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Rational highly dispersed ruthenium for reductive catalytic fractionation of lignocellulose
Nature Communications ( IF 16.6 ) Pub Date : 2022-08-11 , DOI: 10.1038/s41467-022-32451-5
Zhenzhen Liu 1 , Helong Li 1 , Xueying Gao 1 , Xuan Guo 2 , Shuizhong Wang 1 , Yunming Fang 2 , Guoyong Song 1
Affiliation  

Producing monomeric phenols from lignin biopolymer depolymerization in a detachable and efficient manner comes under the spotlight on the fullest utilization of sustainable lignocellulosic biomass. Here, we report a low-loaded and highly dispersed Ru anchored on a chitosan-derived N-doped carbon catalyst (RuN/ZnO/C), which exhibits outstanding performance in the reductive catalytic fractionation of lignocellulose. Nearly theoretical maximum yields of phenolic monomers from lignin are achieved, corresponding to TON as 431 molphenols molRu−1, 20 times higher than that from commercial Ru/C catalyst; high selectivity toward propyl end-chained guaiacol and syringol allow them to be readily purified. The RCF leave high retention of (hemi)cellulose amenable to enzymatic hydrolysis due to the successful breakdown of biomass recalcitrance. The RuN/ZnO/C catalyst shows good stability in recycling experiments as well as after a harsh hydrothermal treatment, benefiting from the coordination of Ru species with N atoms. Characterizations of the RuN/ZnO/C imply a transformation from Ru single atoms to nanoclusters under current reaction conditions. Time-course experiment, as well as reactivity screening of a series of lignin model compounds, offer insight into the mechanism of current RCF over RuN/ZnO/C. This work opens a new opportunity for achieving the valuable aromatic products from lignin and promoting the industrial economic feasibility of lignocellulosic biomass.



中文翻译:

用于木质纤维素还原催化分馏的合理高度分散钌

以可分离和高效的方式从木质素生物聚合物解聚中生产单体酚成为充分利用可持续木质纤维素生物质的焦点。在这里,我们报道了一种锚定在壳聚糖衍生的N掺杂碳催化剂 (RuN/ZnO/C)上的低负载且高度分散的 Ru ,它在木质纤维素的还原催化分馏中表现出出色的性能。从木质素中获得的酚类单体几乎达到理论最大产率,对应于 TON 为 431 molmol Ru -1,比商业Ru/C催化剂高20倍;对丙基末端链的愈创木酚和紫丁香酚的高选择性使它们易于纯化。由于生物质不顺性的成功分解,RCF 留下了易于酶水解的(半)纤维素的高保留。RuN/ZnO/C 催化剂在回收实验中以及经过苛刻的水热处理后表现出良好的稳定性,这得益于 Ru 物种与N的配位原子。RuN/ZnO/C 的表征意味着在当前反应条件下从 Ru 单原子向纳米团簇的转变。时程实验以及一系列木质素模型化合物的反应性筛选,提供了对当前 RCF 对 RuN/ZnO/C 的机理的深入了解。这项工作为从木质素中获得有价值的芳香产品和促进木质纤维素生物质的工业经济可行性提供了新的机会。

更新日期:2022-08-11
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