等离子体还原催化剂在CO2甲烷化反应中的活性

doi:10.7503/cjcu20150948

摘要/Abstract

摘要：

采用浸渍法和原位生长水滑石法制备了Ni-Ce/γ-Al₂O₃和Ni-Ce-LDHs/γ-Al₂O₃ 2种不同类型的催化剂前驱体, 考察了2种前驱体分别经氩-氢等离子体和常规氢热方法还原所得催化剂在CO₂甲烷化反应中的活性. 结果表明, 等离子体还原催化剂的低温活性明显高于常规氢热还原催化剂, 主要表现为前者反应启动的临界温度点比后者低20~30 ℃. 采用X射线衍射(XRD)分析、透射电子显微镜(TEM)、 CO₂程序升温脱附(CO₂-TPD)以及X射线光电子能谱(XPS)对所得催化剂的形貌和结构进行了表征. 结果表明, 等离子体还原催化剂具有较小的活性组分粒径、较高的活性组分分散度以及较高的表面碱性, 这些特性有利于催化剂活性位对CO₂的化学吸附, 使其在甲烷化反应中表现出较好的低温活性.

关键词: 等离子体, 镍, 二氧化碳, 甲烷化, 催化性能

Abstract:

Ni-Ce/γ-Al₂O₃ and Ni-Ce-LDHs/γ-Al₂O₃ catalyst precursors were synthesized by impregnation and in situ chemical-growing methods, respectively. These precursors were reduced by Ar-H₂ cold plasma jet and conventional H₂ thermal reduction. The evaluation of these catalysts were carried out in a CO₂ methanation reaction system. The results showed that the catalysts reduced by plasma had better catalytic activity, the reaction start-temperature with catalysts reduced by plasma was 20—30 ℃ lower than that with catalysts by conventional method. The catalysts were characterized by X-ray diffraction(XRD), transmission electron microscopy(TEM), CO₂-temperature programmed desorption(CO₂-TPD), as well as X-ray photoelectron spectrum(XPS). The results showed that plasma reduction could remarkably improve the dispersion of active components, the alkalinity of support and the size of crystal metal particles. It was these improvements that enhanced the activity of catalysts in methanation reaction.

Key words: Plasma, Nickel, Carbon dioxide, Methanation, Catalytic performance

中图分类号:

O643

TrendMD:

张燕平, 杨春辉, 陈攀, 冉唐春, 李娇, 印永祥. 等离子体还原催化剂在CO₂甲烷化反应中的活性. 高等学校化学学报, 2016, 37(8): 1521.

ZHANG Yanping,YANG Chunhui,CHEN Pan,RAN Tangchun,LI Jiao,YIN Yongxiang. Activity of Catalysts Reduced by Plasma in CO₂ Methanation^†. Chem. J. Chinese Universities, 2016, 37(8): 1521.

图/表 10

Fig.1 Example diagram of free-carbon electricity to chemical energy

Fig.2 Schematic of catalyst reduced with plasma jet

Fig.3 Performance of catalyst LDHs-C-R(a) and LDHs-P-R(b) in CO2 methanation reaction

Fig.4 Performance of catalyst IMPs-C-R(a) and IMPs-P-R(b) in CO2 methanation reaction

Fig.5 Selectivity of catalysts LDHs-C-R and LDHs-P-R(A), IMPs-C-R and IMPs-P-R(B)

Fig.6 XRD patterns of catalysts IMPs(A) and LDHs(B) (A) a. IMPs, b. IMPs-C-R, c. IMPs-P-R; (B) a. LDHs, b. LDHs-C-R, c. LDHs-P-R.

Fig.7 TEM images of catalysts IMPs-C-R(A), IMPs-P-R(B), LDHs-C-R(C) and LDHs-P-R(D)

Fig.8 CO2-TPD profiles of catalysts prepared by different reduction methods (A) a. IMPs-C-R, b. IMPs-P-R; (B) a. LDHs-C-R, b. LDHs-P-R.

Table 1 CO2 desorption peak area over different catalysts

Catalyst	IMPs-C-R	IMPs-P-R	LDHs-C-R	LDHs-P-R
CO₂ desorption peak, β or (β+γ)	4.47	12.81	12.56	19.17

Fig.9 XPS spectra of O1s for catalysts reduced by different methods (A) LDHs-P-R; (B) LDHs-C-R.

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等离子体还原催化剂在CO₂甲烷化反应中的活性

Activity of Catalysts Reduced by Plasma in CO₂ Methanation^†

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