Nitrogen-Doped Carbon-Modified Cobalt-Nanoparticle-Catalyzed Oxidative Cleavage of Lignin beta-O-4 Model Compounds under Mild Conditions

doi:10.1021/acssuschemeng.8b02802

	Nitrogen-Doped Carbon-Modified Cobalt-Nanoparticle-Catalyzed Oxidative Cleavage of Lignin beta-O-4 Model Compounds under Mild Conditions
	Luo, Huihui 1,2; Wang, Lianyue 1; Li, Guosong 1; Shang, Sensen 1; Lv, Ying 1; Niu, Jingyang 2; Gao, Shuang 1
刊名	ACS SUSTAINABLE CHEMISTRY & ENGINEERING
	2018-11-05
卷号	6 期号:11 页码:14188-14196
关键词	Lignin Oxidative cleavage Heterogeneous catalyst Model compounds Cobalt oxides
ISSN号	2168-0485
DOI	10.1021/acssuschemeng.8b02802
通讯作者	Wang, Lianyue(lianyuewang@dicp.ac.cn) ; Niu, Jingyang(jyniu@henu.edu.cn) ; Gao, Shuang(sgao@dicp.ac.cn)
英文摘要	A noble-metal-free Co-based catalyst, derived from pyrolysis of natural vitamin B-12 on activated carbon, is developed for the first time for one-pot oxidative cleavage of lignin linkages to phenols and aromatic esters with molecular oxygen as the oxidant under mild reaction conditions. High yields of phenol were obtained, and no oxidative coupling of phenol was produced based on the present cobalt catalyst. Compared to the previous report, the present catalyst can achieve the oxidative cleavage of beta-O-4 ketones even at room temperature using a dioxygen balloon. The heterogeneous catalyst shows robust recyclability and can be conveniently recovered and reused up to eight times without an appreciable loss of catalytic activity. Moreover, this catalyst system can realize the bond cleavage of organosolv lignin. The evidence of depolymerization was given by two-dimensional heteronuclear single quantum coherence NMR and gel permeation chromatography. Characterization of the catalyst by inductively coupled plasma, N-2 adsorption-desorption, Raman spectroscopy, scanning electron microscopy, transmission electron microscopy (TEM), high-resolution TEM, high-angle angular dark-field scanning TEM, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, and control experiments provide a fundamental understanding of the catalytic materials and the reaction pathway. Co3O4 in situ supported on a N-doped carbon matrix by the way of high-temperature pyrolysis might be a catalytically active species. Two reaction intermediates are detected and confirmed by gas chromatograph-mass spectrometry.
资助项目	National Natural Science Foundation of China[21773227] ; National Natural Science Foundation of China[21403219] ; National Natural Science Foundation of China[21773232]
WOS关键词	C BOND-CLEAVAGE ; SELECTIVE OXIDATION ; AEROBIC OXIDATION ; METAL-FREE ; VALUABLE CHEMICALS ; VANADIUM CATALYST ; MESOPOROUS CARBON ; OXYGEN REDUCTION ; CO3O4 CATALYST ; DEPOLYMERIZATION
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Engineering
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000449577200064
资助机构	National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/166712]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Wang, Lianyue; Niu, Jingyang; Gao, Shuang
作者单位	1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 2.Henan Univ, Henan Key Lab Polyoxometalate Chem, Inst Mol & Crystal Engn, Coll Chem & Chem Engn, Kaifeng 475004, Peoples R China
推荐引用方式 GB/T 7714	Luo, Huihui,Wang, Lianyue,Li, Guosong,et al. Nitrogen-Doped Carbon-Modified Cobalt-Nanoparticle-Catalyzed Oxidative Cleavage of Lignin beta-O-4 Model Compounds under Mild Conditions[J]. ACS SUSTAINABLE CHEMISTRY & ENGINEERING,2018,6(11):14188-14196.
APA	Luo, Huihui.,Wang, Lianyue.,Li, Guosong.,Shang, Sensen.,Lv, Ying.,...&Gao, Shuang.(2018).Nitrogen-Doped Carbon-Modified Cobalt-Nanoparticle-Catalyzed Oxidative Cleavage of Lignin beta-O-4 Model Compounds under Mild Conditions.ACS SUSTAINABLE CHEMISTRY & ENGINEERING,6(11),14188-14196.
MLA	Luo, Huihui,et al."Nitrogen-Doped Carbon-Modified Cobalt-Nanoparticle-Catalyzed Oxidative Cleavage of Lignin beta-O-4 Model Compounds under Mild Conditions".ACS SUSTAINABLE CHEMISTRY & ENGINEERING 6.11(2018):14188-14196.