生物质燃气变换-甲烷化双功能催化剂研究进展

doi:10.16085/j.issn.1000-6613.2019-0122

摘要/Abstract

摘要：

生物质燃气在达到居民使用标准前必须进行提质，变换-甲烷化工艺单元可同时降低CO含量和提高燃气热值，因此研发适合生物质燃气的变换-甲烷化双功能催化剂显得尤为重要。在已广泛研究的单功能水气变换和甲烷化催化剂基础上，近年来国内外对变换-甲烷化双功能催化剂也开展了诸多探究。本文从催化剂组成、制备方法和反应机理三方面对变换-甲烷化双功能催化剂进行了综述，详细介绍了适用于该种催化剂的活性组分、助剂与载体，比较分析了浸渍法、共沉淀法等传统制备方法与火焰喷雾燃烧法、等离子体分解法等新颖制备方法，并对变换-甲烷化双功能催化剂进行了总结和展望，指出未来制备催化剂时助剂可根据具体要求选择性添加，廉价的矿石可替代成为有竞争力的催化剂载体，变换-甲烷指出化机理可借助多种材料表征以及理论计算而获悉。

关键词: 生物质, 燃料, 提质, 一氧化碳, 双功能催化剂

Abstract:

It is essential to upgrade the biogas in order to meet the standard for downstream users. The integrated unit of methanation coupling with water gas shift could simultaneously reduce the CO content and increase the heating value of biogas. As a result, it is crucial to develop the corresponding bifunctional catalysts which can catalyze water gas shift and methanation simultaneously. On the basis of the widely developed catalysts for methanation or water gas shift, the bifunctional catalysts have also been preliminarily investigated. In this paper, the research progress of bifunctional catalysts for methanation coupling with water gas shift is reviewed from three aspects of catalyst composition, preparation method and reaction mechanism. The active metals, promoters and the support of the catalyst are introduced. The traditional preparation methods including impregnation and coprecipitation are compared with some novel methods such as flame combustion and plasma decomposition. Besides, the conclusion and prospect are also made. The promising preparation of the bifunctional catalysts is to selectively add promoters and to utilize cheap minerals as catalyst support. Various characterization techniques and theoretical calculations would be helpful to understand the mechanism of water gas shift coupling with methanation.

Key words: biomass, fuel, upgrade, carbon monoxide, bifunctional catalysts

中图分类号:

O643.3

董新新,金保昇. 生物质燃气变换-甲烷化双功能催化剂研究进展[J]. 化工进展, 2019, 38(12): 5360-5371.

Xinxin DONG,Baosheng JIN. Research progress of bifunctional catalysts for methanation coupling with water gas shift of biogas[J]. Chemical Industry and Engineering Progress, 2019, 38(12): 5360-5371.

图/表 9

表1 MOx-NiO/γ-Al2O3变换-甲烷化催化活性

催化剂	CO转化率（C摩尔分数）/ %	选择性（C摩尔分数）/%
催化剂	CO转化率（C摩尔分数）/ %	CH₄	CO₂
NiO/γ-Al₂O₃	6.4	82.1	9.1
Fe₂O₃-NiO/γ-Al₂O₃	4.8	69.0	18.1
CuO-NiO/γ-Al₂O₃	7.2	82.2	14.5
Co₃O₄-NiO/γ-Al₂O₃	7.8	83.2	12.3

图1 CO在不同Ni-Ru双金属簇的最稳定吸附结构和吸附能

图2 两种催化剂在400℃、H2/CO=3和空速3×104mL/(h·gcat)条件下的CO甲烷化效果

图3 硫化前各催化剂的XRD谱图1—Co/Al; 2—Mo/Al; 3—CoMo/Al; 4—Co-Mo/Al; 5—Mo-Co/Al

图4 稳定性测试后La0.75Ce0.25NiO3/SiO2催化剂中La、Ce和Ni的STEM-EDS图及线扫描分析

图5 Ni@Ru/La2O3-SiO2催化剂结构转化示意图

图6 催化剂焙烧过程相变示意图1—硝酸镍；2—氧化铝；3—无定形氧化镍；4—晶体氧化镍；5—镍铝尖晶石

表2 变换-甲烷化基元反应

序号	基元反应
1	H₂+2* $?$ 2H*
2	CO+* $?$ CO*
3	CO+ $?$ C+O
4	C+H $?$ CH+
5	CH+H $?$ CH₂+ RDS^①
6	CH₂+H $?$ CH₃+
7	CH₃+H $?$ CH₄+2*
8	H₂O+* $?$ H₂+O*
9	CO+O $?$ CO₂+ RDS^①
10	CO₂* $?$ CO₂+*

表2 变换-甲烷化基元反应

序号	基元反应
1	H₂+2* $?$ 2H*
2	CO+* $?$ CO*
3	CO+ $?$ C+O
4	C+H $?$ CH+
5	CH+H $?$ CH₂+ RDS^①
6	CH₂+H $?$ CH₃+
7	CH₃+H $?$ CH₄+2*
8	H₂O+* $?$ H₂+O*
9	CO+O $?$ CO₂+ RDS^①
10	CO₂* $?$ CO₂+*

表3 变换-甲烷化动力学公式参数

常数	参数A	参数B
k₁/mol·Pa^0.5·kg_cat^-1·s^-1	3.711e¹⁷	240100
k₂/mol·Pa^0.5·kg_cat^-1·s^-1	5.431	67130
K_eq1/Pa²	1.198e²³	223064
K_eq2	1.767e^-2	36581
K_CH4/Pa^-1	6.65e^-9	-38280
K_CO/Pa^-1	8.23e^-10	-70650
K_H2/Pa^-1	6.12e^-14	-82900
K_H2O	1.17e⁵	88680

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