The nitrogen reduction reaction(NRR)under ambient conditions is still challenging due to the inertness of N2.Herein,we report a series of superior NRR catalysts identified by examining Ti2NO2 MXenes embedded with 28 d...The nitrogen reduction reaction(NRR)under ambient conditions is still challenging due to the inertness of N2.Herein,we report a series of superior NRR catalysts identified by examining Ti2NO2 MXenes embedded with 28 different single-atom catalysts using first-principles calculations.The stability of this system was first verified using formation energies,and it is discovered that N2 can be effectively adsorbed due to the synergistic effect between single atom catalysis and the Ti atoms.Examination of the electronic structure demonstrated that this design satisfies orbital symmetry matching where“acceptor-donor”interaction scenario can be realized.A new“enzymatic-distal”reaction mechanism that is a mixture of the enzymatic and distal pathways was also discovered.Among all of the candidates,Ni anchored on MXene system achieves an onset potential as low as–0.13 V,which to the best of our knowledge is the lowest onset potential value reported to date.This work elucidates the significance of orbital symmetry matching and provides theoretical guidance for future studies.展开更多
We have studied spin-dependent thermoelectric transport through parallel triple quantum dots with Rashba spinorbital interaction（RSOI） embedded in an Aharonov-Bohm interferometer connected symmetrically to leads usi...We have studied spin-dependent thermoelectric transport through parallel triple quantum dots with Rashba spinorbital interaction（RSOI） embedded in an Aharonov-Bohm interferometer connected symmetrically to leads using nonequilibrium Green＇s function method in the linear response regime.Under the appropriate configuration of magnetic flux phase and RSOI phase,the spin figure of merit can be enhanced and is even larger than the charge figure of merit.In particular,the charge and spin thermopowers as functions of both the magnetic flux phase and the RSOI phase present quadruple-peak structures in the contour graphs.For some specific configuration of the two phases,the device can provide a mechanism that converts heat into a spin voltage when the charge thermopower vanishes while the spin thermopower is not zero,which is useful in realizing the thermal spin battery and inducing a pure spin current in the device.展开更多
文摘The nitrogen reduction reaction(NRR)under ambient conditions is still challenging due to the inertness of N2.Herein,we report a series of superior NRR catalysts identified by examining Ti2NO2 MXenes embedded with 28 different single-atom catalysts using first-principles calculations.The stability of this system was first verified using formation energies,and it is discovered that N2 can be effectively adsorbed due to the synergistic effect between single atom catalysis and the Ti atoms.Examination of the electronic structure demonstrated that this design satisfies orbital symmetry matching where“acceptor-donor”interaction scenario can be realized.A new“enzymatic-distal”reaction mechanism that is a mixture of the enzymatic and distal pathways was also discovered.Among all of the candidates,Ni anchored on MXene system achieves an onset potential as low as–0.13 V,which to the best of our knowledge is the lowest onset potential value reported to date.This work elucidates the significance of orbital symmetry matching and provides theoretical guidance for future studies.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11274208 and 11447170)
文摘We have studied spin-dependent thermoelectric transport through parallel triple quantum dots with Rashba spinorbital interaction（RSOI） embedded in an Aharonov-Bohm interferometer connected symmetrically to leads using nonequilibrium Green＇s function method in the linear response regime.Under the appropriate configuration of magnetic flux phase and RSOI phase,the spin figure of merit can be enhanced and is even larger than the charge figure of merit.In particular,the charge and spin thermopowers as functions of both the magnetic flux phase and the RSOI phase present quadruple-peak structures in the contour graphs.For some specific configuration of the two phases,the device can provide a mechanism that converts heat into a spin voltage when the charge thermopower vanishes while the spin thermopower is not zero,which is useful in realizing the thermal spin battery and inducing a pure spin current in the device.
