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Selective Cellulose Hydrogenolysis to 2,5-Hexanedione and 1-Hydroxy-2-hexanone Using Ni@NC Combined with H3PO4
Liang, Yuan1,2; Wang, Haiyong2; Xin, Haosheng2; Hu, Xiaohong2; Yan, Long2,3; Zhang, Qi2,3; Wang, Chenguang2,3; Liu, Qiying2,3,4; Ma, Longlong1,2,3
2021-11-22
发表期刊ACS SUSTAINABLE CHEMISTRY & ENGINEERING
ISSN2168-0485
卷号9期号:46页码:15394-15405
通讯作者Liu, Qiying(liuqy@ms.giec.ac.cn) ; Ma, Longlong(mall@ms.giec.ac.cn)
摘要The production of ketones from cellulose is critical but challenging due to the easy hydrogenation of ketone groups. Herein, Ni particles encapsulated in N-doped carbon layers (Ni@ NC) were synthesized and used as efficient catalysts for direct cellulose hydrogenolysis to 2,5-hexanedione (HD) and 1-hydroxy-2-hexanone (HHO) in H3PO4 aqueous solution. HD and the first reported HHO in this work could be simultaneously produced with the yields of 34.1% and 24.5%, respectively. It was found that the hydrolyzed glucose was the key intermediate in the formation of these two target products. HD originated from the hydrolysis of 2,5-dimethylfuran (2,5-DMF) that was produced via glucose (from cellulose hydrolysis catalyzed by H3PO4) isomerization to fructose, followed by fructose dehydration to 5-hydroxymethylfurfural (5-HMF) and 5-HMF hydrodeoxgenation. In parallel, HHO was obtained from the selective hydrodeoxygenation of hexoses. The N species of Ni@NC catalysts acted as the basic sites for promoting glucose isomerization to fructose. The production of ketones could be attributed to the tailored hydrogenation ability of Ni@NC, which facilitated the selective preservation of C.O bonds. The synergy between H3PO4 (cellulose hydrolysis and C-O bond splitting by hydrogenolysis), base (aldehyde isomerization to ketone), and metallic Ni (hydrogenation) played an essential role in the formation of ketone-containing products with high yields.
关键词cellulose Ni@NC catalyst ketone-containing chemicals synergistic catalysis reaction pathway
DOI10.1021/acssuschemeng.1c03858
关键词[WOS]DOPED CARBON NANOTUBES ; CATALYTIC CONVERSION ; ETHYLENE-GLYCOL ; EFFICIENT ; NANOPARTICLES ; GRAPHENE ; METAL ; REDUCTION ; GLUCOSE ; BIOMASS
收录类别SCI
语种英语
资助项目National Key R&D Program of China[2019YFC1905303] ; National Natural Science Foundation of China[51976220] ; National Natural Science Foundation of China[51876209]
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Engineering
项目资助者National Key R&D Program of China ; National Natural Science Foundation of China
WOS类目Chemistry, Multidisciplinary ; Green & Sustainable Science & Technology ; Engineering, Chemical
WOS记录号WOS:000753951700005
出版者AMER CHEMICAL SOC
引用统计
被引频次:17[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.giec.ac.cn/handle/344007/35843
专题中国科学院广州能源研究所
通讯作者Liu, Qiying; Ma, Longlong
作者单位1.Univ Sci & Technol China, Dept Engn Sci, Hefei 230026, Peoples R China
2.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou 510640, Peoples R China
3.Guangdong Key Lab New & Renewable Energy Res & De, Guangzhou 510640, Peoples R China
4.CAS Key Lab Renewable Energy, Guangzhou 510640, Peoples R China
第一作者单位中国科学院广州能源研究所
推荐引用方式
GB/T 7714
Liang, Yuan,Wang, Haiyong,Xin, Haosheng,et al. Selective Cellulose Hydrogenolysis to 2,5-Hexanedione and 1-Hydroxy-2-hexanone Using Ni@NC Combined with H3PO4[J]. ACS SUSTAINABLE CHEMISTRY & ENGINEERING,2021,9(46):15394-15405.
APA Liang, Yuan.,Wang, Haiyong.,Xin, Haosheng.,Hu, Xiaohong.,Yan, Long.,...&Ma, Longlong.(2021).Selective Cellulose Hydrogenolysis to 2,5-Hexanedione and 1-Hydroxy-2-hexanone Using Ni@NC Combined with H3PO4.ACS SUSTAINABLE CHEMISTRY & ENGINEERING,9(46),15394-15405.
MLA Liang, Yuan,et al."Selective Cellulose Hydrogenolysis to 2,5-Hexanedione and 1-Hydroxy-2-hexanone Using Ni@NC Combined with H3PO4".ACS SUSTAINABLE CHEMISTRY & ENGINEERING 9.46(2021):15394-15405.
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