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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