无机材料学报 ›› 2020, Vol. 35 ›› Issue (5): 567-572.DOI: 10.15541/jim20190229

• 研究论文 • 上一篇    下一篇

制备方法对Ru/γ-Al2O3与等离子体共活化CO2甲烷化反应的影响

董梦悦,徐卫卫,赵静,底兰波(),张秀玲()   

  1. 大连大学 物理科学与技术学院, 大连 116622
  • 收稿日期:2019-05-15 修回日期:2019-09-12 出版日期:2020-05-20 发布日期:2019-10-23
  • 作者简介:董梦悦(1995-), 女, 硕士研究生. E-mail: dmy_up@sina.com<br/>DONG Mengyue(1995-), female, Master candidate. E-mail: dmy_up@sina.com
  • 基金资助:
    国家自然科学基金(21673026);国家自然科学基金(21773020);大连大学研究生教育教学改革基金

Ru/γ-Al2O3 and Plasma Co-activation for CO2 Methanation: Effect of Catalytic Material Preparation Method

DONG Mengyue,XU Weiwei,ZHAO Jing,DI Lanbo(),ZHANG Xiuling()   

  1. College of Physical Science and Technology, Dalian University, Dalian 116622, China
  • Received:2019-05-15 Revised:2019-09-12 Online:2020-05-20 Published:2019-10-23
  • Supported by:
    National Natural Science Foundation of China(21673026);National Natural Science Foundation of China(21773020);Graduate Education and Teaching Reform Fund of Dalian University

摘要:

等离子体与催化材料协同作用CO2甲烷化反应为CO2再利用提供了可能, 但催化材料的制备方法对其结构和性能有重要影响。本研究以等体积浸渍法制备的Ru/γ-Al2O3为催化材料前驱体, 分别采取H2大气压冷等离子体还原和H2热还原方法制备Ru/γ-Al2O3-P和Ru/γ-Al2O3-T催化材料。考察两种方法制备Ru/γ-Al2O3催化材料与大气压冷等离子体共同作用下CO2甲烷化反应中的催化活性, 并采用不同测试方法研究制备方法对Ru/γ-Al2O3结构的影响, 分析影响Ru/γ-Al2O3催化活性的结构因素, 进而探究了Ru/γ-Al2O3-P和Ru/γ-Al2O3-T催化材料的制备机理。研究结果表明: 载体γ-Al2O3与大气压等离子体共同作用下CO2转化率为24.8%, 主要产物是CO; Ru/γ-Al2O3与大气压等离子体共同作用下的主要产物是甲烷。Ru/γ-Al2O3-T和Ru/γ-Al2O3-P催化材料的CO2转化率分别为66.9%和77.3%。Ru/γ-Al2O3-P较高的催化活性源于其表面Ru还原程度高、Ru/Al原子比高以及Ru单质在载体γ-Al2O3上分散性较好且粒径较小, 说明采用大气压H2冷等离子体技术可制备高活性的负载型金属催化材料。

关键词: Ru/γ-Al2O3, 等离子体还原, 热还原, CO2甲烷化

Abstract:

The synergy of plasma and catalytic materials for CO2 methanation provides the possibility for CO2 reuse. The preparation method of catalytic materials plays an important role on their structure and performance. In this work, Ru/γ-Al2O3-P and Ru/γ-Al2O3-T catalytic materials were prepared by atmospheric-pressure H2 plasma reduction and H2 thermal reduction, respectively, using Ru/γ-Al2O3 precursor prepared by incipient wetness impregnation. The catalytic activity of Ru/γ-Al2O3 prepared by different methods was evaluated during atmospheric-pressure plasma reduction for CO2 methanation reaction. Different techniques were used to investigate the effect of preparation methods on the structure of Ru/γ-Al2O3, analyze the influences of structural factor on the catalytic activity of Ru/γ-Al2O3, and discuss the preparation mechanism of Ru/γ-Al2O3-P and Ru/γ-Al2O3-T. The results show that the CO2 conversion of γ-Al2O3 support is 24.8% under the combination of atmospheric-pressure plasma, and the main product is CO. However, the main CO2 catalytic product of Ru/γ-Al2O3 is methane under the combination of atmospheric-pressure plasma. CO2 conversion over Ru/γ-Al2O3-P is 77.3%, which is higher than that over Ru/γ-Al2O3-T (69.9%). Higher catalytic activity of Ru/γ-Al2O3-P is ascribed to the higher metallic Ru ratio and Ru/Al atomic ratio, as well as the smaller and higher dispersion of Ru nanoparticles. This work proves that highly active supported metal catalytic materials can be prepared by atmospheric-pressure H2 plasma.

Key words: Ru/γ-Al2O3, plasma reduction, thermal reduction, CO2 methanation

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