Dry Reforming of Methane over NiLa-Based Catalysts: Influence of Synthesis Method and Ba Addition on Catalytic Properties and Stability

Ruan Gomes,Milena Santos,Soraia Brandão,Roberto Junior,Cristiane Rodella,Alessandra Beretta,Denilson Costa,Roger Fréty

doi:10.3390/catal9040313

Abstract

CO2 reforming of CH4 to produce CO and H2 is a traditional challenge in catalysis. This area is still very active because of the potentials offered by the combined utilization of two green-house gases. The development of active, stable, and economical catalysts remains a key factor for the exploitation of natural gas (NG) with captured CO2 and biogas to produce chemicals or fuels via syngas. The major issue associated with the dry reforming process is catalyst deactivation by carbon deposition. The development of suitable catalyst formulations is one strategy for the mitigation of coking which becomes especially demanding when noble metal-free catalysts are targeted. In this work NiLa-based catalyst obtained from perovskite precursors La1−xBaxNiO3 (x = 0.0; 0.05; 0.1 and 0.2) and NiO/La2O3 were synthesized, characterized by in situ and operando XRD and tested in the dry reforming of methane. The characterization results showed that the addition of barium promoted BaCO3 segregation and changes in the catalyst structure. This partly affected the activity; however, the incorporation of Ba improved the catalyst resistance to deactivation process. The Ba-containing and Ba-free NiLa-based catalysts performed significantly better than NiO/La2O3 catalysts obtained by wet impregnation.

Highlights

The world energy matrix is essentially based on the use of fossil fuels with an increasing share of natural gas; this factor, together with the improved efficiency of energy conversion systems, has largely contributed in the last 10–15 years to the mitigation of CO2 emissions in the electric power sector worldwide
In order to impact on the CO2 footprint of the chemical and transportation sectors, transition strategies have been developed by oil and energy companies which emphasize the crucial role of a growing exploitation of natural gas (NG) reserves for the production of fuels and chemicals through the indirect conversion into synthesis gas and platform intermediates like methanol [1,2,3,4]
The steam reforming of methane (SRM) is the most widespread industrial process for syngas production with H2 /CO ratio close to 3, which is suitable for the production of fuels such as hydrogen, methanol, dimethyl ether and important chemicals like ammonia [5,6,7]

Summary

Introduction

The world energy matrix is essentially based on the use of fossil fuels with an increasing share of natural gas; this factor, together with the improved efficiency of energy conversion systems, has largely contributed in the last 10–15 years to the mitigation of CO2 emissions in the electric power sector worldwide. In order to impact on the CO2 footprint of the chemical and transportation sectors, transition strategies have been developed by oil and energy companies which emphasize the crucial role of a growing exploitation of NG reserves for the production of fuels and chemicals through the indirect conversion into synthesis gas and platform intermediates like methanol [1,2,3,4]. The steam reforming of methane (SRM) is the most widespread industrial process for syngas production with H2 /CO ratio close to 3, which is suitable for the production of fuels such as hydrogen, methanol, dimethyl ether and important chemicals like ammonia [5,6,7]. DRM represents an interesting solution for exploitation of bio-gas as raw material for the fuel and chemical sectors, alternatively to the more commonly practiced energetic use

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