Adaptive Catalytic Synthesis of Aromatic and Aliphatic Amines via CO2-Induced Feedback Inhibition Using Standard Hydrogenation Catalysts.
- 1Max Planck Institute for Chemical Energy Conversion, Stiftstraße 34-36, 45470Mülheim an der Ruhr, Germany.
- 2Institute of Technical and Macromolecular Chemistry, RWTH Aachen University, 52074Aachen, Germany.
Abstract
Adaptive catalytic systems, able to adjust or be adjusted reversibly in their performance, are finding increasing interest in science and technology. Yet, their development is currently associated with sophisticated catalyst designs integrating catalytic and stimuli-responsive functions on the same material, limiting scalability and practical application. We now demonstrate adaptive selectivity control over standard heterogeneous catalysts using CO2 as a molecular trigger for catalytic hydrogenation. In particular, quinoline, benzonitrile, and nitroarene derivatives are selectively hydrogenated using a commercial Ru/C catalyst to deliver either fully saturated amine products under H2 or partially saturated products under H2/CO2 as feed gas. The selectivity control through the presence or absence of CO2 has proven fully reversible, rapid, and robust and generalized over ten different commercial metal nanoparticle catalysts. The adaptivity originates from in situ modification of the catalyst surface with formate adducts generated reversibly from CO2 hydrogenation, which is facilitated by the basic amine functionalities of the intermediates or products along the reaction sequence. The synthetic potential of this simple and versatile approach is demonstrated for a wide variety of substrates, enabling the synthesis of aromatic or aliphatic amines found in valuable drug molecules (e.g., aspernigerin, angustureine, and galipinine) and as useful synthons for fine chemicals and pharmaceuticals.
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BibTeX
@article{zhang2026adaptive,
title = {{Adaptive Catalytic Synthesis of Aromatic and Aliphatic Amines via CO2-Induced Feedback Inhibition Using Standard Hydrogenation Catalysts.}},
author = {Yuyan Zhang and Yufei Wu and Bhaskar Paul and Liqun Kang and Zhuo Chen and Feng Chen and Qiming Jin and Thomas Wiegand and Serena DeBeer and Walter Leitner and Alexis Bordet},
journal = {Journal of the American Chemical Society},
year = {2026},
month = oct,
doi = {10.1021/jacs.6c13337},
url = {https://europepmc.org/article/MED/42912290},
note = {CC BY},
}
RIS
TY - JOUR
TI - Adaptive Catalytic Synthesis of Aromatic and Aliphatic Amines via CO2-Induced Feedback Inhibition Using Standard Hydrogenation Catalysts.
AU - Yuyan Zhang
AU - Yufei Wu
AU - Bhaskar Paul
AU - Liqun Kang
AU - Zhuo Chen
AU - Feng Chen
AU - Qiming Jin
AU - Thomas Wiegand
AU - Serena DeBeer
AU - Walter Leitner
AU - Alexis Bordet
PY - 2026
DA - 2026/10/01
JO - Journal of the American Chemical Society
DO - 10.1021/jacs.6c13337
UR - https://europepmc.org/article/MED/42912290
AB - Adaptive catalytic systems, able to adjust or be adjusted reversibly in their performance, are finding increasing interest in science and technology. Yet, their development is currently associated with sophisticated catalyst designs integrating catalytic and stimuli-responsive functions on the same material, limiting scalability and practical application. We now demonstrate adaptive selectivity control over standard heterogeneous catalysts using CO2 as a molecular trigger for catalytic hydrogenation. In particular, quinoline, benzonitrile, and nitroarene derivatives are selectively hydrogenated using a commercial Ru/C catalyst to deliver either fully saturated amine products under H2 or partially saturated products under H2/CO2 as feed gas. The selectivity control through the presence or absence of CO2 has proven fully reversible, rapid, and robust and generalized over ten different commercial metal nanoparticle catalysts. The adaptivity originates from in situ modification of the catalyst surface with formate adducts generated reversibly from CO2 hydrogenation, which is facilitated by the basic amine functionalities of the intermediates or products along the reaction sequence. The synthetic potential of this simple and versatile approach is demonstrated for a wide variety of substrates, enabling the synthesis of aromatic or aliphatic amines found in valuable drug molecules (e.g., aspernigerin, angustureine, and galipinine) and as useful synthons for fine chemicals and pharmaceuticals.
SN - 0002-7863
SN - 1520-5126
ER -