TY - JOUR
T1 - Atomic-Scale Observation of the Metal–Promoter Interaction in Rh-Based Syngas-Upgrading Catalysts
AU - Huang, Xing
AU - Teschner, Detre
AU - Dimitrakopoulou, Maria
AU - Fedorov, Alexey
AU - Frank, Benjamin
AU - Kraehnert, Ralph
AU - Rosowski, Frank
AU - Kaiser, Harry
AU - Schunk, Stephan
AU - Kuretschka, Christiane
AU - Schlögl, Robert
AU - Willinger, Marc Georg
AU - Trunschke, Annette
N1 - Publisher Copyright:
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2019/6/24
Y1 - 2019/6/24
N2 - The direct conversion of syngas to ethanol, typically using promoted Rh catalysts, is a cornerstone reaction in CO2 utilization and hydrogen storage technologies. A rational catalyst development requires a detailed structural understanding of the activated catalyst and the role of promoters in driving chemoselectivity. Herein, we report a comprehensive atomic-scale study of metal–promoter interactions in silica-supported Rh, Rh–Mn, and Rh–Mn–Fe catalysts by aberration-corrected (AC) TEM. While the catalytic reaction leads to the formation of a Rh carbide phase in the Rh–Mn/SiO2 catalyst, the addition of Fe results in the formation of bimetallic Rh–Fe alloys, which further improves the selectivity and prevents the carbide formation. In all promoted catalysts, Mn is present as an oxide decorating the metal particles. Based on the atomic insight obtained, structural and electronic modifications induced by promoters are revealed and a basis for refined theoretical models is provided.
AB - The direct conversion of syngas to ethanol, typically using promoted Rh catalysts, is a cornerstone reaction in CO2 utilization and hydrogen storage technologies. A rational catalyst development requires a detailed structural understanding of the activated catalyst and the role of promoters in driving chemoselectivity. Herein, we report a comprehensive atomic-scale study of metal–promoter interactions in silica-supported Rh, Rh–Mn, and Rh–Mn–Fe catalysts by aberration-corrected (AC) TEM. While the catalytic reaction leads to the formation of a Rh carbide phase in the Rh–Mn/SiO2 catalyst, the addition of Fe results in the formation of bimetallic Rh–Fe alloys, which further improves the selectivity and prevents the carbide formation. In all promoted catalysts, Mn is present as an oxide decorating the metal particles. Based on the atomic insight obtained, structural and electronic modifications induced by promoters are revealed and a basis for refined theoretical models is provided.
KW - Rh-based catalysts
KW - atomic-scale imaging
KW - heterogeneous catalysis
KW - metal–promoter interaction
KW - syngas-to-ethanol conversion
UR - http://www.scopus.com/inward/record.url?scp=85066491147&partnerID=8YFLogxK
U2 - 10.1002/anie.201902750
DO - 10.1002/anie.201902750
M3 - Article
C2 - 31066962
AN - SCOPUS:85066491147
SN - 1433-7851
VL - 58
SP - 8709
EP - 8713
JO - Angewandte Chemie International Edition in English
JF - Angewandte Chemie International Edition in English
IS - 26
ER -