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Plasmon-enhanced photocatalytic oxidative coupling of amines in the air using a delicate Ag nanowire@NH_(2)-UiO-66 core-shell nanostructures

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Chinese Chemical Letters 2024年第4期35卷 506-510页

作者： Yuan Zhang Shenghao Gong A.R.Mahammed Shaheer Rong Cao Tianfu Liu Fujian Science Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

MOF-based core-shell structures with high surface area, abundant active sites, and broad absorption bands are viable alternatives to traditional single-component photocatalysts. In this report, we describe the design and construction of delicate Ag nanowires@NH_(2)-UiO-66 with a core-shell structure for use as photocatalysts in imine synthesis under light. The optimized composites exhibited 80% imine production, which was higher than both MOF and Ag NWs. The significant improvement in photocatalytic activity under light may be attributed to the plasmonic effect of silver nanowires and their core-shell structure, which promotes the separation of electron-hole pairs. Moreover, the photocatalytic activity of the core-shell nanostructure may provide valuable insight into the design and construction of MOF-based composite photocatalysts for oxidative coupling of amines.

关键词： Metal-organic frameworks Plasmonic silver nanowires Photocatalyst Core-shell nanostructure oxidative coupling of amines

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Electronic interaction and oxygen vacancy engineering of g-C_(3)N_(4)/α-Bi_(2)O_(3) Zscheme heterojunction for enhanced photocatalytic aerobic oxidative homo-/hetero-coupling of amines to imines in aqueous phase

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Green Carbon 2023年第2期1卷 105-117页

作者： Yanhua Gao Tao Song Xiuling Guo Yan Zhang Yong Yang College of Chemical and Chemical Engineering Qingdao UniversityQingdao 266101China CAS Key Laboratory of Bio-based Materials Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101China Shandong Energy Institute Qingdao 266101China Qingdao New Energy Shandong Laboratory Qingdao 266101China University of Chinese Academy of Sciences Beijing 100049China

Photocatalytic oxidation coupling of amines represents a green and cost-effective method for the synthesis of highly value-added imines under visible light ***,the catalytic efficiency was severely limited by poor visible light response and easy recombination of photogenerated charge ***,we report a g-CgN_(4)/α-Bi_(2)O_(3)Z-scheme heterojunction via electrostatic self-assembly of g-C_(3)N_(4)nanosheets and oxygen-va-cancy-rich aα-Bi_(2)O_(3)microsphere for visible-light driven oxidative coupling of amines to imines in H_(2)0 as green solvent at room *** with diverse functional groups were efficiently converted into the corre-sponding imines in good to excellent ***,this photocatalytic protocol is applicable for the challenging hetero-coupling of two structurally different amines to construct complicated asymmetric imines,which is the first report of photocatalytic hetero-coupling of amines to imines to our ***,the Z-scheme heterojunction also demonstrated high stability and could be readily separated and reused without obvious decay in activity and *** characterizations and control experiments reveal the construction of Z-scheme heterojunction with intimate interface between g-CgN4 and a-Bi_(2)O_(3)greatly boosts the transfer and separation of photogenerated charge carries and enhances the redox ***,the surface oxygen vacancies in a-Biz_(2)O_(3)also benefits the separation of photogenerated charge carriers and acti-vation of *** jointly contributed to an enhanced photocatalytic performance for oxidative coupling of amines to imines.

关键词： Z-scheme heterojunction Oxygen vacancies g-C_(3)N_(4)/α-Bi_(2)O_(3) Photocatalysis oxidative coupling of amines

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Enhancement of visible-light-driven oxidative amine coupling under aerobic and anaerobic conditions by photocatalyst with spatial separation of photoinduced charge carriers

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Nano Research 2023年第4期16卷 4715-4722页

作者： Shasha Wang Kuan Gao Yang Cui Shuwen Li Heyao Zhang Bin Zhang Jie Wu Hongwei Hou Shuangquan Zang Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450001China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China School of Science Xuchang UniversityXuchang 461000China

Spatial separation of oxidation/reduction cocatalyst is an effective means to improve the efficiency of charge separation in photocatalytic reaction ***,a yolk-shell Pd@NH_(2)-UiO-66@Cu_(2)O heterojunction was designed and synthesized by integration of electron collector Pd and hole collector Cu_(2)O inside and outside of a photoactive metal-organic framework(MOF)NH_(2)-UiO-66,*** obtained Pd@NH_(2)-UiO-66@Cu_(2)O heterojunction effectively inhibits the electron and hole recombination through the photo-induced electrons and holes flow inward and outward of the composite,and promotes the reduction and oxidation abilities for the oxidative coupling of benzylamine to *** with Pd/NH_(2)-UiO-66@Cu_(2)O,Pd@NH_(2)-UiO-66,and Pd/NH_(2)-UiO-66,Pd@NH_(2)-UiO-66@Cu_(2)O exhibits the highest photocatalytic *** importantly,Pd@NH_(2)-UiO-66@Cu_(2)O shows a conversion rate of benzylamine up to 99%either by oxidation under aerobic conditions or by strong adsorption of H atom(Hads)under anaerobic *** addition,the catalyst shows good stability and can be recycled at least ten *** work provides useful guidance on construction of MOFs-based composites with spatially separated photoinduced charge carriers to realize efficient oxidation coupling of benzylamine in both aerobic and anaerobic conditions.

关键词： metal-organic frameworks palladium nanoparticle photocatalysis cuprous oxide oxidative coupling of amines

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