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利用 Pd-AlO 活化生物炭催化剂从木质素中选择性解聚形成单体酚类化合物的反应机理。

Unraveling the reaction mechanism of selective C9 monomeric phenols formation from lignin using Pd-AlO-activated biochar catalyst.

机构信息

Department of Chemical Engineering and National Center for Combustion Research and Development, Indian Institute of Technology Madras, Chennai 600036, India.

Multiscale Reaction Engineering, KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia.

出版信息

Bioresour Technol. 2022 Jan;344(Pt B):126204. doi: 10.1016/j.biortech.2021.126204. Epub 2021 Oct 25.

DOI:10.1016/j.biortech.2021.126204
PMID:34710595
Abstract

The conversion of biomass-derived lignin to valuable monomeric phenols at high selectivity is of paramount importance for sustainable biorefineries. In this study, a novel Pd-AlO supported on activated biochar catalyst is developed for lignin hydrogenolysis. The catalyst characterization revealed that the (111) planes of both of Pd and AlO were exposed to the surface. The maximum lignin conversion of 70.4% along with high liquid yield (∼57 wt%) was obtained at 240 °C, 3 h and 3 MPa H pressure. The total monomeric phenols yield in the liquid was 51.6 wt%, out of which C9 monomeric guaiacols constituted ∼ 30.0 wt% with 38.0% selectivity to 4-propyl guaiacol. Using the reaction intermediate, coniferyl alcohol, chemoselective hydrogenation of C=C is proved to occur over the Pd site, while dehydroxylation of C-OH is shown to occur over the alumina site. An impressive carbon atom economy of 60% was achieved for the production of monomeric phenols.

摘要

将生物质衍生木质素高选择性地转化为有价值的单体酚对于可持续的生物精炼厂至关重要。在这项研究中,开发了一种新型的 Pd-AlO 负载在活性生物炭催化剂上,用于木质素加氢解。催化剂表征表明,Pd 和 AlO 的(111)面都暴露在表面上。在 240°C、3 h 和 3 MPa H 压力下,木质素的最大转化率为 70.4%,液体收率(约 57wt%)较高。液体中的总单体酚收率为 51.6wt%,其中 C9 单体愈创木酚占约 30.0wt%,对 4-丙基愈创木酚的选择性为 38.0%。使用反应中间体松柏醇,证明 C=C 的化学选择性加氢发生在 Pd 位上,而 C-OH 的脱羟反应发生在氧化铝位上。对于单体酚的生产,实现了令人印象深刻的 60%的碳原子经济性。

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