表面活性剂辅助共沉淀法制备Ni-Mg-Al固体碱催化剂用于CH4-CO2重整反应

doi:10.1016/S1872-2067(14)60171-6

催化学报 ›› 2014, Vol. 35 ›› Issue (12): 1955-1971.DOI: 10.1016/S1872-2067(14)60171-6

表面活性剂辅助共沉淀法制备Ni-Mg-Al固体碱催化剂用于CH₄-CO₂重整反应

谭鹏甲^a,b, 高志华^a, 沈朝峰^c, 杜亚丽^a, 李晓东^a, 黄伟^a

a. 太原理工大学煤科学与技术教育部和山西省重点实验室, 山西太原030024;
b. 中国航天科工集团第六研究院389厂, 内蒙古呼和浩特010010;
c. 华电电力科学研究院, 浙江杭州310027

收稿日期:2014-04-27 修回日期:2014-07-01 出版日期:2014-11-29 发布日期:2014-11-29
通讯作者: 黄伟, 高志华
基金资助:
国家高技术研究发展计划(863计划, 2013AA051201).

Ni-Mg-Al solid basic layered double oxide catalysts prepared using surfactant-assisted coprecipitation method for CO₂ reforming of CH₄

Pengjia Tan^a,b, Zhihua Gao^a, Chaofeng Shen^c, Yali Du^a, Xiaodong Li^a, Wei Huang^a

a. Key Laboratory of Coal Science and Technology, Ministry of Education of China and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China;
b. The 389 Plant of the Sixth Academy of China Aerospace Science & Industry Corporation, Hohhot 010010, Inner Mongolia, China;
c. Huadian Electric Power Research Institute, Hangzhou 310027, Zhejiang, China

Received:2014-04-27 Revised:2014-07-01 Online:2014-11-29 Published:2014-11-29
Supported by:
This work was supported by the National High Technology Research and Development Program of China (863 Program, 2013AA051201).

摘要/Abstract

摘要：

采用表面活性剂辅助共沉淀法制备了Ni-Mg-Al固体碱催化剂并用于CH₄-CO₂重整反应, 探讨了表面活性剂对Ni(111), Ni(200)晶面的择优取向作用, 在800 ℃下比较了不同表面活性剂制备的催化剂的催化性能, 详细考察了CTAB制备的催化剂CB-LDO在不同反应温度下的催化活性和稳定性.采用红外光谱、X射线衍射、程序升温还原、X射线光电子能谱、高分辨透射电镜和程序升温氧化等表征手段分析了催化剂的活性、稳定性和失活原因.结果表明, 四丙基氢氧化铵(TPAOH)促进Ni(200)的生长, 而聚氧乙烯-聚氧丙烯-聚氧乙烯(P123)、聚乙烯吡咯烷酮(PVP)和十六烷基三甲基溴化铵(CTAB)抑制Ni(200)晶面的生长;Ni(200)的结晶程度对CH₄的活化起到关键的作用, 催化剂CB-LDO在高温下反应会发生晶型的转化, Ni(200)晶面由于反应过程中生成NiAl₂O₄尖晶石而得到缓慢释放, 使催化剂的活性得以维持较高的水平.

关键词: 表面活性剂, 共沉淀法, 镍, 镁铝氧化物, 甲烷, 二氧化碳, 重整

Abstract:

Ni-Mg-Al solid basic catalysts for CO₂ reforming of CH₄ were prepared using a surfactant-assisted coprecipitation method. The preferred orientations of the surfactants on the Ni(111) and Ni(200) crystal planes were investigated. The catalytic performance of the surfactant-modified catalysts was tested at 800 ℃. The cetyltrimethylammonium bromide (CTAB)-modified catalyst (CB-LDO; LDO = layered double oxide) was further studied at various reaction temperatures. All the catalysts were characterized using Fourier-transform infrared spectroscopy, X-ray diffraction, temperature- programmed reduction, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy, and temperature-programmed oxidation. The results show that growth of the Ni(200) plane is promoted by tetrapropylammonium hydroxide and restrained by P123, PVP, and CTAB. The crystallinity degree of Ni(200) plays a key role in the activation of CH₄. The CB-LDO catalysts retain high activities and stabilities, because of the crystal phase transformation at high temperature during the reaction; this leads to the formation of spinel NiAl₂O₄ and exposure of the Ni(200) crystal plane.

Key words: Surfactant, Coprecipitation method, Nickel, Magnesium aluminum oxide, Methane, Carbon dioxide, Reforming

谭鹏甲, 高志华, 沈朝峰, 杜亚丽, 李晓东, 黄伟. 表面活性剂辅助共沉淀法制备Ni-Mg-Al固体碱催化剂用于CH₄-CO₂重整反应[J]. 催化学报, 2014, 35(12): 1955-1971.

Pengjia Tan, Zhihua Gao, Chaofeng Shen, Yali Du, Xiaodong Li, Wei Huang. Ni-Mg-Al solid basic layered double oxide catalysts prepared using surfactant-assisted coprecipitation method for CO₂ reforming of CH₄[J]. Chinese Journal of Catalysis, 2014, 35(12): 1955-1971.

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表面活性剂辅助共沉淀法制备Ni-Mg-Al固体碱催化剂用于CH₄-CO₂重整反应

Ni-Mg-Al solid basic layered double oxide catalysts prepared using surfactant-assisted coprecipitation method for CO₂ reforming of CH₄

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