催化学报

催化学报 ›› 2012, Vol. 33 ›› Issue (12): 1938-1944.DOI: 10.1016/S1872-2067(11)60460-9

• 研究论文 • 上一篇    下一篇

铁镍磷化物催化剂在 CO 加氢制低碳醇反应的应用

宋宪根1,3, 丁云杰1,2,*, 陈维苗1, 董文达1,3, 裴彦鹏1,3, 臧 娟1,3, 严丽1, 吕元1   

  1. 1Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, Liaoning, China; 2State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China; 3Graduate University of Chinese Academy of Sciences, Beijing 100049, China
  • 收稿日期:2012-09-10 修回日期:2012-10-08 出版日期:2013-01-18 发布日期:2012-12-18

Synthesis of Mixed Alcohols from CO Hydrogenation over Iron and Nickel Metal Phosphide Catalysts

SONG Xiangen1,3, DING Yunjie1,2,*, CHEN Weimiao1, DONG Wenda1,3, PEI Yanpeng1,3, ZANG Juan1,3, YAN Li1, LÜ Yuan1   

  1. 1Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, Liaoning, China; 2State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China; 3Graduate University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2012-09-10 Revised:2012-10-08 Online:2013-01-18 Published:2012-12-18

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摘要： 通过程序升温还原法制备了一系列氧化硅负载的不同 P/M (M = Fe 和 Ni) 摩尔比的金属磷化物催化剂, 在 553 K, 5.0 MPa 和 H2:CO = 2 (摩尔比) 的反应条件下用固定床反应器测试了它们催化 CO 加氢反应性能. 结果表明, 在 FePx/SiO2 (x 为 P/M 摩尔比) 催化剂上, 液相产物是以甲醇为主的低碳含氧化物的混合物. 而在 NiPx/SiO2 催化剂上, 气态产物主要为甲烷, 液相产物绝大多数是甲醇. 表征结果表明, 磷化物催化剂上的 Fe2P, Fe3P, Ni, Ni2P, Ni3P 和 Ni12P5 晶相在反应条件下是稳定的, 没有形成磷化物的金属铁, 在反应后转变成碳化铁晶相.

关键词: 一氧化碳, 加氢, 含氧化物, 金属磷化物, 磷化铁, 磷化镍, 氧化硅

Abstract: A series of silica supported iron and nickel metal phosphides with different molar ratios of P to metal were synthesized by the temperature programmed reduction method. Their catalytic performance for CO hydrogenation in a fixed bed reactor was tested with the conditions of 553 K, 5.0 MPa, and H2:CO = 2 (molar ratio). With the FePx/SiO2 catalysts (x denotes the molar ratio of P to metal), the product was a mixture of oxygenates containing methanol as the major component. With the NiPx/SiO2 samples, the liquid product was mainly methanol. The Fe2P, Fe3P, Ni, Ni2P, Ni3P, and Ni12P5 phases were stable during CO hydrogenation, while most of the metallic Fe phase transformed into iron carbide.

Key words: carbon monoxide hydrogenation, oxygenates, metal phosphides, silica, iron phosphide, nickel phosphide