It is first revealed by thermodesorption spectroscopy that when bismuth atoms diffuse the indium atoms through an intermediate graphite layer, they show certain characteristic features. In the Ir (111)-C system at 140...It is first revealed by thermodesorption spectroscopy that when bismuth atoms diffuse the indium atoms through an intermediate graphite layer, they show certain characteristic features. In the Ir (111)-C system at 1400 K δ = 0.4 ± 0.05 and diffusion δ<sub>Bi</sub> = N<sub>dif</sub>/N = 2.5 × 10<sup>-3</sup> bismuth atoms in the Ir(111)-C system. The amount of intercalated and diffused bismuth depends on the electrical field, i.e., on the positive potential in the Ir(111)-C system. It has been noted that a considerable diffusion of bismuth into iridium started at 180 V and increased up to 3000 V. The activation energies for bismuth diffusion into and from iridium were calculated to be E<sub>n1</sub> = 6.05 ± 0.05 eV and E<sub>1n</sub> = 6.3 ± 0.1 eV, respectively.展开更多
The development of highly active DFT catalysts for an electrocatalytic N_(2)reduction reaction(NRR)under mild conditions is a difficult challenge.In this study,a series of atom‐pair catalysts(APCs)for an NRR were fab...The development of highly active DFT catalysts for an electrocatalytic N_(2)reduction reaction(NRR)under mild conditions is a difficult challenge.In this study,a series of atom‐pair catalysts(APCs)for an NRR were fabricated using transition‐metal(TM)atoms(TM=Sc−Zn)doped into g‐CN monolayers.The electrochemical mechanism of APCs for an NRR has been reported by well‐defined density functional theory calculations.The calculated limiting potentials were−0.47 and−0.78 V for the Fe_(2)@CN and Co_(2)@CN catalysts,respectively.Owing to its high suppression of hydrogen evolution reactions,Co_(2)@CN is a superior electrocatalytic material for a N_(2)fixation.Stable Fe_(2)@CN may be a strongly attractive material for an NRR with a relatively low overpotential after an improvement in the selectivity.The two‐way charge transfer affirmed the donation‐acceptance procedure between N_(2)and Fe_(2)@CN or Co_(2)@CN,which play a crucial role in the activation of inert N≡N bonds.This study provides an in‐depth investigation into atom‐pair catalysts and will open up new avenues for highly efficient g‐CN‐based nanostructures for an NRR.展开更多
文摘It is first revealed by thermodesorption spectroscopy that when bismuth atoms diffuse the indium atoms through an intermediate graphite layer, they show certain characteristic features. In the Ir (111)-C system at 1400 K δ = 0.4 ± 0.05 and diffusion δ<sub>Bi</sub> = N<sub>dif</sub>/N = 2.5 × 10<sup>-3</sup> bismuth atoms in the Ir(111)-C system. The amount of intercalated and diffused bismuth depends on the electrical field, i.e., on the positive potential in the Ir(111)-C system. It has been noted that a considerable diffusion of bismuth into iridium started at 180 V and increased up to 3000 V. The activation energies for bismuth diffusion into and from iridium were calculated to be E<sub>n1</sub> = 6.05 ± 0.05 eV and E<sub>1n</sub> = 6.3 ± 0.1 eV, respectively.
文摘The development of highly active DFT catalysts for an electrocatalytic N_(2)reduction reaction(NRR)under mild conditions is a difficult challenge.In this study,a series of atom‐pair catalysts(APCs)for an NRR were fabricated using transition‐metal(TM)atoms(TM=Sc−Zn)doped into g‐CN monolayers.The electrochemical mechanism of APCs for an NRR has been reported by well‐defined density functional theory calculations.The calculated limiting potentials were−0.47 and−0.78 V for the Fe_(2)@CN and Co_(2)@CN catalysts,respectively.Owing to its high suppression of hydrogen evolution reactions,Co_(2)@CN is a superior electrocatalytic material for a N_(2)fixation.Stable Fe_(2)@CN may be a strongly attractive material for an NRR with a relatively low overpotential after an improvement in the selectivity.The two‐way charge transfer affirmed the donation‐acceptance procedure between N_(2)and Fe_(2)@CN or Co_(2)@CN,which play a crucial role in the activation of inert N≡N bonds.This study provides an in‐depth investigation into atom‐pair catalysts and will open up new avenues for highly efficient g‐CN‐based nanostructures for an NRR.
