Understanding the Dynamics Governing Electrocatalytic Hydrodeoxygenation of Lignin Bio-Oil to Hydrocarbons

IF 15.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2025-01-21 DOI:10.1021/jacs.4c14254

Jialu Wang, Man Ho Han, Kezia Megagita Gerby Langie, Da Hye Won, Mi-Young Lee, Cheoulwoo Oh, Hyo Sang Jeon, Jai Hyun Koh, Hyung-Suk Oh, Dong Ki Lee, Woong Hee Lee

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Abstract

Electrocatalytic hydrodeoxygenation (EHDO) is a promising approach for upgrading biomass-derived bio-oils to sustainable fuels without the use of high-pressure hydrogen gas and elevated temperatures. However, direct EHDO for realistic hydrophobic lignin-based oil production remains challenging. Herein, we discuss the molecular dynamics that govern the EHDO of lignin bio-oil over Pt/C in an acidic electrolyte added with 2-propanol or a surfactant. Excellent conversion (98.1%) and a high yield (79.0%) of hydrogenated products, including 40.5% propyl-cyclohexane, are achieved under ambient temperature and pressure. Experimental results and various investigations on molecular dynamics suggest that EHDO occurs at the water-solvent-catalyst three-phase boundary. Proton transfer significantly influences the current density of EHDO. Factors such as cluster size and vector of lignin-based oil to electrode govern the selectivity and Faradaic efficiency of EHDO. This work advances the understanding of dynamics for EHDO and suggests governing factors to improve it.

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木质素生物油电催化加氢脱氧制烃动力学研究

电催化加氢脱氧（EHDO）是一种很有前途的方法，可以在不使用高压氢气和高温的情况下将生物质衍生的生物油升级为可持续燃料。然而，直接EHDO用于现实的疏水性木质素基石油生产仍然具有挑战性。本文讨论了木质素生物油在加入2-丙醇或表面活性剂的酸性电解质中在Pt/C上的EHDO的分子动力学。在常温常压条件下，反应产物转化率高达98.1%，加氢产物收率高达79.0%，其中丙基环己烷的收率为40.5%。实验结果和各种分子动力学研究表明，EHDO发生在水-溶剂-催化剂三相边界。质子转移对EHDO的电流密度有显著影响。聚类大小和木质素基油电极载体等因素决定了EHDO的选择性和法拉第效率。这项工作促进了对EHDO动力学的理解，并提出了改善EHDO的控制因素。

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来源期刊

Journal of the American Chemical Society 化学-化学综合

CiteScore

24.40

自引率

6.00%

发文量

2398

审稿时长

1.6 months

期刊介绍： The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.