期刊
FUEL PROCESSING TECHNOLOGY
卷 253, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.fuproc.2023.108001
关键词
Single -atom alloy; Ni catalyst; DFT and microkinetic modeling; Bio-oil; Hydrodeoxygenation
This study explores the potential application of single-atom-alloy (SAA) catalysts in bio-oils hydrodeoxygenation refining using density functional theory (DFT) and microkinetic modeling. It establishes the relationships between stability, adsorptive properties, and activity structures for bio-oil derivatives, providing guidance for the synthesis of cost-effective SAA combinations.
In the search for sustainable fuels, high-performing, cost-effective, and abundant catalysts are needed for bio-oils hydrodeoxygenation refining, with single-atom-alloy (SAA) catalysts showing potential for outstanding activity and economic bi-metallic assembly. Hydrodeoxygenation upgrading of modelled bio-oil molecules, namely, phenol, anisole, benzaldehyde, and vanillin, has been systematically explored here over a wide-range of SAA Ni (111)-based catalysts (Pd, Pt, Cu, Co, Fe, Ru, Re, Rh, V, W, and Mo) using density functional theory (DFT) and microkinetic modeling. Stability, adsorptive, and activity structural-property-relationships were established for bio-oil derivatives that can direct the synthesis process of cost-effective SAA combinations. DFT revealed the thermodynamic atomic dispersion tendency of the SAA catalysts. Furthermore, the OH*- and O* - induced on the catalyst surface enhanced the SAA upper-layer stability. Single-atoms shifted the d-band center towards the fermi-level in agreement with bio-oils adsorption energies and Caryl - O lengths. The free-energy pathways at 573 K unveiled the SAAs role in lowering the activation barriers, with W-Ni(111) best-performing towards selective phenol and anisole direct deoxygenation, whilst Mo-Ni(111) directs the facile activation of benzaldehyde and vanillin C--O scission. The microkinetic/thermodynamic analysis of O*-poisoning showed that Mo-Ni(111) withstands high O*-coverage, indicative by higher deoxygeneration rates in 350-950 K and greater coverage of the desired product.
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