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负载于HPMoVO耦合Ni/C双功能催化剂上的木质素衍生酚类化合物的高效加氢脱氧反应

Efficient Hydrodeoxygenation of Lignin-Derived Phenolic Compounds over Bifunctional Catalyst Comprising HPMoVO Coupled with Ni/C.

作者信息

Yin Tao, Luo Yang, Singh Chauhan Arvind, Shu Riyang, Tian Zhipeng, Wang Chao, Chen Ying, Kumar Gupta Navneet

机构信息

Guangdong Provincial Key Laboratory of Functional Soft Condensed Matter, School of Materials and Energy, Guangdong University of Technology, Guangzhou, 510006, PR China.

Centre for Sustainable Technologies, Indian Institute of Science, Gulmohar Marg, Mathikere, 560012, Bengaluru, India.

出版信息

Chemphyschem. 2024 Nov 4;25(21):e202400505. doi: 10.1002/cphc.202400505. Epub 2024 Sep 9.

Abstract

In the catalytic transformation of bio-oil into liquid fuels having alkanes via hydrodeoxygenation (HDO), the acid and metal sites in the catalyst are pivotal for promoting the HDO of lignin-derived phenolic compounds. This study introduces a novel bifunctional catalyst comprising phosphomolybdenum-vanadium heteropolyacids (HPMoVO) coupled with Ni/C. The HDO reaction of the model compound guaiacol was carried out under reaction conditions of 230 °C, revealing the superior performance of HPMoVO with Ni/C catalysts compared to the conventional acids, even at low dosage. The Keggin structure of HPMoVO provided a solid catalyst with strong acidic and redox properties, alongside advantages such as ease of synthesis, cost-effectiveness, and tunable acid and redox properties at the molecular level. Characterization of Ni/C and the prepared acid demonstrated favorable pore structure with a mesopore volume of 0.281 cm/g and an average pore size of 3.404 nm, facilitating uniform distribution and catalytic activity of Ni-metal. Incorporating acid enhances the acidic sites, fostering synergistic interactions between metal and acidic sites within the catalyst, thereby significantly enhancing HDO performance. Guaiacol conversion at 230 °C reached 100 %, with a cyclohexane selectivity of 89.3 %. This study offers a promising avenue for the conversion and upgrading of lignin-derived phenolic compounds.

摘要

在通过加氢脱氧(HDO)将生物油催化转化为含有烷烃的液体燃料的过程中,催化剂中的酸性位点和金属位点对于促进木质素衍生的酚类化合物的HDO至关重要。本研究介绍了一种新型双功能催化剂,它由磷钼钒杂多酸(HPMoVO)与Ni/C耦合而成。在230℃的反应条件下进行了模型化合物愈创木酚的HDO反应,结果表明,即使在低用量下,HPMoVO与Ni/C催化剂的性能也优于传统酸。HPMoVO的Keggin结构提供了一种具有强酸性和氧化还原性质的固体催化剂,同时具有易于合成、成本效益高以及在分子水平上可调节酸和氧化还原性质等优点。Ni/C和制备的酸的表征显示出良好的孔结构,中孔体积为0.281 cm/g,平均孔径为3.404 nm,有利于Ni金属的均匀分布和催化活性。引入酸增强了酸性位点,促进了催化剂中金属位点和酸性位点之间的协同相互作用,从而显著提高了HDO性能。在230℃时愈创木酚转化率达到100%,环己烷选择性为89.3%。本研究为木质素衍生的酚类化合物的转化和升级提供了一条有前景的途径。

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