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Towards a feasible and stable thermocatalytic conversion of CO2 to methanol and E-fuels

Problem statement

Unarguably, CO2 is a crucial concern affecting climate change. To cope with or solve the issue, viable valorization strategies are required for efficient usage of CO2, allowing for a circular economy. We aim to convert CO2 into CO, methane, methanol, dimethyl ether, or E-fuels.

Our activities in CO2 conversion are related to (i) analyzing the stability of industrially relevant catalysts under realistic conditions and (ii) developing new catalytic materials based on Cu. In (i), we are developing reactors that augment the kinetic information: (a) in situ and operando spectroscopic reactors that work under (close to) working conditions to study structure-performance relationships, (b) periodic reactors with transient or variable conditions over time or space. In (ii), we work mainly with novel materials such as metal-organic frameworks (MOFs).

We guide the design of these catalysts based on stability and using density functional theory (DFT) and microkinetic modeling.

Goals

  • Develop advanced structure-function-deactivation relationships of industrially relevant catalysts
  • Analyze the effect of “activity modifiers,” such as sulfur species, aromatics, chlorine, etc., on the catalyst structure and performance
  • Improve the catalyst structure-function correlations using in-situ, operando, and dynamic techniques and reactors
  • Synthesize new catalytic materials with enhanced stability and selectivity
  • Develop a microkinetic-based modeling framework to analyze the catalyst performance
CO2-2023

Related People

Juan David Trueba
Vijay V. Kumar

Related Publications

Copper nanoparticles encapsulated in zeolitic imidazolate framework-8 as a stable and selective CO2 hydrogenation catalyst

by Velisoju, Cerrillo, Ahmad, Mohamed, Yerrayya, Cheng, Yao, Zheng, Shekhah, Telalovic, Narciso, Cavallo, Eddaoudi, Ramos-Fernandez, Castaño
Nature Comm. Year: 2024 DOI: https://doi.org/10.1038/s41467-024-46388-4

Abstract

Metal–organic frameworks have drawn attention as potential catalysts owing to their unique tunable surface chemistry and accessibility. However, their application in thermal catalysis has been limited because of their instability under harsh temperatures and pressures, such as the hydrogenation of CO2 to methanol. Herein, we use a controlled two-step method to synthesize finely dispersed Cu on a zeolitic imidazolate framework-8 (ZIF-8). This catalyst suffers a series of transformations during the CO2 hydrogenation to methanol, leading to ~14 nm Cu nanoparticles encapsulated on the Zn-based MOF that are highly active (2-fold higher methanol productivity than the commercial Cu–Zn–Al catalyst), very selective (>90%), and remarkably stable for over 150 h. In situ spectroscopy, density functional theory calculations, and kinetic results reveal the preferential adsorption sites, the preferential reaction pathways, and the reverse water gas shift reaction suppression over this catalyst. The developed material is robust, easy to synthesize, and active for CO2 utilization.

Keywords

CO2 HCE