray diffraction (XRD), inductively coupled plasma atomic emission spectrometry (ICP-AES), and X-ray photoelectron spectroscopy (XPS) were used to characterize the resulting materials. Phenol was used as model compound to test the hydrodeoxygenation (HDO) activity of the La-Ni-Mo-B amorphous catalysts. Adding lanthanum could decrease the particle size, increase the content of Ni⁰ and promote the reduction of Mo⁶⁺ to Mo⁴⁺ . But excess lanthanum would cover some of the Ni⁰, and Mo⁴⁺ active sites. The high hydrogenation activity was attributed to the amorphous structure of the catalyst and the high content of Ni⁰ and the high degree of deoxygenation was attributed to the high content of MoO₂. The HDO reation of phenol on the La-Ni-Mo-B amorphous catalyst proceeded with a hydrogenation-dehydration route, thus decreasing the aromatic content of the HDO products. Both the conversion and the total deoxygenation degree were up to 99.0%. The deactivation of the La-Ni-Mo-B amorphous catalysts during the HDO reation of phenol at high temperature was mainly caused by the crystallization of the amorphous structure.

Key words: Amorphous catalyst, La-Ni-Mo-B, Hydrodeoxygenation, Phenol, Bio-oil

王威燕, 张小哲, 杨运泉, 杨彦松, 彭会左, 罗和安. La-Ni-Mo-B非晶态催化剂的制备及其苯酚加氢脱氧催化性能[J]. 物理化学学报, 2012, 28(05), 1243-1251. doi: 10.3866/PKU.WHXB201203081

WANG Wei-Yan, ZHANG Xiao-Zhe, YANG Yun-Quan, YANG Yan-Song, PENG Hui-Zuo, LUO He-An. Preparation of La-Ni-Mo-B Amorphous Catalyst and Its Catalytic Properties for Hydrodeoxygenation of Phenol[J]. Acta Phys. -Chim. Sin. 2012, 28(05), 1243-1251. doi: 10.3866/PKU.WHXB201203081

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201203081

https://www.whxb.pku.edu.cn/CN/Y2012/V28/I05/1243

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