Acetaldehyde is a key chemical intermediate traditionally produced via the ethylene-based Wacker oxidation process, which is both costly and environmentally harmful. Selective oxidation of bioethanol to acetaldehyde offers a greener and more sustainable alternative, yet most reported catalysts struggle with the usual trade-off between activity and selectivity, typically yielding less than 90% acetaldehyde.
Notably, Liu and Hensen demonstrated a specific Au0-Cu+ synergy in the state-of-the-art Au/MgCuCr2O4 catalyst, achieving over 95% AC yield at 250oC with stable performance for over 500 hours (J. Am. Chem. Soc. 2013, 135, 14032; J. Catal. 2015, 331, 138; J. Catal. 2017, 347, 45). Despite this significant step made more than a decade ago, the quest for more efficient, non-toxic catalysts capable of promoting selective ethanol oxidation at lower temperatures remains a major challenge.
Recently, the research team led by Prof. Peng Liu (Huazhong University of Science and Technology) and Prof. Emiel J.M. Hensen (Eindhoven University of Technology) reported significant progress in selective ethanol oxidation. They developed a series of Au/LaMnCuO3 catalysts with varying Mn/Cu ratios, among which the Au/LaMn0.75Cu0.25O3 composition exhibited a pronounced synergistic effect between gold nanoparticles and moderately Cu-doped LaMnO3 perovskite. This synergy enabled efficient ethanol oxidation below 250oC, outperforming the previously benchmarked Au/MgCuCr2O4 catalyst. The findings were published in the Chinese Journal of Catalysis (DOI: 10.1016/S1872-2067(25)64686-9 ).
To improve the efficiency of converting bioethanol into acetaldehyde—a valuable chemical used in plastics and pharmaceuticals, researchers developed a new class of catalysts based on perovskite materials. These supports were synthesized using a sol-gel combustion method and then coated with gold nanoparticles. By adjusting the ratio of manganese to copper in the perovskite structure, the team identified an optimal composition (Au/LaMn0.75Cu0.25O3) that achieved a high acetaldehyde yield of 95% at 225°C and maintained stable performance for 80 hours. Catalysts with higher copper content were less effective, largely because copper tends to lose its active form during the reaction. The improved performance of the optimized catalyst is linked to a cooperative interaction between gold, manganese, and copper ions.
To better understand how these elements work together, the researchers used advanced computational techniques, including density functional theory and microkinetic simulations. These studies revealed that doping copper into the perovskite creates active sites near the gold particles that help activate oxygen and ethanol molecules more efficiently. The optimized catalyst also showed a lower energy barrier for key reaction steps, making the process more efficient. Both experimental and theoretical results highlight the importance of fine-tuning the catalyst composition to achieve better performance.
The results were published in Chinese Journal of Catalysis (DOI: 10.1016/S1872-2067(25)64686-9 )
About the Journal
Chinese Journal of Catalysis is co-sponsored by Dalian Institute of Chemical Physics, Chinese Academy of Sciences and Chinese Chemical Society, and it is currently published by Elsevier group. This monthly journal publishes in English timely contributions of original and rigorously reviewed manuscripts covering all areas of catalysis. The journal publishes Reviews, Accounts, Communications, Articles, Highlights, Perspectives, and Viewpoints of highly scientific values that help understanding and defining of new concepts in both fundamental issues and practical applications of catalysis. Chinese Journal of Catalysis ranks among the top one journals in Applied Chemistry with a current SCI impact factor of 17.7. The Editors-in-Chief are Profs. Can Li and Tao Zhang.
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