Facile synthesis of photocatalysts with highly dispersed metal centers is a high-priority target yet still a significant challenge.In this work,a series of Co-C_(3)N_(4) photocatalysts with different Co contents atomi...Facile synthesis of photocatalysts with highly dispersed metal centers is a high-priority target yet still a significant challenge.In this work,a series of Co-C_(3)N_(4) photocatalysts with different Co contents atomically dispersed on g-CaN4 have been prepared via one-step thermal treatment of cobalt-based metal-organic frameworks(MOFs)and urea in the air.Thanks to the highly dispersed and rich exposed Co sites,as well as good charge separation efficiency and abundant mesopores,the optimal 25-Co-C_(3)N_(4),in the absence of noble metal catalysts/sensitizers,exhibits excellent performance for photocatalytic C0_(2) reduction to CO under visible.light irradiation,with a high CO evolution rate of 394.4μmol·g^(-1)·h^(-1),over 80 times higher than that of pure g-C_(3)N_(4)(4.9μmol·g^(-1)·h^(-1)).In:addition,by this facile synthesis strategy,the atomically dispersed Fe and Mn anchoring on g-C_(3)N_(4)(Fe-C_(3)N_(4) and Mn-C_(3)N_(4))have been also obtained,indicating the reliability and universality of this strategy in synthesizing photocatalysts with highly dispersed metal centers.This work paves a new way to develop cost-effective photocatalysts for photocatalytic C0_(2) reduction.展开更多
The application of multifunctional materials in various fields such as electronics and signal processors has attracted massive attention. Herein, a new organic-inorganic hybrid material [Et_(3)NCH_(2)Cl]_(2)[MnBr_(4)]...The application of multifunctional materials in various fields such as electronics and signal processors has attracted massive attention. Herein, a new organic-inorganic hybrid material [Et_(3)NCH_(2)Cl]_(2)[MnBr_(4)](1) is reported, which contains two organic amines cations and one [MnBr_(4)] tetrahedral ion. Compound 1 has a dielectric anomaly signal at 338 K, which proves its thermodynamic phase transition. The single crystal measurements at 200 K and 380 K show that the phase transition of compound 1 is caused by the thermal vibration of organic amine cations in the lattice. Moreover, compound 1 shows yellow-green luminescence under UV light irradiation. The magnetism measurements indicate that compound 1 shows switchable magnetic properties. This organic–inorganic material is a multifunctional material with dielectric, optical, and magnetic synergetic switchable effects, which expands a new direction for designing multifunctional materials.展开更多
The self-assembly of HL(L=[5-(ethoxycarbonyl)-4-phenyl-3,4-dihydropyrimidin-2(1H)-one-6-yl]methanesulfonate) with Sm(ClO4)3·6H2O yielded a 2D coordination polymer {[SmL3(H2O)2]·4H2O}n(1).Its crystallographic...The self-assembly of HL(L=[5-(ethoxycarbonyl)-4-phenyl-3,4-dihydropyrimidin-2(1H)-one-6-yl]methanesulfonate) with Sm(ClO4)3·6H2O yielded a 2D coordination polymer {[SmL3(H2O)2]·4H2O}n(1).Its crystallographic data indicated that it belonged to a triclinic system,space group P-1,a=1.42233(8),b=1.47155(8),c=1.53868(9) nm,α=8.62710(10),β=6.35250(10),γ=71.5790(10)°,V=2.7241(3) nm3,Z=2,R1=0.0693,wR2=0.1054.X-ray analysis revealed that the local coordination environment around Sm(III) was a slightly distorted dodecahedron in which Sm center was eight-coordinate geometry with eight oxygen atoms from three sulfonic groups,three carbonyl groups and two aqua ligands.Each L-acted as a bidentate spacer to link two Sm centers,resulted in the formation of a 2D hexagonally grid network.The discrete 2D planes in 1 were assembled into a 3D supramolecular network via strong hydrogen bonds among noncoordinated aqua O atoms,coordinated aqua O atoms,and noncoordinated O atoms of sulfonic groups and carbonyl groups.Furthermore,this metal-organic polymer exhibited strong photoluminescence maximized at 379 nm upon 274 nm excitation in the solid state at room temperature.展开更多
基金supported by the National Natural Science Foundation of China(Nos.21861001,21931007,21962002,22001043,and 22071182)the National Key R&D Program of China(No.2017YFA0700104)+3 种基金the Natural Science Foundation of Jiangxi Province(No.20202BAB203001)the Science Foundation of Jiangxi Provincial Office of Education(No.GJJ190753)the 111 Project of China(No.D17003)the Science&Technology Development Fund of Tianjin Education Commission for Higher Education(No.2018KJ129).
