The 4f-5d transitions of Er3+ ions doped in crystals were widely studi ed due to their potential applications in quantum cutting phosphors and VUV lase rs,etc.The theory to do the calculations of 4f-5d transitions and...The 4f-5d transitions of Er3+ ions doped in crystals were widely studi ed due to their potential applications in quantum cutting phosphors and VUV lase rs,etc.The theory to do the calculations of 4f-5d transitions and various rela ted aspects,such as the ways to determining various parameters,were summarized .The impacts of various interactions on the spectra were also demonstrated clea rly with Er3+ ions in crystals CaF2 and LiYF4.Predicted results were compared w ith measured spectra.展开更多
The electrocatalytic conversion of CO_(2) into valuable chemical feedstocks using renewable electricity offers a compelling strategy for closing the carbon loop.While copper-based materials are effective in catalyzing...The electrocatalytic conversion of CO_(2) into valuable chemical feedstocks using renewable electricity offers a compelling strategy for closing the carbon loop.While copper-based materials are effective in catalyzing CO_(2) to C_(2+)products,the instability of Cu^(+)species,which tend to reduce to Cu~0 at cathodic potentials during CO_(2) reduction,poses a significant challenge.Here,we report the development of SmCu_(2)O and investigate the influence of f-d orbital hybridization on the CO_(2) reduction reaction (CO_(2)RR).Supported by density functional theory (DFT) calculations,our experimental results demonstrate that hybridization between Sm^(3+)4f and Cu^(+)3d orbitals not only improves the adsorption of *CO intermediates and increases CO coverage to stabilize Cu^(+) but also facilitates CO_(2) activation and lowers the energy barriers for CAC coupling.Notably,Sm-Cu_(2)O achieves a Faradaic efficiency for C_(2)H_(4) that is 38%higher than that of undoped Cu_(2)O.Additionally,it sustains its catalytic activity over an extended operational period exceeding 7 h,compared to merely 2 h for the undoped sample.This research highlights the potential of fd orbital hybridization in enhancing the efficacy of copper-based catalysts for CO_(2)RR,pointing towards a promising direction for the development of durable,high-performance electrocatalysts for sustainable chemical synthesis.展开更多
基金Project supported by the National Natural Science Foundation of China (10874173,10704090,11074315,11011120083)the Foundation of the Education Committee of Chongqing (KJ090523)the Knowledge Innovation Project of the Chinese Academy of Sciences (KJCX2-YW-M1)
文摘The 4f-5d transitions of Er3+ ions doped in crystals were widely studi ed due to their potential applications in quantum cutting phosphors and VUV lase rs,etc.The theory to do the calculations of 4f-5d transitions and various rela ted aspects,such as the ways to determining various parameters,were summarized .The impacts of various interactions on the spectra were also demonstrated clea rly with Er3+ ions in crystals CaF2 and LiYF4.Predicted results were compared w ith measured spectra.
基金Financial support from the National Natural Science Foundation of China(grant nos.22379006,21575016,U20A20154,22279005)from the National Program for Support of Top-notch Young Professionals is gratefully acknowledged。
文摘The electrocatalytic conversion of CO_(2) into valuable chemical feedstocks using renewable electricity offers a compelling strategy for closing the carbon loop.While copper-based materials are effective in catalyzing CO_(2) to C_(2+)products,the instability of Cu^(+)species,which tend to reduce to Cu~0 at cathodic potentials during CO_(2) reduction,poses a significant challenge.Here,we report the development of SmCu_(2)O and investigate the influence of f-d orbital hybridization on the CO_(2) reduction reaction (CO_(2)RR).Supported by density functional theory (DFT) calculations,our experimental results demonstrate that hybridization between Sm^(3+)4f and Cu^(+)3d orbitals not only improves the adsorption of *CO intermediates and increases CO coverage to stabilize Cu^(+) but also facilitates CO_(2) activation and lowers the energy barriers for CAC coupling.Notably,Sm-Cu_(2)O achieves a Faradaic efficiency for C_(2)H_(4) that is 38%higher than that of undoped Cu_(2)O.Additionally,it sustains its catalytic activity over an extended operational period exceeding 7 h,compared to merely 2 h for the undoped sample.This research highlights the potential of fd orbital hybridization in enhancing the efficacy of copper-based catalysts for CO_(2)RR,pointing towards a promising direction for the development of durable,high-performance electrocatalysts for sustainable chemical synthesis.
