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Stable catalyst design for the viable activation of methane to syngas, hydrogen, and chemicals

Problem statement

Methane and light alkanes are surplus species and by-products with relatively poor economic interest. Our goal is to activate C–H σ-bond to produce hydrogen, olefins, carbon monoxide, and carbon nanofibers, following different process strategies such as oxidative coupling (for olefins), CO2 dry reforming (for syngas), cracking or catalytic decomposition (for hydrogen-free of COx and sequestrated carbon nanotubes/nanofibers), cracking/co-cracking with CO or methanol. We work on developing, synthesizing, characterizing, and testing innovative catalysts with a twist of reaction engineering concepts, looking at multi-scale implications.

We delve into the mechanistic insights of a series of in-house synthesized metal-supported heterogeneous catalysts by combining them with dynamic reactors and ab initio calculations. We explore catalysts with promoted lifetime, activity, selectivity, and heat exchange.

We investigate novel reactor designs grounded on forced dynamic (operando) fluidized-bed reactors at high pressures to amplify the kinetic information and hydrogen.

Goals

  • Develop a microkinetic-based modeling framework to analyze the catalyst performance
  • Scale the technical catalyst for its application in demanding exothermic (oxidative coupling of methane using SiC and spray drying) or fluidized-bed (catalytic decomposition of methane) conditions
  • Develop new catalytic concepts based on Ni-alloys (Ni-Fe, -Co, -Zn…)
  • Improve the catalyst structure-function correlations using in-situ, operando, and dynamic techniques and reactors
CHA2023

Related People

Xueqin Bai (Bruce)

Related Publications

Assessment of Thermogravimetric Methods for Calculating Coke Combustion-Regeneration Kinetics of Deactivated Catalyst

by Ochoa, Ibarra, Bilbao, Arandes, Castaño
Chem. Eng. Sci. Year: 2017

Abstract

This work compares different methodologies for calculating the kinetic parameters of coke combustion, employed for catalyst regeneration, using thermogravimetric methods. A reference fluid catalytic cracking (FCC) spent catalyst was used as a representative example of the deactivated catalyst for the combustion runs, pre-used in the cracking of a vacuum gas oil at 773 K and 3 s. Three different types of approaches have been performed in order to obtain kinetic combustion parameters: (i) kinetic model-based, (ii) isoconversional and (iii) modulated methods. Additionally, a series of empirical modifications have been proposed to predict the kinetic behavior at different heating rates for the model-based approach. Using the best conditions and methods, the combustion activation energy of coke, deposited after the reaction mentioned, is in the order of ∼114, ∼156, and ∼162 kJ mol−1 for the kinetic model-based, isoconversional and modulated methods, respectively. The recommendations for measuring kinetic parameters are reported together with the benefits/disadvantages using the three mentioned approaches.

Keywords

O2H OLG CHA FCC REF MKM