文摘Facile synthesis of photocatalysts with highly dispersed metal centers is a high-priority target yet still a significant challenge.In this work,a series of Co-C_(3)N_(4) photocatalysts with different Co contents atomically dispersed on g-CaN4 have been prepared via one-step thermal treatment of cobalt-based metal-organic frameworks(MOFs)and urea in the air.Thanks to the highly dispersed and rich exposed Co sites,as well as good charge separation efficiency and abundant mesopores,the optimal 25-Co-C_(3)N_(4),in the absence of noble metal catalysts/sensitizers,exhibits excellent performance for photocatalytic C0_(2) reduction to CO under visible.light irradiation,with a high CO evolution rate of 394.4μmol·g^(-1)·h^(-1),over 80 times higher than that of pure g-C_(3)N_(4)(4.9μmol·g^(-1)·h^(-1)).In:addition,by this facile synthesis strategy,the atomically dispersed Fe and Mn anchoring on g-C_(3)N_(4)(Fe-C_(3)N_(4) and Mn-C_(3)N_(4))have been also obtained,indicating the reliability and universality of this strategy in synthesizing photocatalysts with highly dispersed metal centers.This work paves a new way to develop cost-effective photocatalysts for photocatalytic C0_(2) reduction.
基金supported by the the National Natural Science Foundation of China (Nos.21875093, 22161002 and22105089)Natural Science Foundation of Jiangxi Province (Nos.20224BAB214005, 20204BCJ22015 and 20202ACBL203001)Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry (No.20212BCD42018)。
文摘The application of multifunctional materials in various fields such as electronics and signal processors has attracted massive attention. Herein, a new organic-inorganic hybrid material [Et_(3)NCH_(2)Cl]_(2)[MnBr_(4)](1) is reported, which contains two organic amines cations and one [MnBr_(4)] tetrahedral ion. Compound 1 has a dielectric anomaly signal at 338 K, which proves its thermodynamic phase transition. The single crystal measurements at 200 K and 380 K show that the phase transition of compound 1 is caused by the thermal vibration of organic amine cations in the lattice. Moreover, compound 1 shows yellow-green luminescence under UV light irradiation. The magnetism measurements indicate that compound 1 shows switchable magnetic properties. This organic–inorganic material is a multifunctional material with dielectric, optical, and magnetic synergetic switchable effects, which expands a new direction for designing multifunctional materials.
基金Project supported by the National Natural Science Foundation of China (20861001)Foundation of Science and Technology of Jiangxi Provincial Education Department (GJJ08505)
文摘The self-assembly of HL(L=[5-(ethoxycarbonyl)-4-phenyl-3,4-dihydropyrimidin-2(1H)-one-6-yl]methanesulfonate) with Sm(ClO4)3·6H2O yielded a 2D coordination polymer {[SmL3(H2O)2]·4H2O}n(1).Its crystallographic data indicated that it belonged to a triclinic system,space group P-1,a=1.42233(8),b=1.47155(8),c=1.53868(9) nm,α=8.62710(10),β=6.35250(10),γ=71.5790(10)°,V=2.7241(3) nm3,Z=2,R1=0.0693,wR2=0.1054.X-ray analysis revealed that the local coordination environment around Sm(III) was a slightly distorted dodecahedron in which Sm center was eight-coordinate geometry with eight oxygen atoms from three sulfonic groups,three carbonyl groups and two aqua ligands.Each L-acted as a bidentate spacer to link two Sm centers,resulted in the formation of a 2D hexagonally grid network.The discrete 2D planes in 1 were assembled into a 3D supramolecular network via strong hydrogen bonds among noncoordinated aqua O atoms,coordinated aqua O atoms,and noncoordinated O atoms of sulfonic groups and carbonyl groups.Furthermore,this metal-organic polymer exhibited strong photoluminescence maximized at 379 nm upon 274 nm excitation in the solid state at room temperature.