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Visible-light-driven selective cleavage of C[sbnd]C bonds in lignin model substrates using carbon nitride-supported ruthenium single-atom catalyst
2023-04-15
发表期刊CHEMICAL ENGINEERING JOURNAL; (IF:13.3[JCR-2023],13.2[5-Year])
ISSN1385-8947
EISSN1873-3212
卷号462
发表状态已发表
DOI10.1016/j.cej.2023.142282
摘要

The selective cleavage of the C[sbnd]C bonds in lignin is highly pursued to obtain aromatic monomers from renewable resources but remains challenging due to their high dissociation energies and steric hindrance between bulky aromatic groups. Herein, a mesoporous carbon nitride-supported ruthenium single-atom photocatalyst (Ru1/MCN) is reported for efficient oxidative Cα-Cβ bonds scissoring towards lignin β-O-4 model compounds with high activity and selectivity under visible–light irradiation and room temperature. With this strategy, a nearly total conversion of > 99% and > 98% selectivity of C[sbnd]C bond cleavage can be achieved upon 2–phenoxy–1–phenylethanol. In-depth investigations verify that the Cβ-H extraction by photogenerated holes is the critical step of the transformation, which directly generates the Cβ radical intermediates and thus promotes the selective Cα-Cβ bonds breaking by coupling with superoxide radicals induced by photogenerated electrons. This work explores the potential of single-atom catalysts for photocatalytic production of aromatics from renewable biomass feedstocks.

关键词Carbon nitrides Lignin model valorizations Photocatalysis Selective C-C bond cleavage Single-atom catalysts
学科门类Chemistry (all) ; Environmental Chemistry ; Chemical Engineering (all) ; Industrial and Manufacturing Engineering
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收录类别SCI ; EI ; SCOPUS
语种英语
资助项目National Natural Science Foundation of China[
WOS研究方向Engineering
WOS类目Engineering, Environmental ; Engineering, Chemical
WOS记录号WOS:000954522600001
出版者ELSEVIER SCIENCE SA
EI入藏号20231113703321
EI主题词Carbon nitride
EI分类号547.1 Precious Metals ; 801.4 Physical Chemistry ; 802.2 Chemical Reactions ; 803 Chemical Agents and Basic Industrial Chemicals ; 804 Chemical Products Generally ; 804.1 Organic Compounds ; 811.3 Cellulose, Lignin and Derivatives ; 931.3 Atomic and Molecular Physics
原始文献类型Article
Scopus 记录号2-s2.0-85149695728
来源库SCOPUS
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文献类型期刊论文
条目标识符https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/286513
专题物质科学与技术学院
物质科学与技术学院_硕士生
物质科学与技术学院_PI研究组_王竹君组
通讯作者Chen, Zupeng
作者单位
1.Nanjing Forestry Univ, Coll Chem Engn, Jiangsu Co Innovat Ctr Efficient Proc & Utilizat F, Int Innovat Ctr Forest Chem & Mat, Longpan Rd 159, Nanjing 210037, Peoples R China
2.Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
3.Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai, Peoples R China
4.Leibniz Inst Katalyse eV, Albert Einstein Str 29a, Rostock, Germany
推荐引用方式
GB/T 7714
Deng, Jun,Zhou, Chi,Yang, Yue,et al. Visible-light-driven selective cleavage of C[sbnd]C bonds in lignin model substrates using carbon nitride-supported ruthenium single-atom catalyst[J]. CHEMICAL ENGINEERING JOURNAL;,2023,462.
APA Deng, Jun.,Zhou, Chi.,Yang, Yue.,Nan, Bing.,Dong, Lin.,...&Chen, Zupeng.(2023).Visible-light-driven selective cleavage of C[sbnd]C bonds in lignin model substrates using carbon nitride-supported ruthenium single-atom catalyst.CHEMICAL ENGINEERING JOURNAL;,462.
MLA Deng, Jun,et al."Visible-light-driven selective cleavage of C[sbnd]C bonds in lignin model substrates using carbon nitride-supported ruthenium single-atom catalyst".CHEMICAL ENGINEERING JOURNAL; 462(2023).
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