Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is chall...Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+) on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2) generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+) interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H_(4) formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of *CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2) products at the Cu^(0)/Cu^(+) interface than that of H_(2) under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2) products.展开更多
The novel copper?complex with salicylaldehyde benzoylhydrazone and pyridine ligands, Cu(C14H10N2O2)(C5H5N), has been synthesized and characterized by elemental analysis, IR and thermal analysis. The crystal structure ...The novel copper?complex with salicylaldehyde benzoylhydrazone and pyridine ligands, Cu(C14H10N2O2)(C5H5N), has been synthesized and characterized by elemental analysis, IR and thermal analysis. The crystal structure of the title complex has been determined by single crystal X ray diffraction techniques. The crystal belongs to monoclinic with space group P21/c. The cell parameters are: a=1.6362(9)nm, b=1.7140(9)nm, c=1.2255(7)nm, β=105.168(9)°, V=3.317(3)nm3, Z=8, Dc=1.525g·cm-3, μ(MoKα)=1.334mm-1, F(000)=1560. The structure wasrefined to final R1=0.0376, wR2=0.0909. The copper?ion lies in a distorted square planar environment composed of two oxygen atoms, one nitrogen atom of tridentate acyhydrazone Schiff base ligand and one nitrogen atom of the pyridine ligand. CCDC: 193111.展开更多
Grafting dodecyl in EDTA,A ligand-N,N′-di ( dodecyl ) disodium ethylenediamine di-acetic acid was synthesized and its complex C 30 H 58 O 4N 2Cu ( Ⅱ ) was obtained in chloroformme∶thanol=1∶1( V/V ).The products we...Grafting dodecyl in EDTA,A ligand-N,N′-di ( dodecyl ) disodium ethylenediamine di-acetic acid was synthesized and its complex C 30 H 58 O 4N 2Cu ( Ⅱ ) was obtained in chloroformme∶thanol=1∶1( V/V ).The products were characterized by IR?EA? 1HNMR and UV spectra.展开更多
The crystal and molecular structure of the title complex, Cu（ada）2（py）2（H2O）（ada=adamantanecarboxylic group, py=pyridine）, C 32H 42CuN2O5, were determined by XRD. It belongs to monoclinic system with space gro...The crystal and molecular structure of the title complex, Cu（ada）2（py）2（H2O）（ada=adamantanecarboxylic group, py=pyridine）, C 32H 42CuN2O5, were determined by XRD. It belongs to monoclinic system with space group P21/n and crystal cell parameters:a=1.619 9（3）, b=0.680 5（1）, c=2.802 8（6） nm, β=94.15（3）°; V=3.082（1） nm 3, Z=4, Dc=1.289 g/cm3, Mr=589.22, μ（MoKα）=0.750 mm -1, F（000）=1 268. The structure was refined to R=0.057 8 and wR=0.158 1 for 4 447 observed reflections with I≥2σ（I）. The aquo complex is mononuclear with distorted square-pyramidal coordination.展开更多
A novel coordination polymer, [Cu(m-BDOA)(bipy)·H2O]n (m-BDOA2-=benzene-1,3-dioxyacetate), was synthesized and characterized by elemental analysis, IR spectra, X-ray single crystal structure analysis. Crystallogr...A novel coordination polymer, [Cu(m-BDOA)(bipy)·H2O]n (m-BDOA2-=benzene-1,3-dioxyacetate), was synthesized and characterized by elemental analysis, IR spectra, X-ray single crystal structure analysis. Crystallographic data are as follows: orthorhombic, space group Pna21, a=1.606 9(3) nm, b=1.685 9(3) nm, c=0.699 7(1) nm, V=1.8955(7) nm3, Z=4, Dc=1.619 g·cm-3, -ligand, two nitrogen atoms of 2,2′-bipy ligand and one coordinated water, there is a distorted square pyramidal environment. Two copper atoms are bridged by m-BDOA2-ligand, forming a one-dimensional chain along a axis. The adjacent distance of Cu...Cu atoms is 0.877 3 nm. The crystal network was formed by the intermolecular hydrogen bond and π-packing interactions.展开更多
文摘Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+) on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2) generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+) interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H_(4) formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of *CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2) products at the Cu^(0)/Cu^(+) interface than that of H_(2) under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2) products.
文摘The novel copper?complex with salicylaldehyde benzoylhydrazone and pyridine ligands, Cu(C14H10N2O2)(C5H5N), has been synthesized and characterized by elemental analysis, IR and thermal analysis. The crystal structure of the title complex has been determined by single crystal X ray diffraction techniques. The crystal belongs to monoclinic with space group P21/c. The cell parameters are: a=1.6362(9)nm, b=1.7140(9)nm, c=1.2255(7)nm, β=105.168(9)°, V=3.317(3)nm3, Z=8, Dc=1.525g·cm-3, μ(MoKα)=1.334mm-1, F(000)=1560. The structure wasrefined to final R1=0.0376, wR2=0.0909. The copper?ion lies in a distorted square planar environment composed of two oxygen atoms, one nitrogen atom of tridentate acyhydrazone Schiff base ligand and one nitrogen atom of the pyridine ligand. CCDC: 193111.
文摘Grafting dodecyl in EDTA,A ligand-N,N′-di ( dodecyl ) disodium ethylenediamine di-acetic acid was synthesized and its complex C 30 H 58 O 4N 2Cu ( Ⅱ ) was obtained in chloroformme∶thanol=1∶1( V/V ).The products were characterized by IR?EA? 1HNMR and UV spectra.
文摘The crystal and molecular structure of the title complex, Cu（ada）2（py）2（H2O）（ada=adamantanecarboxylic group, py=pyridine）, C 32H 42CuN2O5, were determined by XRD. It belongs to monoclinic system with space group P21/n and crystal cell parameters:a=1.619 9（3）, b=0.680 5（1）, c=2.802 8（6） nm, β=94.15（3）°; V=3.082（1） nm 3, Z=4, Dc=1.289 g/cm3, Mr=589.22, μ（MoKα）=0.750 mm -1, F（000）=1 268. The structure was refined to R=0.057 8 and wR=0.158 1 for 4 447 observed reflections with I≥2σ（I）. The aquo complex is mononuclear with distorted square-pyramidal coordination.
文摘A novel coordination polymer, [Cu(m-BDOA)(bipy)·H2O]n (m-BDOA2-=benzene-1,3-dioxyacetate), was synthesized and characterized by elemental analysis, IR spectra, X-ray single crystal structure analysis. Crystallographic data are as follows: orthorhombic, space group Pna21, a=1.606 9(3) nm, b=1.685 9(3) nm, c=0.699 7(1) nm, V=1.8955(7) nm3, Z=4, Dc=1.619 g·cm-3, -ligand, two nitrogen atoms of 2,2′-bipy ligand and one coordinated water, there is a distorted square pyramidal environment. Two copper atoms are bridged by m-BDOA2-ligand, forming a one-dimensional chain along a axis. The adjacent distance of Cu...Cu atoms is 0.877 3 nm. The crystal network was formed by the intermolecular hydrogen bond and π-packing interactions.
