Water Splitting Integrated with Self-Transfer Hydrogenolysis for Efficient Demethoxylation of Guaiacols to Phenols over the Ni/MgO Catalyst

氢解 催化作用 加氢脱氧 愈创木酚 化学 产量(工程) 水溶液 木质素 酚类 苯酚 双水相体系 化学工程 有机化学 选择性 无机化学 材料科学 工程类 冶金
作者
Xiaohong Ren,Qiang Qian,Zhuohua Sun,Ting Wei,Xiaoqiang Yu,Zeming Rong,Changzhi Li
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:14 (7): 5247-5259 被引量:11
标识
DOI:10.1021/acscatal.4c00038
摘要

This work demonstrates the upgrading of lignin-derived monomers through a cascade demethoxylation, aqueous-phase reforming reaction, eliminating the need for external hydrogen supply. The core of this research lies in the use of neat water as both reaction medium and the hydrogen donor over a multifunctional Ni/MgO catalyst, which is responsible for water splitting, aqueous-phase reforming of in situ generated methanol, and selective cleavage of the C–O bond, finally establishing an efficient one-pot approach achieving a high yield of phenols. Reaction mechanism studies proved that the initial H* source came from water by its splitting on the surface of the Ni/MgO catalyst, which triggered the fracture of the aromatic ether bond to afford phenols and CH3O*. The subsequent aqueous-phase reforming of CH3O* and OH* generated more hydrogen and further accelerated the hydrodeoxygenation (HDO) process. A high conversion of 87.8% with a selectivity of 88.9% for phenol could be achieved at 190 °C from guaiacol. Thanks to the interesting water-splitting mechanisms and strong metal–support interaction (SMSI), Ni/MgO exhibited significantly enhanced stability compared to the previously reported nanoporous Ni catalysts. Further, with real lignin as the substrate, 16.3 wt % combined yield of phenol and 4-methylphenol could be acquired under optimized conditions. Overall, this "H2-free" approach offers a promising alternative to conventional biorefinery processes, addressing the challenges of hydrogen sourcing and economic feasibility.
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