The synthesis of fused arenes from non-aromatic precursors is useful but challenging.Herein,the synthesis of widely-used naphthylamines was focused.The three-component reactions of p-quinols,enals and amines were inve...The synthesis of fused arenes from non-aromatic precursors is useful but challenging.Herein,the synthesis of widely-used naphthylamines was focused.The three-component reactions of p-quinols,enals and amines were investigated under the dienamine/iminium-based dual organocatalysis.The efficient synthesis of naphthylamines was achieved via a formal[3+3]cyclization of the amines activated p-quinols and enals,with the following Bu_(4)NOAc/AgNO_(3) facilitated dual aromatization.The different reactivity of in-situ generated dienamine and iminium intermediates resulted in the differentiating catalysis,providing an efficient and practical methodology for the synthesis of fused arenes from non-aromatic precursors.展开更多
Utilizing interfacial interaction between different components of a heterojunction to induce defect formation may be an interesting approach for improving the catalytic performance.Here,introducing 3 nm CdS clusters(S...Utilizing interfacial interaction between different components of a heterojunction to induce defect formation may be an interesting approach for improving the catalytic performance.Here,introducing 3 nm CdS clusters(S)on NH_(2)-MIL-125(Ti)nanosheets(NMT-NS)to construct the heterojunction catalysts(Sx/NMT-NS)can induce the generation of abundant defects and Ti^(3+)sites due to the lattice distortion of NMT-NS and the transfer of interfacial charges.These defects and Ti^(3+)sites can chemisorb benzyl alcohol(BZO)molecules through a C–O…Ti coordination while capture and activate O2molecules from air.Furthermore,Z-scheme heterojunction between Cd S clusters and NMT-NS optimizes the transfer and separation of photogenerated electrons-holes,thus accelerating the production of·O_(2)^(-).Therefore,S1.8/NMT-NS achieves a highly efficient conversion of benzylamine(BZA)(>99%)and BZO to N-benzylidene benzylamine(N-BZA)in air atmosphere under visible light,with a selectivity of 99%.Finally,a photocatalytic mechanism involving the activation of reactants molecule and the transfer of photogenerated carriers is propounded at molecular level.展开更多
基金the Department of Science and Technology of Jilin Province(20220402046GH,20220101066JC)Research Projects from Education Department of Jilin Province(JJKH20250313BS)are greatly acknowledged.
文摘The synthesis of fused arenes from non-aromatic precursors is useful but challenging.Herein,the synthesis of widely-used naphthylamines was focused.The three-component reactions of p-quinols,enals and amines were investigated under the dienamine/iminium-based dual organocatalysis.The efficient synthesis of naphthylamines was achieved via a formal[3+3]cyclization of the amines activated p-quinols and enals,with the following Bu_(4)NOAc/AgNO_(3) facilitated dual aromatization.The different reactivity of in-situ generated dienamine and iminium intermediates resulted in the differentiating catalysis,providing an efficient and practical methodology for the synthesis of fused arenes from non-aromatic precursors.
基金supported by the National Natural Science Foundation of China(No.22002030)Innovational Found for Scientific and Technological Personnel of Hainan Province(No.NHXXRCXM202301)+1 种基金Collaborative Innovation Center of Ecological Civilization,Hainan University(No.XTCX2022STC11)the Shandong Laboratory of Advanced Materials and Green Manufacturing at Yantai(No.AMGM2024F23)。
文摘Utilizing interfacial interaction between different components of a heterojunction to induce defect formation may be an interesting approach for improving the catalytic performance.Here,introducing 3 nm CdS clusters(S)on NH_(2)-MIL-125(Ti)nanosheets(NMT-NS)to construct the heterojunction catalysts(Sx/NMT-NS)can induce the generation of abundant defects and Ti^(3+)sites due to the lattice distortion of NMT-NS and the transfer of interfacial charges.These defects and Ti^(3+)sites can chemisorb benzyl alcohol(BZO)molecules through a C–O…Ti coordination while capture and activate O2molecules from air.Furthermore,Z-scheme heterojunction between Cd S clusters and NMT-NS optimizes the transfer and separation of photogenerated electrons-holes,thus accelerating the production of·O_(2)^(-).Therefore,S1.8/NMT-NS achieves a highly efficient conversion of benzylamine(BZA)(>99%)and BZO to N-benzylidene benzylamine(N-BZA)in air atmosphere under visible light,with a selectivity of 99%.Finally,a photocatalytic mechanism involving the activation of reactants molecule and the transfer of photogenerated carriers is propounded at molecular level.
