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Atomic‐Scale Observation of the Metal–Promoter Interaction in Rh‐Based Syngas‐Upgrading Catalysts
Author(s) -
Huang Xing,
Teschner Detre,
Dimitrakopoulou Maria,
Fedorov Alexey,
Frank Benjamin,
Kraehnert Ralph,
Rosowski Frank,
Kaiser Harry,
Schunk Stephan,
Kuretschka Christiane,
Schlögl Robert,
Willinger MarcGeorg,
Trunschke Annette
Publication year - 2019
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201902750
Subject(s) - catalysis , syngas , bimetallic strip , carbide , metal , materials science , rhodium , oxide , atomic units , chemical engineering , chemoselectivity , chemistry , inorganic chemistry , metallurgy , organic chemistry , engineering , physics , quantum mechanics
The direct conversion of syngas to ethanol, typically using promoted Rh catalysts, is a cornerstone reaction in CO 2 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/SiO 2 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.