Enhanced Targeted Deoxygenation Catalytic Pyrolysis of Lignin to Aromatic Hydrocarbons over Oxygen Vacancies Pt-MoOx/TiO2

IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL ChemCatChem Pub Date : 2025-02-17 DOI:10.1002/cctc.202401727
Yi Gao, Jiajun Yu, Bo Zhang, Wei Jin, Huiyan Zhang
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Abstract

Catalytic pyrolysis technology has been widely used in the conversion of lignin to aromatics, but the catalysts still suffer from poor stability and low product yields due to the lack of oxygen vacancy design. In this study, we report a multi-active site synergistic strategy to enhance the cleavage of lignin aryl carbon-oxygen bonds. Pt-MoOx/TiO2 has a large specific surface area and pore volume, showing a significant medium mesopore size, which was favorable for trapping macromolecular oxides. Meanwhile, a significant synergistic effect was found between hydrogen-activated metallic Pt and molybdenum oxide, which both inhibited the hydrogenation of the aryl ring and promoted the dissociation of hydrogen, thus providing more active sites. More importantly, the defective oxygen vacancies played a key role in the adsorption and activation of oxygen-containing groups, facilitating the absorption of active hydrogen formed by hydrogen spillover. Under the conditions of atmospheric pressure and 400 °C, the high efficiency conversion (100%) of m-cresol was achieved, and guaranteed a high yield of aromatics (98%) and high selectivity (98%). Extending to lignin, the yield of aromatics can reach 5 wt.%. The catalyst remained highly active after 6 h of continuous operation, and there was no significant decrease in yield after two regenerations.

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氧空位Pt-MoOx/TiO2上木质素定向脱氧催化热解制芳烃的研究
催化热解技术在木质素制芳烃转化中得到了广泛的应用,但由于缺乏氧空位设计,催化剂的稳定性差,产物收率低。在这项研究中,我们报道了一种多活性位点协同策略来增强木质素芳基碳氧键的裂解。Pt-MoOx/TiO2具有较大的比表面积和孔容,具有显著的中等介孔大小,有利于捕获大分子氧化物。同时,氢活化金属Pt与氧化钼之间存在显著的协同作用,既抑制芳基环的加氢,又促进氢的解离,从而提供更多的活性位点。更重要的是,缺陷氧空位对含氧基团的吸附和活化起着关键作用,有利于氢溢出形成的活性氢的吸收。在常压和400℃条件下,间甲酚的转化率达到100%,保证了芳烃收率98%和选择性98%。延伸到木质素,芳香烃的收率可达5 wt.%。催化剂连续运行6 h后仍保持较高的活性,2次再生后收率无明显下降。
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来源期刊
ChemCatChem
ChemCatChem 化学-物理化学
CiteScore
8.10
自引率
4.40%
发文量
511
审稿时长
1.3 months
期刊介绍: With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.
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