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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

Related Publications

Enlarging the Three-Phase Boundary to Raise CO2/CH4 Conversions on Exsolved Ni–Fe Alloy Perovskite Catalysts by Minimal Rh Doping

by Yao, Cheng, Bai, Davaasuren, Melinte, Morlanes, Cerrillo, Velisoju, Kolubah, Zheng, Han, Bakr, Gascon, Mohamed, Castaño
ACS Catal. Year: 2024 DOI: https://doi.org/10.1021/acscatal.4c00151

Abstract

Exsolved Ni–Fe alloy perovskite catalysts exhibit remarkable coking resistance during C–H and C–O activation. However, metallic utilization is typically incomplete, resulting in relatively low catalytic activity. Herein, we investigated minimal doping with Rh to boost the catalytic activity in the dry reforming of methane by promoting exsolution and enlargement of the three-phase boundary between the alloy, support, and reactants. The Rh influences the formation of the Ni–Fe alloy, as revealed by X-ray diffraction, and promotes the individual and collective CH4 and CO2 conversions, as revealed by packed bed reactor runs, temperature-programmed surface reactions, and in situ infrared spectroscopy. A minimal 0.21 wt % Rh addition enlarges the three-phase boundary while improving oxygen mobility and storage. The oxygen mobility is responsible for promoting CH4dissociation and dynamic removal of carbon-containing intermediates, such that the catalyst remains stable for over 100 h under both 1 and 14 bar.

Keywords

CRE CHA