文献类型：期刊文献

英文题名：Breaking the Limit of Lignin Monomer Production via Cleavage of Interunit Carbon-Carbon Linkages

作者：Dong, Lin[1,2];Lin, Longfei[3];Han, Xue[3];Si, Xiaoqin[4];Liu, Xiaohui[1,2];Guo, Yong[1,2];Lu, Fang[4];Rudic, Svemir[5];Parker, Stewart F.[5];Yang, Sihai[3];Wang, Yanqin[1,2]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Feringa Nobel Prize Scientist Joint Res Ctr, Key Lab Adv Mat,Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Joint Int Res Lab Precis Chem & Mol Engn, Feringa Nobel Prize Scientist Joint Res Ctr, Res Inst Ind Catalysis,Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[3]Univ Manchester, Sch Chem, Manchester M13 9PL, Lancs, England;[4]Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China;[5]STFC Rutherford Appleton Lab, ISIS Facil, Chilton OX11 0QX, Oxon, England

年份：2019

卷号：5

期号：6

起止页码：1521

外文期刊名：CHEM

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000476610100013)】；

基金：This work was supported financially by the National Natural Science Foundation of China (21832002, 21872050, 21808063, and 91545103), the Science and Technology Commission of Shanghai Municipality (2018SHZDZX03), the Programme of Introducing Talents of Discipline to Universities (B16017) in China, the Fundamental Research Funds for the Central Universities (222201718003), and the University of Manchester, Royal Society, and Engineering and Physical Sciences Research Council (EP/P011632/1) in the UK. We are especially grateful to the Science and Technology Facilities Council (STFC) and the ISIS Neutron Facility for access to the Beamline TOSCA. We thank S. Xu, Q. Xia, C. Goodway, and M. Kibble for their help at the beamline. Computing resources (time on the SCARF cluster for the CASTEP calculations) were provided by STFC's e-Science facility.

语种：英文

摘要：Conversion of lignin into monocyclic hydrocarbons as commodity chemicals and drop-in fuels is a highly desirable target for biorefineries. However, this is severely hindered by the presence of stable interunit carbon-carbon linkages in native lignin and those formed during lignin extraction. Herein, we report a newmultifunctional catalyst, Ru/NbOPO4, that achieves the first example of catalytic cleavage of both interunit C-C and C-O bonds in one-pot lignin conversions to yield 124%-153% of monocyclic hydrocarbons, which is 1.2-1.5 times the yields obtained from the established nitrobenzene oxidation method. This catalyst also exhibits high stability and selectivity (up to 68%) to monocyclic arenes over repeated cycles. The mechanism of the activation and cleavage of 5-5 C-C bonds in biphenyl, as a lignin model adopting the most robust C-C linkages, has been revealed via in situ inelastic neutron scattering coupled with modeling. This study breaks the conventional theoretical limit on lignin monomer production.