Designing Efficient Single-Atom Alloy Catalysts for Selective C═O Hydrogenation: A First-Principles, Active Learning and Microkinetic Study

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Designing Efficient Single-Atom Alloy Catalysts for Selective C═O Hydrogenation: A First-Principles, Active Learning and Microkinetic Study
Title:
Designing Efficient Single-Atom Alloy Catalysts for Selective C═O Hydrogenation: A First-Principles, Active Learning and Microkinetic Study
Journal Title:
ACS Applied Materials & Interfaces
Keywords:
Publication Date:
24 November 2023
Citation:
Feng, H., Zhang, M., Ge, Z., Deng, Y., Pu, P., Zhou, W., Yuan, H., Yang, J., Li, F., Zhang, X., & Zhang, Y.-W. (2023). Designing Efficient Single-Atom Alloy Catalysts for Selective C═O Hydrogenation: A First-Principles, Active Learning and Microkinetic Study. ACS Applied Materials & Interfaces, 15(48), 55903–55915. https://doi.org/10.1021/acsami.3c15108
Abstract:
Selective hydrogenation of α,β-unsaturated aldehydes into unsaturated alcohols is a process in high demand in organic synthesis, pharmaceuticals, and food production. This process requires the precise hydrogenation of CO bonds, a challenge that requires a tailored catalyst. Single-atom alloys (SAAs), where individual atoms of one metal are distributed in a host metal matrix, offer a potential solution to this challenge. Nevertheless, identifying the appropriate SAA capable of targeted adsorption and the efficient activation of CO bonds remains a substantial hurdle. In this work, we synergistically combine density functional theory (DFT) calculations, active learning, and microkinetic simulations to design SAAs for the efficient and selective hydrogenation of α,β-unsaturated aldehydes. We first comprehensively assessed the potential of 66 SAAs across 264 surfaces (including (100), (110), (111), and (320) crystal planes), to gauge their potential in activating CC and CO bonds. Our assessment unveiled the excellent selectivity of the Ti1Au SAA in activating CO bonds. Moreover, our detailed DFT calculations further demonstrated the high catalytic activity of Ti1Au(320) and Ti1Au(111) surfaces with a low activation energy barrier of only 0.60 eV. Subsequently, we conducted microkinetic simulations on the selective hydrogenation process of crotonaldehyde, by selecting Ti1Au (320) and (111) surfaces as the catalysts and demonstrated that they exhibited a remarkable selectivity and nearly 100% conversion toward crotyl alcohol in the temperature range from 373 to 553 K. The present study not only reveals novel SAAs for targeted hydrogenation of α,β-unsaturated aldehydes but also establishes a promising path toward efficient design of selective hydrogenation catalysts more broadly.
License type:
Publisher Copyright
Funding Info:
This research / project is supported by the A*STAR - SERC Central Research Fund (CRF)
Grant Reference no. : NA

This work was supported by the National Natural Science Foundation of China (22173003), the China Scholarship Council (No. 202206880016), the Italy-Singapore Science and Technology Cooperation (Grant No. R23101R040)
Description:
This document is the Accepted Manuscript version of a Published Work that appeared in final form inACS Applied Materials & Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see doi.org/10.1021/acsami.3c15108
ISSN:
1944-8252
1944-8244
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