Gao Zhuoyou, Wang Mengying, Shang Ningzhao, Gao Wei, Cheng Xiang, Gao Shutao, Gao Yongjun, Wang Chun
College of Science, Hebei Agricultural University, Baoding 071001, China.
College of Chemical and Environmental Science, Hebei University, Baoding 071000, China.
Dalton Trans. 2023 Aug 15;52(32):11076-11084. doi: 10.1039/d3dt01819a.
Hydrodeoxygenation (HDO) is an indispensable approach to produce renewable biofuels and value-added chemicals using natural biomass and its derivatives. 2,5-Dimethylfuran (DMF) is considered to be a very promising liquid biofuel, and it can be fabricated by HDO of the biomass derivative 5-hydroxymethylfurfural (HMF). Herein, a highly efficient bifunctional catalyst, Co/HAP(Ce), was fabricated by anchoring highly dispersed Co on Ce-doped hydroxyapatite (HAP(Ce)). Co/HAP(Ce) displayed excellent HDO catalytic activity to convert HMF to DMF, and 99% HMF conversion and 96% DMF selectivity can be obtained under 150 °C, 2 MPa H conditions for 5 h. Density functional theory calculations revealed that H can be more easily activated by Co/HAP(Ce). Systematic studies confirmed that the high activity of Co/HAP(Ce) can be ascribed to the desired acid-alkali properties, highly dispersed cobalt species and strong metal-support interactions. This research provides a cost effective approach for designing efficient catalysts for HDO of biomass and its derivatives.
加氢脱氧（HDO）是利用天然生物质及其衍生物生产可再生生物燃料和增值化学品的不可或缺的方法。2,5-二甲基呋喃（DMF）被认为是一种非常有前景的液体生物燃料，它可以通过生物质衍生物5-羟甲基糠醛（HMF）的加氢脱氧反应制备。在此，通过将高度分散的Co锚定在Ce掺杂的羟基磷灰石（HAP（Ce））上制备了一种高效双功能催化剂Co/HAP（Ce）。Co/HAP（Ce）对将HMF转化为DMF表现出优异的加氢脱氧催化活性，在150℃、2MPa氢气条件下反应5小时，可实现99%的HMF转化率和96%的DMF选择性。密度泛函理论计算表明，Co/HAP（Ce）能更轻易地活化氢。系统研究证实，Co/HAP（Ce）的高活性可归因于其理想的酸碱性质、高度分散的钴物种以及强的金属-载体相互作用。该研究为设计用于生物质及其衍生物加氢脱氧的高效催化剂提供了一种经济有效的方法。
