Preparation of Cellulose Nanofibers from Corn Stalks by Fenton Reaction: A New Insight into the Mechanism by an Experimental and Theoretical Study

纤维素 催化作用 木质素 吸附 密度泛函理论 化学工程 反应机理 拉曼光谱 化学 纳米纤维 纤维 离子 扫描电子显微镜 材料科学 光化学 物理化学 纳米技术 计算化学 复合材料 有机化学 工程类 物理 光学
作者
Rui-Cheng Qin,Yi-Ying Ma,Dan Wang,Nan-Zhu Bao,Chun‐Guang Liu
出处
期刊:Journal of Agricultural and Food Chemistry [American Chemical Society]
卷期号:71 (4): 1907-1920 被引量:5
标识
DOI:10.1021/acs.jafc.2c08475
摘要

Agricultural biomass wastes are an abundant feedstock for biorefineries. However, most of these wastes are not treated in the right way. Here, corn stalks (CSs) were assigned as the raw material to produce cellulose nanofibers (CNFs) via in situ Fenton oxidation treatment. In order to probe the formation mechanism of an in situ Fenton reactor, the bonding interaction of hydrated Fe2+ ions and fiber has been systemically studied based on adsorption experiments, IR spectroscopy, density functional theory (DFT) calculations, and Raman spectroscopy. The results indicate that the coordination of the hydrated Fe2+ ion to the fiber generates a quasi-octahedral-coordinated sphere around the Fe center. The Jahn-Teller distortion effect of the Fe center promotes the Fe-O2H2 bonding interaction via reduction of the energy gap of the dz2 orbital of the Fe center and π2py/π2pz orbitals of the H2O2 molecule. The oxidation treatment of the pretreated CS by the in situ Fenton process shows the formation of a new carboxyl group on the fiber surface. The scanning electron microscopy image shows that the Fenton-treated fiber was scattered into the nanosized CNFs with a diameter of up to 50 nm. Both experimental and theoretical studies show that the pseudo-first-order kinetic reaction could describe the in situ Fenton kinetics well. Moreover, the proposed catalytic cycle shows that the large thermodynamic barrier is the cleavage of the O-O bond of H2O2 to generate the •OH radical, and the whole catalytic cycle is found to be spontaneous at room temperature.
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