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题名: Promoting Lignin Depolymerization and Restraining the Condensation via an Oxidation-Hydrogenation Strategy
作者: Zhang, Chaofeng1;  Li, Hongji1, 2;  Lu, Jianmin1;  Zhang, Xiaochen1;  MacArthur, Katherine E.3, 4;  Heggen, Marc3, 4;  Wang, Feng1
关键词: lignin ;  oxidation-hydrogenation ;  phenolic monomer ;  NaNO2/DDQ/NHPI ;  NiMo sulfide ;  lignin fragments' condensation
刊名: ACS CATALYSIS
发表日期: 2017-05-01
DOI: 10.1021/acscatal.7b00148
卷: 7, 页:3419-3429
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: For lignin valorization, simultaneously achieving the efficient cleavage of ether bonds and restraining the condensation of the formed fragments represents a challenge thus far. Herein, we report a two-step oxidation-hydrogenation strategy to achieve this goal. In the oxidation step, the O-2/NaNO2/DDQ/NHPI system selectively oxidizes C alpha H-OH to C-alpha=O within the beta-O-4 structure. In the subsequent hydrogenation step, the alpha-O-4 and the preoxidized beta-O-4 structures are further hydrogenated over a NiMo sulfide catalyst, leading to the cleavage of C-beta-OPh and C-alpha-OPh bonds. Besides the transformation of lignin model compounds, the yield of phenolic monomers from birch wood is up to 32% by using this two-step strategy. The preoxidation of C-alpha-OH to C-alpha=O not only weakens the C-beta-OPh ether bond but also avoids the condensation reactions caused by the presence of C-alpha(+) from dehydroxylation of C alpha H-OH. Furthermore, the NiMo sulfide prefers to catalyze the hydrogenative cleavage of the C-beta-OPh bond connecting with a C-alpha=O rather than catalyze the hydrogenation of C-alpha=O back to the original C alpha H-OH, which further ensures and utilizes the advantages of preoxidation.
关键词[WOS]: C-O BONDS ;  MODEL COMPOUNDS ;  CATALYZED DEPOLYMERIZATION ;  IONIC LIQUID ;  KRAFT LIGNIN ;  ARYL ETHERS ;  LIGNOCELLULOSE FRACTIONATION ;  ALCOHOL OXIDATION ;  VANADIUM CATALYST ;  ORGANOSOLV LIGNIN
语种: 英语
WOS记录号: WOS:000401054300041
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/152307
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Forschungszentrum Julich, Ernst Ruska Ctr Microscopy & Spect Electrons, D-52425 Julich, Germany
4.Forschungszentrum Julich, Peter Grunberg Inst, D-52425 Julich, Germany

Recommended Citation:
Zhang, Chaofeng,Li, Hongji,Lu, Jianmin,et al. Promoting Lignin Depolymerization and Restraining the Condensation via an Oxidation-Hydrogenation Strategy[J]. ACS CATALYSIS,2017,7:3419-3429.
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