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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

Engineering the TiOx Overlayer on Ni Catalyst to Balance Conversion and Stability for Methane Dry-CO2 Reforming

by Bai, Yao, Cheng, Mohamed, Telalovic, Melinte, Emwas, Gascon
ACS Sustainable Chem. Eng. Year: 2024 DOI: https://doi.org/10.1021/acssuschemeng.3c07051

Abstract

Ni-supported catalyst is a viable system to convert methane and carbon dioxide into syngas through methane dry reforming, with the main drawbacks of its fast deactivation being sintering and coking. Here, we developed methods to engineer a TiOx overlayer on Ni/TiO2 catalysts to shield the catalyst against sintering and coking while preserving the Ni accessibility and, thus, conversion. These methods involved altering TiO2crystal phases, pretreatment, and reaction conditions in the reforming stage. Through characterization, testing, and operando spectroscopy, we found that the TiOx overlayer with incomplete Ni coverage maintained a balanced conversion and stability by quenching the sintering and coking. Conversely, thick or nonexistent overlayers led to lower conversions or faster deactivation. The formation of TiOx overlayer increased the CO2activation capacity and oxygen mobility and protected Ni from sintering by its shield function. At the same time, the reaction pathways remained unchanged despite the TiOx overlayer with different morphologies.

Keywords

CHA HCE