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Impact of nitrogen species and content on the catalytic activity to C-O bond cleavage of lignin over N-doped carbon supported Ru-based catalyst
被引:35
作者:
Li, Tianjin
[1
]
Lin, Hongfei
[2
]
Ouyang, Xinping
[1
]
Qiu, Xueqing
[1
]
Wan, Zechen
[1
]
Ruan, Tao
[1
]
机构:
[1] South China Univ Technol, Sch Chem & Chem Engn, Guangzhou 510640, Guangdong, Peoples R China
[2] Washington State Univ, Voiland Sch Chem Engn & Bioengn, Pullman, WA 99164 USA
来源:
基金:
中国国家自然科学基金;
关键词:
N-doped carbon;
Lignin;
Catalytic hydrogenolysis;
Aromatic monomers;
C-O bond;
MODEL COMPOUNDS;
ORGANOSOLV LIGNIN;
BETA-O-4;
LINKAGES;
PHENOLIC MONOMERS;
METAL-CATALYSTS;
DEPOLYMERIZATION;
HYDROGENOLYSIS;
HYDRODEOXYGENATION;
HYDROGENATION;
NANOPARTICLES;
D O I:
10.1016/j.fuel.2020.118324
中图分类号:
TE [石油、天然气工业];
TK [能源与动力工程];
学科分类号:
0807 ;
0820 ;
摘要:
The selective cleavage of C-O bond in lignin is the key to convert them into aromatic compounds and then to produce liquid fuels and chemicals. N-doped carbon nanosheets were obtained by direct pyrolysis of glucosamine hydrochloride (GAH) and melamine. Highly-dispersed and small-sized Ru nanoparticles (NPs) supported N-doped carbon by impregnation method, which can efficiently convert lignin to obtain 40.70% aromatic monomers. It was 2.3 times than that of the commercial catalyst (Ru/C) and the catalyst could be used at least five runs with an insignificant loss in the yield of aromatic monomers. The morphology, specific surface area, nitrogen species and content of supports could be tuned by controlling the weight of melamine. The results showed that the melamine and GAH were condensed to form layered graphitic carbon nitride (g-C3N4) and a carbon skeleton at 600 degrees C, respectively. Then, the produced %N from the decomposition of g-C3N4 at high temperature (> 700 degrees C) could improve nitrogen concentration, increase the specific area and result in the graphene-like wrinkled morphology. The presence of pyridinic N not only served as metal coordination sites to stabilize and disperse Ru NPs but also enhanced the proportions of Ru-0 through the electronic interactions. The DFT calculations implied that the pyridinic N contributed to the highest adsorption energy for 2-phenoxy-1-henethanol (PPE) and a reduction of the disassociation energy for Calkyl-O bond compared with graphite N and pure C.
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页数:10
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