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

巴豆醛 催化作用 选择性 密度泛函理论 材料科学 还原消去 Atom(片上系统) 光化学 计算化学 组合化学 纳米技术 化学 有机化学 计算机科学 嵌入式系统
作者
Haisong Feng,Meng Zhang,Zhen Ge,Yuan Deng,Pengxin Pu,Wenyu Zhou,Hao Yuan,Jing Yang,Feng Li,Xin Zhang,Yong‐Wei Zhang
出处
期刊:ACS Applied Materials & Interfaces [American Chemical Society]
卷期号:15 (48): 55903-55915 被引量:4
标识
DOI:10.1021/acsami.3c15108
摘要

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 C═O 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 C═O 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 C═C and C═O bonds. Our assessment unveiled the excellent selectivity of the Ti1Au SAA in activating C═O 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.
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