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作 者:Mingren Jin Seyed Mohsen Sadeghzadeh Jinzhu Chen
机构地区:[1]College of Chemistry and Materials Science,Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications,Jinan University,Guangzhou 511443,Guangdong,China [2]New Materials Technology and Processing Research Center,Department of Chemistry,Neyshabur Branch,Islamic Azad University,Neyshabur,Iran
出 处:《Journal of Energy Chemistry》2023年第7期638-652,I0013,共16页能源化学(英文版)
基 金:supported by the National Natural Science Foundation of China(22075104);the Youth Science and Technology Innovation Talent of Guangdong TeZhi Plan,China(2019TQ05L111);Innovation Team Project in Guangdong Colleges and Universities,China(2021KCXTD009);Educational Commission of Guangdong Province of China(2021ZDZX4037)。
摘 要:Visible light-driven valorization of biomass has recently been a pioneering field for nitrogen-containing heterocyclics syntheses due to its sustainable features.Herein,various aromatic ring-doped g-C_(3)N_(4) nanosheets(Ar-g-C_(3)N_(4);Ar=Py,Pm,Ph)were precisely designed to modulate their intrinsic electronic and band structure,which involves pyridine(Py),pyrimidine(Pm),and benzene(Ph)-doped g-C_(3)N_(4).Photocatalysts(CoPc/Ar-g-C_(3)N_(4)) of cobalt(II)phthalocyanine(CoPc)-fabricated Ar-g-C_(3)N_(4) were then developed for oxidative cyclization of furoin with 1,2-phenylenediamines for syntheses of various biomass-derived quinoxalines under visible-light irradiation.The catalytic activity(in terms of TOFs)of serial CoPc/Ar-g-C_(3)N_(4) samples increased with their transient photocurrents with CoPc/Py-g-C_(3)N_(4) as the most active one.For CoPc/Py-g-C_(3)N_(4),CoPc species functioned as both sensitizer and catalytic sites;while,doped Py led to a narrowed bandgap energy.Mechanism research further demonstrated that O_(2) was activated to superoxide radical(·O_(2)^(-)) by photoexcited high-level-energy electron(HLEE)transfer from Py-g-C_(3)N_(4) to CoPc for the subsequent aerobic oxidation.
关 键 词:Biomass Functionalized carbon nitride Nitrogen-containing heterocyclics Photocatalysis QUINOXALINE
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