Deciphering Particle Morphology Effects in Cinnamaldehyde Hydrogenation over Palladium Nanostructures

IF 4.3 Q2 ENGINEERING, CHEMICAL

ACS Engineering Au Pub Date : 2023-09-08 DOI:10.1021/acsengineeringau.3c00017

Govind Porwal, Haseena K V, S. Sreedhala, Tuhin Suvra Khan, M. Ali Haider* and C. P. Vinod*,

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Abstract

Chemoselective hydrogenation of α-β unsaturated hydrocarbons is a widely studied chemical transformation. In this study, hydrogenation of cinnamaldehyde (CAL) to the corresponding products, viz hydrocinnamaldehyde (HCAL) and hydrocinnamyl alcohol (HCOL) and cinnamyl alcohol (COL), over the different exposed facets of a Pd-based catalyst is studied. The Pd octahedra having (111) facet shows 90% selectivity toward HCAL with 100% conversion in a short duration (45 min). Pd cube having (100) facet shows selectivity (55%) toward HCOL, while Pd spheres show initial selectivity toward HCAL but to HCOL over a prolonged reaction period. The experimental results are corroborated by density functional theory (DFT) calculations, wherein we observe a lower activation barrier E_a = 51 kJ/mol for HCAL formation on the Pd(111) surface. However, an alternative route through the COL intermediate is more prominent on the Pd(100) surface.

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肉桂醛加氢对钯纳米结构的解译粒子形态影响

α-β不饱和碳氢化合物的化学选择性氢化是一种广泛研究的化学变化。本研究对肉桂醛（CAL）在钯基催化剂的不同暴露面上加氢生成相应产物（即氢化肉桂醛（HCAL）、氢化肉桂醇（HCOL）和肉桂醇（COL））的情况进行了研究。具有(111)面的钯八面体对 HCAL 的选择性为 90%，在短时间内（45 分钟）转化率达到 100%。具有 (100) 面的钯立方体对 HCOL 具有 55% 的选择性，而钯球体对 HCAL 具有初始选择性，但在较长的反应时间内对 HCOL 具有选择性。实验结果得到了密度泛函理论（DFT）计算的证实，我们观察到在 Pd(111) 表面形成 HCAL 的活化势垒 Ea = 51 kJ/mol 较低。然而，在 Pd（100）表面，通过 COL 中间体的另一种途径更为突出。

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ACS Engineering Au 化学工程技术-

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期刊介绍：）ACS Engineering Au is an open access journal that reports significant advances in chemical engineering applied chemistry and energy covering fundamentals processes and products. The journal's broad scope includes experimental theoretical mathematical computational chemical and physical research from academic and industrial settings. Short letters comprehensive articles reviews and perspectives are welcome on topics that include:Fundamental research in such areas as thermodynamics transport phenomena (flow mixing mass & heat transfer) chemical reaction kinetics and engineering catalysis separations interfacial phenomena and materialsProcess design development and intensification (e.g. process technologies for chemicals and materials synthesis and design methods process intensification multiphase reactors scale-up systems analysis process control data correlation schemes modeling machine learning Artificial Intelligence)Product research and development involving chemical and engineering aspects (e.g. catalysts plastics elastomers fibers adhesives coatings paper membranes lubricants ceramics aerosols fluidic devices intensified process equipment)Energy and fuels (e.g. pre-treatment processing and utilization of renewable energy resources; processing and utilization of fuels; properties and structure or molecular composition of both raw fuels and refined products; fuel cells hydrogen batteries; photochemical fuel and energy production; decarbonization; electrification; microwave; cavitation)Measurement techniques computational models and data on thermo-physical thermodynamic and transport properties of materials and phase equilibrium behaviorNew methods models and tools (e.g. real-time data analytics multi-scale models physics informed machine learning models machine learning enhanced physics-based models soft sensors high-performance computing)