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Heterogeneous Ni–Ru/H-ZSM-5 one-pot catalytic conversion of lignin into monophenols
Renewable Energy ( IF 9.0 ) Pub Date : 2021-02-13 , DOI: 10.1016/j.renene.2021.01.150
Feng Lin , Yulong Ma , Yonggang Sun , Kanghe Zhao , Tingting Gao , Yingbo Zhu

Due to the inertness and structural complexity of lignin, upgrading lignin to biofuels and fine chemicals still faces great challenges. In this paper, a one-pot method was used to catalyze straw lignin with H-ZSM-5 supported by Ni and Ru bimetals, and the lignin conversion rate reached 88.1%. The yield of monophenol was 19.5%, of which the yield of 4-ethylphenol and 4-ethylguaiacol was 4.9% and 3.8%, respectively. The 2D HSQC NMR analysis confirmed that the Ni–Ru/H-ZSM-5 catalyst had an obvious activity of breaking Cβ-O bonds before and after the reaction. The result showed that after loading metal Ni and Ru, the Lewis acid of the catalytic system was greatly increased, which caused electron transfer between Ni and Ru. 3Ni-1.5Ru/H-ZSM-5 had the strongest activity due to the largest synergy among Ni, Ru and H-ZSM-5. The synergy was the key factor leading to the cleavage of C–C and C–O bonds in straw lignin and the high-performance catalytic degradation of lignin. Besides, the effect of reaction solvent and hydrogen resource on upgrading lignin to fine chemicals over 3Ni-1.5Ru/HZSM-5 catalyst was also intensively investigated. This research developed a method for the direct conversion of lignin into valuable monophenols.



中文翻译:

Ni-Ru / H-ZSM-5非均相一锅催化木质素转化为单酚

由于木质素的惰性和结构复杂性,将木质素升级为生物燃料和精细化学品仍然面临巨大挑战。本文采用一锅法以镍和钌双金属为载体的H-ZSM-5催化秸秆木质素,木质素转化率达到88.1%。单酚的产率为19.5%,其中4-乙基苯酚和4-乙基愈创木酚的产率分别为4.9%和3.8%。所述2D HSQC NMR分析证实,镍-钌/ H-ZSM-5催化剂具有破C的明显活性β-O键在反应前后。结果表明,负载金属镍和钌后,催化体系的路易斯酸大大增加,引起镍与钌之间的电子转移。3Ni-1.5Ru / H-ZSM-5具有最强的活性,这是由于Ni,Ru和H-ZSM-5之间的协同作用最大。协同作用是导致稻草木质素中C–C和C–O键断裂以及木质素高效催化降解的关键因素。此外,还深入研究了反应溶剂和氢资源对木质素在3Ni-1.5Ru / HZSM-5催化剂上转化为精细化学品的影响。这项研究开发了一种将木质素直接转化为有价值的单酚的方法。

更新日期:2021-02-19
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