Protection Group Effects During α,γ-Diol Lignin Stabilization Promote High-Selectivity Monomer Production
Protection Group Effects During α,γ-Diol Lignin Stabilization Promote High-Selectivity Monomer Production
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DOI：
10.1002/anie.201710838
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发表时间：
2018-01-26
影响因子：
16.6
通讯作者：
Luterbacher, Jeremy S.
中科院分区：
文献类型：
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作者：
Lan, Wu;Amiri, Masoud Talebi;Luterbacher, Jeremy S.
在生物质预处理过程中引入保护基团，以稳定木质素在其提取过程中的β-二醇基团，并防止其缩合。乙醛和丙醛稳定的，-二醇没有任何芳环烷基化，这显着增加了最终产品的选择性。随后由Pd/C催化的氢解产生基于Klason木质素的接近理论产率的木质素单体（48%来自桦树，20%来自云杉，70%来自高-姜基转基因杨树），并且在杨树的情况下具有对单一4-正丙醇姜基醇产物的高选择性（80%）。与天然木材的直接氢化不同，用Ni/C保护的木质素的氢解也导致对该单一产物的高选择性（78%），为用贱金属催化剂高选择性木质素升级铺平了道路。提取的木质素的使用促进了多糖的增值，导致所有三种主要生物质聚合物高产率为单一主要产物。
Protection groups were introduced during biomass pretreatment to stabilize lignin's ,-diol group during its extraction and prevent its condensation. Acetaldehyde and propionaldehyde stabilized the ,-diol without any aromatic ring alkylation, which significantly increased final product selectivity. The subsequent hydrogenolysis catalyzed by Pd/C generated lignin monomers at near-theoretical yields based on Klason lignin (48% from birch, 20% from spruce, 70% from high-syringyl transgenic poplar), and with high selectivity to a single 4-n-propanolsyringol product (80%) in the case of the poplar. Unlike direct hydrogenation of native wood, hydrogenolysis of protected lignin with Ni/C also led to high selectivity to this single product (78%), paving the way to high-selectivity lignin upgrading with base metal catalysts. The use of extracted lignin facilitated valorization of polysaccharides, leading to high yields of all three major biomass polymers to a single major product.