Hydrogenation of CO2 to synthetic natural gas (SNG) with 100% selectivity over a Ni–ZnO–MgO catalyst†

IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Mahendra Kumar Meena, Shalini Biswas and Prakash Biswas
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引用次数: 0

Abstract

The CO2 hydrogenation activity of a Ni–ZnO–MgO catalyst prepared by the co-precipitation technique is evaluated in a down-flow tubular reactor. The physicochemical properties of the catalyst were characterized by various techniques, including N2-physisorption, X-ray diffraction (XRD), temperature-programmed reduction (TPR), temperature-programmed desorption (TPD), hydrogen chemisorption, FE-SEM, TGA, TEM, XPS, etc. Hydrogenation experiments were performed at different temperatures (200–400 °C) and mild pressure (1–15 bar) at a constant feed gas (H2/CO2/N2) molar ratio of 3 : 1 : 3. The total feed flow rate was maintained at 3 × 10−3 mol min−1. Results demonstrated that the Ni–ZnO–MgO catalyst was ∼100% selective to CH4. ZnO helped to improve not only the catalyst stability via hydrogen spillover effect but also the nickel metal dispersion, and MgO enhanced the CO2 adsorption. Overall, the reaction mechanism followed the formate species pathway to obtain almost 100% methane selectivity. Time-on-stream study suggested that the catalyst was stable with negligible carbon formation. The used catalyst characterization results showed that the catalyst morphology remained unchanged before and after the reaction. Therefore, the developed Ni–ZnO–MgO catalyst is very promising for the selective hydrogenation of CO2 to synthetic natural gas (SNG).

在Ni-ZnO-MgO催化剂上以100%选择性加氢CO2制合成天然气(SNG
在下流式管式反应器中对共沉淀法制备的Ni-ZnO-MgO催化剂的CO2加氢活性进行了评价。采用n2物理吸附、x射线衍射(XRD)、程序升温还原(TPR)、程序升温解吸(TPD)、氢化学吸附、FE-SEM、TGA、TEM、XPS等技术表征了催化剂的理化性质。加氢实验在不同温度(200-400℃)和常压(1 - 15 bar)下进行,原料气(H2/CO2/N2)摩尔比为3:1:3。总进料流量维持在3 × 10−3 mol min−1。结果表明,Ni-ZnO-MgO催化剂对CH4的选择性为~ 100%。氧化锌通过氢溢出效应提高了催化剂的稳定性,同时提高了镍的分散性,氧化镁增强了催化剂对CO2的吸附。总体而言,该反应机制遵循甲酸类途径,甲烷选择性接近100%。时间流研究表明,催化剂是稳定的,可以忽略碳的形成。所用催化剂的表征结果表明,反应前后催化剂形态保持不变。因此,所研制的Ni-ZnO-MgO催化剂在CO2选择性加氢制合成天然气(SNG)方面具有广阔的应用前景。
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来源期刊
Reaction Chemistry & Engineering
Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)
CiteScore
6.60
自引率
7.70%
发文量
227
期刊介绍: Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.
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