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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

Simultaneous Modeling of the Kinetics for n-Pentane Cracking and the Deactivation of a HZSM-5 Based Catalyst

by Cordero-Lanzac, Aguayo, Gayubo, Castaño, Bilbao
Chem. Eng. J. Year: 2018

Abstract

A kinetic model for the catalytic cracking of n-pentane over a HZSM-5 zeolite (Si/Al = 15) based catalyst has been proposed. In this model, the kinetic scheme of reactions is based on the paraffin cracking mechanisms and uses lumps (light olefins, light paraffins, C5+ paraffins, aromatics and methane). The reaction steps of the scheme are related with the catalytic cracking routes: protolytic cracking, β-scission, oligomerization-cracking, hydride transfer, olefin condensation and methane formation. In addition, a kinetic deactivation equation has been used for modeling the catalyst deactivation, depending on the coke precursors (light olefins and aromatics) concentration. The catalyst has been prepared by agglomerating the HZSM-5 zeolite with a mesoporous matrix of weak acidity, using pseudoboehmite as a binder. The kinetic runs have been carried out in a fixed bed reactor using the following conditions: 350–550 °C, 1.4 bar, space time up to 1.1 gcat h−1 molC−1 and time on stream up to 15 h. The formation of olefins and aromatics, as well as the catalyst deactivation, are favored at high temperatures. A mathematical methodology based on the Levenberg-Marquardt algorithm has been used for the kinetic parameters estimation. The method has allowed for the simultaneous computing of the kinetic parameters of each step of the reaction scheme and the deactivation kinetics, from the experimental results of evolution with the time on stream of each lump concentration.

Keywords

O2H CHA MKM