Operando spectroscopic monitoring of active species in CO2 hydrogenation at elevated pressure and temperature : steady-state versus transient analysis

Gau, Alina; Hack, Jannis; Maeda, Nobutaka; Meier, Daniel Matthias

doi:10.1021/acs.energyfuels.1c02592

Publication type:	Article in scientific journal
Type of review:	Peer review (publication)
Title:	Operando spectroscopic monitoring of active species in CO2 hydrogenation at elevated pressure and temperature : steady-state versus transient analysis
Authors:	Gau, Alina Hack, Jannis Maeda, Nobutaka Meier, Daniel Matthias
et. al:	No
DOI:	10.1021/acs.energyfuels.1c02592
Published in:	Energy & Fuels
Issue Date:	7-Sep-2021
Publisher / Ed. Institution:	American Chemical Society
ISSN:	0887-0624 1520-5029
Language:	English
Subjects:	Oxides; Inorganic carbon compounds; Alcohols; Infrared spectroscopy; Infrared light
Subject (DDC):	540: Chemistry
Abstract:	Operando infrared spectroscopy is an invaluable tool to provide a deep insight into underlying mechanisms in heterogeneous catalysis. Recent advances in spectroscopic techniques enabled operando analysis under elevated pressure and temperature. In this study we compared a conventional steady-state IR analysis with a transient IR analysis by modulation excitation spectroscopy (MES) using a model reaction, CO2 hydrogenation to methanol at 30 bar and 250 °C. The steady-state IR spectra provide information about surface properties of catalysts while the transient IR spectra are a powerful tool to unveil the kinetics of surface species involved in catalytic cycles and therefore to determine rate-limiting step. Operando MES-IR spectroscopy evidenced that under the reaction conditions (30 bar, 250 °C) hydrogenation of surface methoxy species (CH3O−) is the rate-limiting step for the Cu–Zn based catalyst. We herein demonstrate that comparative analysis of both steady-state and transient spectra at elevated pressure provides a solid understanding of surface processes, allowing a rational catalyst design.
URI:	https://digitalcollection.zhaw.ch/handle/11475/23095
Fulltext version:	Published version
License (according to publishing contract):	Licence according to publishing contract
Departement:	School of Engineering
Organisational Unit:	Institute of Materials and Process Engineering (IMPE)
Appears in collections:	Publikationen School of Engineering

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Gau, A., Hack, J., Maeda, N., & Meier, D. M. (2021). Operando spectroscopic monitoring of active species in CO2 hydrogenation at elevated pressure and temperature : steady-state versus transient analysis. Energy & Fuels. https://doi.org/10.1021/acs.energyfuels.1c02592

Gau, A. et al. (2021) ‘Operando spectroscopic monitoring of active species in CO2 hydrogenation at elevated pressure and temperature : steady-state versus transient analysis’, Energy & Fuels [Preprint]. Available at: https://doi.org/10.1021/acs.energyfuels.1c02592.

A. Gau, J. Hack, N. Maeda, and D. M. Meier, “Operando spectroscopic monitoring of active species in CO2 hydrogenation at elevated pressure and temperature : steady-state versus transient analysis,” Energy & Fuels, Sep. 2021, doi: 10.1021/acs.energyfuels.1c02592.

GAU, Alina, Jannis HACK, Nobutaka MAEDA und Daniel Matthias MEIER, 2021. Operando spectroscopic monitoring of active species in CO2 hydrogenation at elevated pressure and temperature : steady-state versus transient analysis. Energy & Fuels. 7 September 2021. DOI 10.1021/acs.energyfuels.1c02592

Gau, Alina, Jannis Hack, Nobutaka Maeda, and Daniel Matthias Meier. 2021. “Operando Spectroscopic Monitoring of Active Species in CO2 Hydrogenation at Elevated Pressure and Temperature : Steady-State versus Transient Analysis.” Energy & Fuels, September. https://doi.org/10.1021/acs.energyfuels.1c02592.

Gau, Alina, et al. “Operando Spectroscopic Monitoring of Active Species in CO2 Hydrogenation at Elevated Pressure and Temperature : Steady-State versus Transient Analysis.” Energy & Fuels, Sept. 2021, https://doi.org/10.1021/acs.energyfuels.1c02592.